Advanced Materials

Cover image for Vol. 29 Issue 24

Early View (Online Version of Record published before inclusion in an issue)

VIEW

  1. 1 - 100
  2. 101 - 200
  3. 201 - 278
  1. Communications

    1. Low-Cost Zeta Potentiometry Using Solute Gradients

      Sangwoo Shin, Jesse T. Ault, Jie Feng, Patrick B. Warren and Howard A. Stone

      Version of Record online: 9 JUN 2017 | DOI: 10.1002/adma.201701516

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      A cost-effective technique for measuring zeta potentials is demonstrated. The method uses solute gradients to induce particle and fluid motions via diffusiophoresis and diffusioosmosis. By visualizing the particle dynamics in a dead-end space, both zeta potentials for the particles and the walls can be determined independently. The method can be implemented with a low-cost microscope, which is orders of magnitude less expensive than conventional zeta potentiometers.

    2. 3D Nitrogen-Anion-Decorated Nickel Sulfides for Highly Efficient Overall Water Splitting

      Pengzuo Chen, Tianpei Zhou, Mengxing Zhang, Yun Tong, Chengan Zhong, Nan Zhang, Lidong Zhang, Changzheng Wu and Yi Xie

      Version of Record online: 9 JUN 2017 | DOI: 10.1002/adma.201701584

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      Metallic N-anion decorated Ni3S2 brings high surface active site exposure, enhanced conductivity, optimal hydrogen evolution reaction (HER) Gibbs free-energy, and water adsorption energy change, acting as superior bifunctional electrocatalysts for the HER/oxygen evolution reaction (OER). The metallic N-Ni3S2/NF 3D electrode only needs a low cell voltage of 1.48 V to reach the current density of 10 mA cm−2, which is superior to most Ni-based electrode materials.

    3. Efficient Flexible Solar Cell based on Composition-Tailored Hybrid Perovskite

      Cheng Bi, Bo Chen, Haotong Wei, Stephan DeLuca and Jinsong Huang

      Version of Record online: 9 JUN 2017 | DOI: 10.1002/adma.201605900

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      A different precursor ratio is found to be essential for the formation of high-quality perovskite films on flexible substrates compared to those formed on rigid substrates. A high efficiency of 18.1% is achieved for flexible perovskite solar-cell devices made on an indium tin oxide/poly(ethylene terephthalate) substrate via a low-temperature (≤100 °C) solution process.

    4. Metal Immiscibility Route to Synthesis of Ultrathin Carbides, Borides, and Nitrides

      Zixing Wang, Vidya Kochat, Prafull Pandey, Sanjay Kashyap, Soham Chattopadhyay, Atanu Samanta, Suman Sarkar, Praveena Manimunda, Xiang Zhang, Syed Asif, Abhisek K. Singh, Kamanio Chattopadhyay, Chandra Sekhar Tiwary and Pulickel M. Ajayan

      Version of Record online: 8 JUN 2017 | DOI: 10.1002/adma.201700364

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      Ultrathin tantalum carbide, nitride, and borides are synthesized on the surface of copper by heating a copper-tantalum immiscible couple in a precursor gas (C2H2, NH3, or B). This growth is caused by the immiscibility of the metals, which only allows clusters of Ta to migrate through the Cu matrix. These ultrathin crystals can increase the oxidation and wear resistance of copper.

    5. Delocalized Spin States in 2D Atomic Layers Realizing Enhanced Electrocatalytic Oxygen Evolution

      Shichuan Chen, Zhixiong Kang, Xin Hu, Xiaodong Zhang, Hui Wang, Junfeng Xie, XuSheng Zheng, Wensheng Yan, Bicai Pan and Yi Xie

      Version of Record online: 8 JUN 2017 | DOI: 10.1002/adma.201701687

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      Delocalized spin states in transition-metal-based compounds by introducing structural distortion to their confined 2D atomic layers can enhance activity in electrocatalytic oxygen evolution. This work establishes new way for the design of advanced electrocatalysts in transition-metal-based compounds via regulation of spin states.

    6. 3D Printing by Multiphase Silicone/Water Capillary Inks

      Sangchul Roh, Dishit P. Parekh, Bhuvnesh Bharti, Simeon D. Stoyanov and Orlin D. Velev

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201701554

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      An efficient technique for fabricating multiphase 3D printable polydimethylsiloxane (PDMS) ink is introduced. The ink is a capillary suspension consisting of PDMS microbeads (cured), PDMS liquid precursor (uncured), and water (continuous phase). Upon curing, the printed PDMS ink becomes highly porous, elastic, flexible, and extensible, which promises industrial applications such as biomedical products and bioscaffolds.

    7. Phase-Transformation Ductilization of Brittle High-Entropy Alloys via Metastability Engineering

      Hailong Huang, Yuan Wu, Junyang He, Hui Wang, Xiongjun Liu, Ke An, Wei Wu and Zhaoping Lu

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201701678

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      The “metastability-engineering” strategy is exploited in brittle body-centered cubic high-entropy alloys (HEAs) via tailoring the thermal and mechanical stability of the constituent phases, and consequently, transformation-induced ductility and work hardening capability are successfully achieved. This not only has important implications for developing high-performance HEAs, but also sheds light on overcoming the long-standing strength–ductility tradeoff of metallic materials in general.

    8. 3R MoS2 with Broken Inversion Symmetry: A Promising Ultrathin Nonlinear Optical Device

      Jia Shi, Peng Yu, Fucai Liu, Peng He, Rui Wang, Liang Qin, Junbo Zhou, Xin Li, Jiadong Zhou, Xinyu Sui, Shuai Zhang, Yanfeng Zhang, Qing Zhang, Tze Chien Sum, Xiaohui Qiu, Zheng Liu and Xinfeng Liu

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201701486

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      A 2D van der Waals crystal (3R MoS2) can serve as a promising ultrathin nanoscale frequency doubling crystal under phase matching conditions. Thickness and wavelength-dependent second harmonic generation spectrum of 3R MoS2 offers the selection rules of appropriate working conditions. Polarization enhancement with two petals along staggered stacking direction appears in 3R MoS2 is observed.

    9. Controllable Dynamic Zigzag Pattern Formation in a Soft Helical Superstructure

      Zhi-gang Zheng, Rafael S. Zola, Hari Krishna Bisoyi, Ling Wang, Yannian Li, Timothy J. Bunning and Quan Li

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201701903

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      Controllable dynamic zigzag-shaped pattern formation in a photoresponsive soft self-organized helical superstructure is accomplished via the coupled stimuli effect of electric field and light, which has enabled a unique diffraction pattern not found before.

    10. Water-Plasma-Enabled Exfoliation of Ultrathin Layered Double Hydroxide Nanosheets with Multivacancies for Water Oxidation

      Rong Liu, Yanyong Wang, Dongdong Liu, Yuqin Zou and Shuangyin Wang

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201701546

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      Ultrathin CoFe layered double hydroxide nanosheets with multivacancies are prepared by water-plasma-enabled exfoliation. The water plasma can destroy the electrostatic interactions between the host metal layers and the interlayer cations, resulting in fast exfoliation. The etching effect of plasma can simultaneously produce multivacancies. The increased active sites and the multivacancies significantly contribute to the enhanced electrocatalytic activity for OER.

    11. Self-Regulating Iris Based on Light-Actuated Liquid Crystal Elastomer

      Hao Zeng, Owies M. Wani, Piotr Wasylczyk, Radosław Kaczmarek and Arri Priimagi

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201701814

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      The iris is a biological tissue that can change the pupil size to stabilize the light transmission into the eye. An iris-inspired soft device is reported that can automatically adjust aperture size in response to the change of incident light intensity. The device is made of radially photoaligned liquid crystal elastomer, using anisotropic thermal expansion to realize the desired photoactuation mode.

    12. Highly Anisotropic Sb2Se3 Nanosheets: Gentle Exfoliation from the Bulk Precursors Possessing 1D Crystal Structure

      Huaibing Song, Tiaoyang Li, Jia Zhang, Ying Zhou, Jiajun Luo, Chao Chen, Bo Yang, Cong Ge, Yanqing Wu and Jiang Tang

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201700441

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      Anisotropic Sb2Se3 nanosheets are exfoliated from bulk Sb2Se3 possessing 1D crystal structure, and their photoconductive photodetectors reveal strong responsivity and highly anisotropic in-plane transport.

    13. Benzothiazolium Single Crystals: A New Class of Nonlinear Optical Crystals with Efficient THz Wave Generation

      Seung-Heon Lee, Jian Lu, Seung-Jun Lee, Jae-Hyun Han, Chan-Uk Jeong, Seung-Chul Lee, Xian Li, Mojca Jazbinšek, Woojin Yoon, Hoseop Yun, Bong Joo Kang, Fabian Rotermund, Keith A. Nelson and O-Pil Kwon

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201701748

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      A new class of nonlinear optical crystals introducing benzothiazolium exhibit large macroscopic optical nonlinearity with optimal molecular ordering and suitable crystal characteristics for intense terahertz (THz) wave generation. This results in one order of magnitude higher THz wave generation efficiency with considerably broader bandwidth than inorganic standard ZnTe crystal when pumped at the technologically important wavelength of 800 nm.

    14. Observation of Various and Spontaneous Magnetic Skyrmionic Bubbles at Room Temperature in a Frustrated Kagome Magnet with Uniaxial Magnetic Anisotropy

      Zhipeng Hou, Weijun Ren, Bei Ding, Guizhou Xu, Yue Wang, Bing Yang, Qiang Zhang, Ying Zhang, Enke Liu, Feng Xu, Wenhong Wang, Guangheng Wu, Xixiang Zhang, Baogen Shen and Zhidong Zhang

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201701144

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      Various and spontaneous magnetic skyrmionic bubbles are observed for the first time at room temperature in a frustrated kagome Fe3Sn2 magnet. The magnetization dynamics are investigated using Lorentz transmission electron microscopy, revealing that transformations between different bubbles are via motion of Bloch lines driven by the magnetic field. These results demonstrate that Fe3Sn2 facilitates control of topological spin textures at room temperature.

    15. Small-Molecule Solar Cells with Simultaneously Enhanced Short-Circuit Current and Fill Factor to Achieve 11% Efficiency

      Li Nian, Ke Gao, Yufeng Jiang, Qikun Rong, Xiaowen Hu, Dong Yuan, Feng Liu, Xiaobin Peng, Thomas P. Russell and Guofu Zhou

      Version of Record online: 7 JUN 2017 | DOI: 10.1002/adma.201700616

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      High-efficiency all-small-molecule organic solar cells using two electron donors with distinctively different absorption and structural features are reported. Such a combination works well and synergically improves device current and fill factor, yielding a milestone efficiency of 10.97%.

    16. Enhancing Photodynamic Therapy through Resonance Energy Transfer Constructed Near-Infrared Photosensitized Nanoparticles

      Ling Huang, Zhanjun Li, Yang Zhao, Jinyi Yang, Yucheng Yang, Aarushi Iris Pendharkar, Yuanwei Zhang, Sharon Kelmar, Liyong Chen, Wenting Wu, Jianzhang Zhao and Gang Han

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201604789

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      Resonance energy transfer constructed NIR-absorbing BODIPY-based photosensitized dyad nanoparticles are developed. These nanoparticles enable targeted photodynamic therapy upon application of low-power NIR LED light irradiation. This work provides a new concept for the design of biocompatible nanoparticles with significantly improved NIR sensitivity, which is key to photodynamic therapy development.

    17. Tunable Photocontrolled Motions Using Stored Strain Energy in Malleable Azobenzene Liquid Crystalline Polymer Actuators

      Xili Lu, Shengwei Guo, Xia Tong, Hesheng Xia and Yue Zhao

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201606467

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      By prestoring mechanical strain energy in a reprocessable liquid crystal polymer network containing azobenzene mesogens, unprecedented mechanical force can be generated under UV light irradiation, which enables continuous light-driven motions of large polymer actuators in the form of wheels and spring-like “motors,” with tunable moving speed and controllable moving direction.

    18. Bioinspired Ultrastrong Solid Electrolytes with Fast Proton Conduction along 2D Channels

      Guangwei He, Mingzhao Xu, Jing Zhao, Shengtao Jiang, Shaofei Wang, Zhen Li, Xueyi He, Tong Huang, Moyuan Cao, Hong Wu, Michael D. Guiver and Zhongyi Jiang

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201605898

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      The advancement of solid electrolytes is severely impeded by the strong tradeoff relationship between ion-conduction and mechanical properties. Through integrating 2D channels and “brick-and-mortar” architecture into one materials system, an unprecedented combination of high proton conductivity and superior mechanical strength are achieved. This intriguing design may pave the way for the bioinspired design of next-generation high-performance solid electrolytes.

  2. Reviews

    1. Reviving Lithium-Metal Anodes for Next-Generation High-Energy Batteries

      Yanpeng Guo, Huiqiao Li and Tianyou Zhai

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700007

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      Dendrite growth, continuous side reactions, and infinite volume changes inside a lithium-metal anode severely hamper its application in high-energy batteries. Concrete failure mechanisms and effective strategies, including lowering the local current density, reducing anion depletion, smoothing interfaces, reshaping the lithium-ion flux, and mechanically blocking dendrites, are comprehensively reviewed.

  3. Communications

    1. Reliable Piezoelectricity in Bilayer WSe2 for Piezoelectric Nanogenerators

      Ju-Hyuck Lee, Jae Young Park, Eun Bi Cho, Tae Yun Kim, Sang A. Han, Tae-Ho Kim, Yanan Liu, Sung Kyun Kim, Chang Jae Roh, Hong-Joon Yoon, Hanjun Ryu, Wanchul Seung, Jong Seok Lee, Jaichan Lee and Sang-Woo Kim

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201606667

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      WSe2 bilayers with turbostratic stacking have reliable piezoelectric properties that cannot be obtained from a WSe2 monolayer. The flexible piezoelectric WSe2 bilayers exhibit a prominent mechanical durability of up to 0.95% of strain as well as reliable energy harvesting performance, which is adequate to drive a small liquid crystal display without external energy sources.

    2. Discovery of Rapid and Reversible Water Insertion in Rare Earth Sulfates: A New Process for Thermochemical Heat Storage

      Naoyuki Hatada, Kunihiko Shizume and Tetsuya Uda

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201606569

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      Water molecules can be inserted in crystalline rare earth sulfates such as La2(SO4)3 without phase change, accompanied by heat release. Since the reaction proceeds rapidly and reversibly upon changing temperature and water vapor pressure in the temperature range 50–250 °C, it will be a promising process for thermal energy storage, especially for low-grade waste heat and solar energy.

    3. Orientational Coupling Locally Orchestrates a Cell Migration Pattern for Re-Epithelialization

      Benhui Hu, Wan Ru Leow, Shahrouz Amini, Brenda Nai, Xiaoqian Zhang, Zhiyuan Liu, Pingqiang Cai, Zhuyun Li, Yun-Long Wu, Ali Miserez, Chwee Teck Lim and Xiaodong Chen

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700145

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      The spatial organization of adjacent adherent paths within sparsely distributed extracellular matrix (ECM) has a significant impact on the orientational coupling between cell polarization and collective cell migration for wound healing. This coupling effect determines the migration pattern and thus the efficiency for human keratinocytes to regain their cohesion. The findings may help to design an implantable ECM to optimize tissue regeneration.

    4. Graphitized Carbon Fibers as Multifunctional 3D Current Collectors for High Areal Capacity Li Anodes

      Tong-Tong Zuo, Xiong-Wei Wu, Chun-Peng Yang, Ya-Xia Yin, Huan Ye, Nian-Wu Li and Yu-Guo Guo

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700389

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      Graphitized carbon fiber electrode is demonstrated to improve the cycling performance of high-areal-capacity Li anodes due to dual reaction types, reduced current density, and confined volume change. This Li anode can deliver a high areal capacity of 8 mA h cm−2 without Li dendrites and displays low voltage hysteresis, high plating/stripping efficiency, and long cycling lifespan.

    5. Hierarchical Co(OH)F Superstructure Built by Low-Dimensional Substructures for Electrocatalytic Water Oxidation

      Shanhong Wan, Jing Qi, Wei Zhang, Weina Wang, Shaokang Zhang, Kaiqiang Liu, Haoquan Zheng, Junliang Sun, Shuangyin Wang and Rui Cao

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700286

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      3D Co(OH)F microspheres are synthesized for highly efficient electrocatalytic water oxidation. The microspheres are built by 2D nanoflake building blocks, which are further woven by 1D nanorod foundations. The hierarchical structure of this free-standing Co(OH)F material combines the merits of all material dimensions in heterogeneous catalysis.

    6. Postsynthetic Doping of MnCl2 Molecules into Preformed CsPbBr3 Perovskite Nanocrystals via a Halide Exchange-Driven Cation Exchange

      Guangguang Huang, Chunlei Wang, Shuhong Xu, Shenfei Zong, Ju Lu, Zhuyuan Wang, Changgui Lu and Yiping Cui

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700095

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      A novel halide exchange-driven cation exchange strategy is developed to prepare dually emitting Mn-doped CsPb(Cl/Br)3 nanocrystals (NCs). The key is the simultaneous reactions of halide exchange and cation exchange at the same time and lattice site, which can be satisfied only by direct doping of MnCl2 molecules into NCs.

    7. Manganese-Based Layered Double Hydroxide Nanoparticles as a T1-MRI Contrast Agent with Ultrasensitive pH Response and High Relaxivity

      Bei Li, Zi Gu, Nyoman Kurniawan, Weiyu Chen and Zhi Ping Xu

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700373

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      Novel Mn-based layered double hydroxide (Mn-LDH) nanoparticles show excellent magnetic resonance imaging capacity with outstanding pH-ultrasensitivity at pH 7.4–6.5 and superb longitudinal relaxivity. These Mn-LDH nanoparticles are able to clearly image tumor tissue for 2 d in vivo. Together with demonstrated capacity for drug and gene delivery, Mn-LDH nanomaterials are potential theranostic agents for cancer treatment.

    8. Modulation of Metal and Insulator States in 2D Ferromagnetic VS2 by van der Waals Interaction Engineering

      Yuqiao Guo, Haitao Deng, Xu Sun, Xiuling Li, Jiyin Zhao, Junchi Wu, Wangsheng Chu, Sijia Zhang, Haibin Pan, Xusheng Zheng, Xiaojun Wu, Changqing Jin, Changzheng Wu and Yi Xie

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700715

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      Van der Waals interaction engineering in VS2 brings the first intrinsic ferromagnetic semiconductor in 2D transition-metal dichalcogenides (TMDCs). An experimental realization of intrinsic magnetic ordering in a pristine TMDC lattice is reported. The pristine VS2 lattice provides a new platform for precise manipulation of both charge and spin degrees of freedom in 2D TMDCs, availing spintronic applications.

    9. A Game Changer: A Multifunctional Perovskite Exhibiting Giant Ferroelectricity and Narrow Bandgap with Potential Application in a Truly Monolithic Multienergy Harvester or Sensor

      Yang Bai, Pavel Tofel, Jaakko Palosaari, Heli Jantunen and Jari Juuti

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700767

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      A multifunctional perovskite composition exhibiting giant ferroelectricity and narrow bandgap is reported. Ceramics and thick-films are fabricated via solid-state reaction and laser machining, respectively. Their balanced piezoelectric, pyroelectric, and photovoltaic properties and the multitask feature pave the way to the development of all-in-one multisource energy harvesting and multifunctional sensing devices based on the simplest solution of materials and structures.

    10. Synthesis of Ultrathin PdCu Alloy Nanosheets Used as a Highly Efficient Electrocatalyst for Formic Acid Oxidation

      Nailiang Yang, Zhicheng Zhang, Bo Chen, Ying Huang, Junze Chen, Zhuangchai Lai, Ye Chen, Melinda Sindoro, An-Liang Wang, Hongfei Cheng, Zhanxi Fan, Xiaozhi Liu, Bing Li, Yun Zong, Lin Gu and Hua Zhang

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700769

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      Ultrathin PdCu alloy nanosheets are synthesized via a facile wet-chemistry method. These nanosheets after being treated with ethylenediamine exhibit superior electrocatalytic activity toward formic acid oxidation.

    11. Confining the Nucleation of Pt to In Situ Form (Pt-Enriched Cage)@CeO2 Core@Shell Nanostructure as Excellent Catalysts for Hydrogenation Reactions

      Songyan Song, Xianchun Liu, Junqi Li, Jing Pan, Fan Wang, Yan Xing, Xiao Wang, Xiaogang Liu and Hongjie Zhang

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700495

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      High-quality CeO2-encapsulated Pt-enriched cages with ultrathin walls are successfully synthesized via a kinetic-controlled process. The products exhibit enhanced catalytic activity and selectivity for cinnamaldehyde hydrogenation reaction among the different CeO2-based core@shell samples.

    12. Metasurfaces and Colloidal Suspensions Composed of 3D Chiral Si Nanoresonators

      Ruggero Verre, Lei Shao, Nils Odebo Länk, Pawel Karpinski, Andrew B. Yankovich, Tomasz J. Antosiewicz, Eva Olsson and Mikael Käll

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701352

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      3D film structuring and a novel gradient mask transfer technique are combined to fabricate the first intrinsically chiral dielectric metasurface in the form of a monolayer of twisted silicon nanocrescents that can be easily detached and dissolved into colloidal suspension.

    13. Structurally and Functionally Optimized Silk-Fibroin–Gelatin Scaffold Using 3D Printing to Repair Cartilage Injury In Vitro and In Vivo

      Weili Shi, Muyang Sun, Xiaoqing Hu, Bo Ren, Jin Cheng, Chenxi Li, Xiaoning Duan, Xin Fu, Jiying Zhang, Haifeng Chen and Yingfang Ao

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701089

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      A structurally and functionally optimized scaffold is designed for knee cartilage regeneration by integrating silk fibroin with gelatin in combination with bone-marrow-stem-cell (BMSC)-specific-affinity peptide using 3D printing technology. This dually optimized scaffold can efficiently recruit endogenic BMSCs and provide a suitable microenvironment for neocartilage formation, thus successfully achieving regeneration of cartilage in a knee joint.

    14. Approaching Intra- and Interchain Charge Transport of Conjugated Polymers Facilely by Topochemical Polymerized Single Crystals

      Yifan Yao, Huanli Dong, Feng Liu, Thomas P. Russell and Wenping Hu

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701251

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      High-quality conjugated-polymer crystals with extended conjugation and exceptionally high degree of molecular order are obtained through a modified topochemical polymerization method. For the first time, the fundamental studies of intra- and interchain charge transport based on an individual polymer crystal are approached, giving a high carrier mobility up to 50 cm2 V−1 s−1 along the backbones, which is two orders of magnitude greater than that in the interchain direction.

    15. Ultrafast Growth of High-Quality Monolayer WSe2 on Au

      Yang Gao, Yi-Lun Hong, Li-Chang Yin, Zhangting Wu, Zhiqing Yang, Mao-Lin Chen, Zhibo Liu, Teng Ma, Dong-Ming Sun, Zhenhua Ni, Xiu-Liang Ma, Hui-Ming Cheng and Wencai Ren

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700990

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      Ultrafast growth of high-quality uniform monolayer WSe2 is achieved by chemical vapor deposition using Au as a reusable substrate. The growth rate is ≈2–3 orders of magnitude faster than those reported due to the small energy barriers and exothermic characteristic, and the materials show excellent crystal quality and extraordinary electrical properties comparable to those of exfoliated samples.

    16. A High-Performance Li–O2 Battery with a Strongly Solvating Hexamethylphosphoramide Electrolyte and a LiPON-Protected Lithium Anode

      Bin Zhou, Limin Guo, Yantao Zhang, Jiawei Wang, Lipo Ma, Wen-Hua Zhang, Zhengwen Fu and Zhangquan Peng

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701568

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      A high-performance Li–O2 battery is realized by employing a strongly solvating hexamethylphosphoramide (HMPA) electrolyte that can effectively dissolve Li2O2 and a LiPON-protected lithium anode that can be reversibly cycled in HMPA electrolyte. A combination of advanced research techniques provide compelling evidence that operation of the HMPA-based Li–O2 battery is backed by nearly reversible formation/decomposition of Li2O2 with negligible side reactions.

    17. A Supramolecular Artificial Light-Harvesting System with an Ultrahigh Antenna Effect

      Jing-Jing Li, Yong Chen, Jie Yu, Ni Cheng and Yu Liu

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701905

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      An efficient artificial light-harvesting system is fabricated based on a supramolecular strategy in aqueous solution. In this system, the supramolecular assembly acts as a donor, and nile red that is loaded into the assembly acts as acceptor. Significantly, an efficient energy-transfer process occurs between the assembly and the loaded nile red, leading to an extremely high antenna effect.

    18. Piezo-Phototronic Effect on Selective Electron or Hole Transport through Depletion Region of Vis–NIR Broadband Photodiode

      Haiyang Zou, Xiaogan Li, Wenbo Peng, Wenzhuo Wu, Ruomeng Yu, Changsheng Wu, Wenbo Ding, Fei Hu, Ruiyuan Liu, Yunlong Zi and Zhong Lin Wang

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701412

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      A high-performance p-Si/n-ZnO broadband photodiode is fabricated, working in a wide wavelength range from visible to near-infrared light. The photodiode is illuminated with different wavelengths to selectively choose the photogenerated charge carriers (either electrons or holes) passing through the depletion region. This enables the possibility to investigate the piezo-phototronic effect on performance in two cases separately for the first time.

    19. Giant Ferroelectric Polarization in Ultrathin Ferroelectrics via Boundary-Condition Engineering

      Lin Xie, Linze Li, Colin A. Heikes, Yi Zhang, Zijian Hong, Peng Gao, Christopher T. Nelson, Fei Xue, Emmanouil Kioupakis, Longqing Chen, Darrel G. Schlom, Peng Wang and Xiaoqing Pan

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701475

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      A giant enhancement of ferroelectric polarization in ultrathin 2 nm BiFeO3 film is reported. With the addition of a Bi2O3−x monolayer on the surface of ferroelectric BiFeO3 thin films, the ferroelectric polarization of the ultrathin BiFeO3 film is stabilized and dramatically increased up to ≈150 µC cm−2, demonstrating the possibility of enhancing the performance of ferroelectric materials at the reduced dimension.

    20. Electric-Field-Controlled Dopant Distribution in Organic Semiconductors

      Lars Müller, Seon-Young Rhim, Vipilan Sivanesan, Dongxiang Wang, Sebastian Hietzschold, Patrick Reiser, Eric Mankel, Sebastian Beck, Stephen Barlow, Seth R. Marder, Annemarie Pucci, Wolfgang Kowalsky and Robert Lovrincic

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701466

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      The electric-field-controlled movement of dopants in organic semiconductors is investigated with electrical measurements, optical microscopy, and spatially resolved infrared spectroscopy. This study evaluates two p-type dopants in a polymer and small molecule host material and utilizes the movement to build a proof-of-concept memristive device by reversibly changing the overall conductivity of thin films.

    21. Real-Time Observation of Carbon Nanotube Etching Process Using Polarized Optical Microscope

      Qiuchen Zhao, Fengrui Yao, Zequn Wang, Shibin Deng, Lianming Tong, Kaihui Liu and Jin Zhang

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701959

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      A hot-wall chemical reactor equipped with a polarized optical microscope is used to realize in situ real-time observation of the etching process in carbon nanotubes, and a “random etching” behavior is discovered. It is revealed that the random behavior reflects the unique “self-termination” phenomenon. Kinetic mechanism of single-walled carbon nanotube etching process is also discussed.

    22. Homogeneous 2D MoTe2 p–n Junctions and CMOS Inverters formed by Atomic-Layer-Deposition-Induced Doping

      June Yeong Lim, Atiye Pezeshki, Sehoon Oh, Jin Sung Kim, Young Tack Lee, Sanghyuck Yu, Do Kyung Hwang, Gwan-Hyoung Lee, Hyoung Joon Choi and Seongil Im

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701798

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      Homogeneous 2D MoTe2 p–n junction and complementary metal–oxide–semiconductor (CMOS) inverters integrated by selective n-type doping are demonstrated, which are obtained by H-diffusion during atomic layer deposition on initial p-type MoTe2. This 2D α-MoTe2 CMOS inverters with a p–n junction exhibits promising static and dynamic performances, forecasting future prospects to overcome the limits of 3D Si CMOS.

    23. The Optical Janus Effect: Asymmetric Structural Color Reflection Materials

      Grant T. England, Calvin Russell, Elijah Shirman, Theresa Kay, Nicolas Vogel and Joanna Aizenberg

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201606876

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      Viewing-direction-dependent reflected color is rationally designed and patterned to create several different types of asymmetric structural color films using a variety of fabrication methods and materials. The reflection properties of these materials are calculated analytically a priori to enable a diverse array of color combinations and effects to be created.

    24. Carbon Nanotubes as an Ultrafast Emitter with a Narrow Energy Spread at Optical Frequency

      Chi Li, Xu Zhou, Feng Zhai, Zhenjun Li, Fengrui Yao, Ruixi Qiao, Ke Chen, Matthew Thomas Cole, Dapeng Yu, Zhipei Sun, Kaihui Liu and Qing Dai

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201701580

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      Field-driven photoemission sources based on metal tips allow ultrafast characterization with ultimate spatio–temporal resolution, but suffer large energy spreads (>3 eV). Photoemission from carbon nanotubes excited by a 410 nm femtosecond laser is realized in the field-driven regime with a 0.25 eV energy spread, which benefits from the high field enhancement and great stability of the carbon nanotubes.

    25. A Molecular Polycrystalline Ferroelectric with Record-High Phase Transition Temperature

      Qiang Pan, Zhi-Bo Liu, Han-Yue Zhang, Wan-Ying Zhang, Yuan-Yuan Tang, Yu-Meng You, Peng-Fei Li, Wei-Qiang Liao, Ping-Ping Shi, Rong-Wei Ma, Ru-Yuan Wei and Ren-Gen Xiong

      Version of Record online: 6 JUN 2017 | DOI: 10.1002/adma.201700831

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      Guanidinium perchlorate is found to show multiaxial ferroelectricity with extremly low coercive field. Its polycrystalline samples show properties similar to those in ceramic ferroelectrics, such as switchable polarization and piezoelectric coefficient for the powder-pressed plates.

  4. Reviews

    1. Endeavor of Iontronics: From Fundamentals to Applications of Ion-Controlled Electronics

      Satria Zulkarnaen Bisri, Sunao Shimizu, Masaki Nakano and Yoshihiro Iwasa

      Version of Record online: 5 JUN 2017 | DOI: 10.1002/adma.201607054

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      Iontronics bridges the two worlds of electronics and ionics at the interface of electronic conductors and ionic conductors. Recent progress in this emerging field is highlighted from both the fundamental material science aspects and application perspectives. This includes the discovery of new physics and of the emerging functionality of ion-controlled electronics for thermoelectrics, neuromorphic devices, and flexible electronics.

  5. Communications

    1. Control of Circularly Polarized Electroluminescence in Induced Twist Structure of Conjugate Polymer

      Dong-Myung Lee, Jin-Wook Song, Yu-Jin Lee, Chang-Jae Yu and Jae-Hoon Kim

      Version of Record online: 5 JUN 2017 | DOI: 10.1002/adma.201700907

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      Highly circularly polarized electroluminescence (|gEL| = 1.13) is generated from twisted stacking of achiral conjugated polymer induced by nonemitting chiral dopant of high helical twisting power. The location of the recombination zone is a crucial parameter for determining the degree of circular polarization. The result is applied to an organic light-emitting display to improve the luminous efficiency by 60%.

    2. Iodine Vacancy Redistribution in Organic–Inorganic Halide Perovskite Films and Resistive Switching Effects

      Xiaojian Zhu, Jihang Lee and Wei D. Lu

      Version of Record online: 5 JUN 2017 | DOI: 10.1002/adma.201700527

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      Electric field and light illumination controlled iodine vacancy (VI) redistribution and resistive switching effects are demonstrated in organic–inorganic halide perovskite films. The diffusion energy barrier of VI is ≈0.17 eV. The VI diffusion dynamics can be modulated through engineering the anode material and controlling illumination conditions. An electrical-write and optical-erase memory element is demonstrated.

    3. Stimuli-Responsive, Shape-Transforming Nanostructured Particles

      Junhyuk Lee, Kang Hee Ku, Mingoo Kim, Jae Man Shin, Junghun Han, Chan Ho Park, Gi-Ra Yi, Se Gyu Jang and Bumjoon J. Kim

      Version of Record online: 5 JUN 2017 | DOI: 10.1002/adma.201700608

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      Dynamic, temperature-driven transformation of the shape and morphology of polymer particles is demonstrated using polystyrene-b-poly(4-vinylpyridine) block copolymers (BCPs) and temperature-responsive poly(N-isopropylacrylamide) (PNIPAM) surfactants. The temperature-directed positioning of PNIPAM depending on its solubility determines both the shape and morphology of the BCP particles, suggesting great promise of these particles for use in sensing, smart coatings, and drug delivery applications.

    4. Indium Phosphide-Based Quantum Dots with Shell-Enhanced Absorption for Luminescent Down-Conversion

      Dorian Dupont, Mickael D. Tessier, Philippe F. Smet and Zeger Hens

      Version of Record online: 5 JUN 2017 | DOI: 10.1002/adma.201700686

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      InP-based quantum dots (QDs) with shell-enhanced absorption for more efficient luminescent down-conversion are proposed. Synthetic methods to coat InP QDs with a ZnSe shell containing small amounts of Cd are developed. This allows the QD absorption at 450 nm, the typical pump wavelength for optical down-conversion, to be enhanced, and concomitantly suppresses self-absorption and reduces QD loading in QD-in-polymer-based luminescent down-convertor coatings.

    5. You have full text access to this OnlineOpen article
      Electrostatic Mechanophores in Tuneable Light-Emitting Piezopolymer Nanowires

      Luana Persano, Andrea Camposeo, Aleksandr V. Terentjevs, Fabio Della Sala, Eduardo Fabiano, Martina Montinaro and Dario Pisignano

      Version of Record online: 1 JUN 2017 | DOI: 10.1002/adma.201701031

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      Electromechanical coupling through piezoelectric polymers tunes the emission of organic molecules in active nanowires. Highly bendable arrays of counter-ion dye-doped wires made of a poly(vinylidenefluoride) copolymer are realized, which show a reversible shift of the emission upon applying dynamic stress during bending. Electrostatic mechanophores may provide anisotropic molecular systems with an optical sensing capability for monitoring local stress and damage in transparent materials, optoelectronics, and soft robotics.

    6. High-Contrast Fluorescence Detection of Metastatic Breast Cancer Including Bone and Liver Micrometastases via Size-Controlled pH-Activatable Water-Soluble Probes

      Hu Xiong, Hao Zuo, Yunfeng Yan, Gino Occhialini, Kejin Zhou, Yihong Wan and Daniel J. Siegwart

      Version of Record online: 31 MAY 2017 | DOI: 10.1002/adma.201700131

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      Size-controlled pH activatable probes can universally detect both primary tumor and breast cancer metastases in the liver, lung, pancreas, and kidneys. Covalent functionalization with bisphosphonate successfully enhances bone metastasis imaging and simultaneously illuminates micrometastases in the liver with high signal-to-noise ratio.

    7. Ultrahigh and Selective SO2 Uptake in Inorganic Anion-Pillared Hybrid Porous Materials

      Xili Cui, Qiwei Yang, Lifeng Yang, Rajamani Krishna, Zhiguo Zhang, Zongbi Bao, Hui Wu, Qilong Ren, Wei Zhou, Banglin Chen and Huabin Xing

      Version of Record online: 31 MAY 2017 | DOI: 10.1002/adma.201606929

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      Selective recognition and dense packing of SO2 clusters through multiple synergistic host–guest and guest–guest interactions within SiF62−-anion-pillared hybrid porous materials sets new benchmarks for SO2 capture. The binding sites of anions and aromatic rings in SIFSIX materials grasp every atom of SO2 firmly via Sδ+···Fδ− electrostatic interactions and Oδ−···Hδ+ dipole–dipole interactions.

    8. You have full text access to this OnlineOpen article
      Crystallization Kinetics and Morphology Control of Formamidinium–Cesium Mixed-Cation Lead Mixed-Halide Perovskite via Tunability of the Colloidal Precursor Solution

      David P. McMeekin, Zhiping Wang, Waqaas Rehman, Federico Pulvirenti, Jay B. Patel, Nakita K. Noel, Michael B. Johnston, Seth R. Marder, Laura M. Herz and Henry J. Snaith

      Version of Record online: 31 MAY 2017 | DOI: 10.1002/adma.201607039

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      The dissolution of colloids that are present in the formamidinium–cesium perovskite ([HC(NH2)2]0.83Cs0.17Pb(Br0.2I0.8)3) precursor solution is triggered with the addition of hydrohalic acids. Dynamic light scattering intensity measurement shows the gradual dissolution of these colloids over a period of time. These colloids impact the morphology, crystal quality, and optoelectronic properties of the perovskite, leading to improvements in solar-cell efficiency.

    9. You have full text access to this OnlineOpen article
      Electron Hopping Across Hemin-Doped Serum Albumin Mats on Centimeter-Length Scales

      Nadav Amdursky, Xuhua Wang, Paul Meredith, D. Jason Riley, David J. Payne, Donal D. C. Bradley and Molly M. Stevens

      Version of Record online: 31 MAY 2017 | DOI: 10.1002/adma.201700810

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      Protein-based free-standing mats can be used as macroscopic electron mediators. This study demonstrates how molecular doping of protein mats with hemin permits electron hopping between hemin molecules and results in the highest measured centimeter-length conductance for a protein-based material yet reported. The hemin-doped protein mats display both biocompatibility and fabrication simplicity, which present advantages for their use in bioelectronic devices.

  6. Reviews

    1. Morphology-Conserved Transformations of Metal-Based Precursors to Hierarchically Porous Micro-/Nanostructures for Electrochemical Energy Conversion and Storage

      Min Chen, Yueguang Zhang, Lidan Xing, Youhao Liao, Yongcai Qiu, Shihe Yang and Weishan Li

      Version of Record online: 30 MAY 2017 | DOI: 10.1002/adma.201607015

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      Hierarchically porous micro-/nanostructures are favorable for enhancing electrochemical performances of energy conversion and storage devices. Hierarchically porous micro-/nanostructures produced by the morphology-conserved transformations of various metal-based precursors are summarized, and their applications as electrodes and/or catalysts in rechargeable batteries, supercapacitors, and solar cells, are systematically discussed.

  7. Communications

    1. A Strategy to Design High-Density Nanoscale Devices utilizing Vapor Deposition of Metal Halide Perovskite Materials

      Bohee Hwang and Jang-Sik Lee

      Version of Record online: 30 MAY 2017 | DOI: 10.1002/adma.201701048

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      Utilizing sequential vapor deposition, a CH3NH3PbI3-based nanoscale memory device that uses 250 nm via-hole structures and a CH3NH3PbI3-based cross-point array structure is demonstrated. The CH3NH3PbI3-based nanoscale resistive switching random access memory (ReRAM) shows fast switching speed, low operation voltage, good endurance, and long data retention. The proposed method paves the way for fabricating organic–inorganic perovskite-based nanoscale memories with complementary metal-oxide semiconductor (CMOS) compatibility.

    2. Simultaneous Enhancement of Charge Separation and Hole Transportation in a TiO2–SrTiO3 Core–Shell Nanowire Photoelectrochemical System

      Fei Wu, Yanhao Yu, Huang Yang, Lazarus N. German, Zhenquan Li, Jianguo Chen, Weiguang Yang, Lu Huang, Weimin Shi, Linjun Wang and Xudong Wang

      Version of Record online: 30 MAY 2017 | DOI: 10.1002/adma.201701432

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      In a TiO2–SrTiO3 core–shell nanowire photoelectrochemical (PEC) photoanode, the ferroelectric shell provides a spontaneous polarization to enhance charge separation. Meanwhile the favorable charge mobility in the shell also facilitates hole transport for water oxidation, leading to a significant enhancement of the PEC performance.

    3. Flexible and Responsive Chiral Nematic Cellulose Nanocrystal/Poly(ethylene glycol) Composite Films with Uniform and Tunable Structural Color

      Kun Yao, Qijun Meng, Vincent Bulone and Qi Zhou

      Version of Record online: 30 MAY 2017 | DOI: 10.1002/adma.201701323

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      Composite films of chiral nematic cellulose nanocrystals (CNCs) and poly(ethylene glycol) (PEG) with various uniform structural colors covering the entire visible spectrum are prepared by the intercalation of PEG between CNCs and subsequent formation of a layered helical structure upon drying. The CNC/PEG(80/20) composite film displays smooth and reversible structural color change between green and transparent when exposed to increasing and decreasing humidity conditions.

    4. Flyweight, Superelastic, Electrically Conductive, and Flame-Retardant 3D Multi-Nanolayer Graphene/Ceramic Metamaterial

      Qiangqiang Zhang, Dong Lin, Biwei Deng, Xiang Xu, Qiong Nian, Shengyu Jin, Kevin D. Leedy, Hui Li and Gary J. Cheng

      Version of Record online: 29 MAY 2017 | DOI: 10.1002/adma.201605506

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      A flyweight, superelastic, electrically conductive, and flame-retardant 3D multi-nanolayer graphene/ceramic metamaterial, with microstructure-derived superelasticity and structural robustness achieved by designing hierarchical honeycomb microstructures, assembles with multi-nanolayered cellular walls of graphene and Al2O3 ceramic that serve as basic functional strengthening and elastic units.

    5. 2D Porous Carbons prepared from Layered Organic–Inorganic Hybrids and their Use as Oxygen-Reduction Electrocatalysts

      Shuang Li, Chong Cheng, Hai-Wei Liang, Xinliang Feng and Arne Thomas

      Version of Record online: 29 MAY 2017 | DOI: 10.1002/adma.201700707

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      The formation of layered organic–inorganic hybrids and their subsequent pyrolysis is suggested as a universal and scalable strategy for the synthesis of 2D porous carbon nanosheets with well-defined 2D morphology, nanometer thickness, high surface area, and tunable heteroatom doping. These 2D carbon nanomaterials show remarkable electrocatalytic performances in the oxygen-reduction reaction and outperform commercial state-of-the-art Pt/C catalyst in zinc–air batteries.

  8. Progress Reports

    1. Tailoring Biomaterials for Cancer Immunotherapy: Emerging Trends and Future Outlook

      Chao Wang, Yanqi Ye, Quanyin Hu, Adriano Bellotti and Zhen Gu

      Version of Record online: 26 MAY 2017 | DOI: 10.1002/adma.201606036

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      Cancer immunotherapy has recently received tremendous attention and has created a paradigm shift in the treatment of cancer. An overview of the latest studies on tailoring biomaterials for enhancement of anticancer immunity is presented, including delivery of therapeutics to antigen-presenting cells, delivery of therapeutics to the tumor microenvironment, engineering of immune cells, and constructing immune scaffolds.

  9. Communications

    1. Precise Two-Photon Photodynamic Therapy using an Efficient Photosensitizer with Aggregation-Induced Emission Characteristics

      Bobo Gu, Wenbo Wu, Gaixia Xu, Guangxue Feng, Feng Yin, Peter Han Joo Chong, Junle Qu, Ken-Tye Yong and Bin Liu

      Version of Record online: 26 MAY 2017 | DOI: 10.1002/adma.201701076

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      A new two-photon photosensitizer is synthesized and formulated into organic dots with aggregation-induced emission characteristics, large two-photon absorption cross section, high reactive-oxygen-species generation efficiency, and excellent photostability and biocompatibility, enabling in vitro cancer cell ablation and in vivo brain-blood-vessel closure with 5 µm precision under two-photon excitation.

    2. Hierarchically Enhanced Impact Resistance of Bioinspired Composites

      Grace X. Gu, Mahdi Takaffoli and Markus J. Buehler

      Version of Record online: 26 MAY 2017 | DOI: 10.1002/adma.201700060

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      An order of magnitude tougher than nacre, conch shells are known for being one of the toughest biological body armors. However, the complexity of the conch shell architecture creates a barrier to emulating its cross-lamellar structure in synthetic materials. In this paper, a 3D biomimetic conch shell prototype is presented, which can replicate the crack arresting mechanisms embedded in the natural architecture.

    3. Printable and Rewritable Full Block Copolymer Structural Color

      Han Sol Kang, Jinseong Lee, Suk Man Cho, Tae Hyun Park, Min Ju Kim, Chanho Park, Seung Won Lee, Kang Lib Kim, Du Yeol Ryu, June Huh, Edwin L. Thomas and Cheolmin Park

      Version of Record online: 26 MAY 2017 | DOI: 10.1002/adma.201700084

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      An ink-jet printable and rewritable full-color structural color display is obtained by the position- and concentration-controlled deposition of a single, colorless, water-based ink containing a reversible crosslinking agent, ammonium persulfate, onto a self-assembled block copolymer photonic-crystal film. The information is quickly written and erased over 50 times with resolution nearly equivalent to a office ink-jet printer.

    4. Wet-Chemical Synthesis of Hollow Red-Phosphorus Nanospheres with Porous Shells as Anodes for High-Performance Lithium-Ion and Sodium-Ion Batteries

      Jianbin Zhou, Xianyu Liu, Wenlong Cai, Yongchun Zhu, Jianwen Liang, Kailong Zhang, Yang Lan, Zhuoheng Jiang, Gongming Wang and Yitai Qian

      Version of Record online: 26 MAY 2017 | DOI: 10.1002/adma.201700214

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      Preparing nanostructured phosphorus by a chemical synthetic approach is always challenging. A wet solvothermal method is developed to fabricate hollow phosphorous nanospheres (HPNs) with porous shells via a gas-bubble-directed formation mechanism. More importantly, due to the merits of porous and hollow structures, HPNs reveal excellent electrochemical performance as anodes for lithium-ion and sodium-ion batteries.

    5. Reduced Interface-Mediated Recombination for High Open-Circuit Voltages in CH3NH3PbI3 Solar Cells

      Christian M. Wolff, Fengshuo Zu, Andreas Paulke, Lorena Perdigón Toro, Norbert Koch and Dieter Neher

      Version of Record online: 26 MAY 2017 | DOI: 10.1002/adma.201700159

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      Perovskite solar cells have emerged as one of the most promising solar-cell technologies for the next generation of photovoltaics. Despite simple and cheap processing, the solar cells exhibit comparably little loss in open-circuit voltage. An approach to further reduce this loss by optimizing the charge selectivity of the fullerene-based electron contact in efficient devices is shown.

    6. Thermally Stable MAPbI3 Perovskite Solar Cells with Efficiency of 19.19% and Area over 1 cm2 achieved by Additive Engineering

      Yongzhen Wu, Fengxian Xie, Han Chen, Xudong Yang, Huimin Su, Molang Cai, Zhongmin Zhou, Takeshi Noda and Liyuan Han

      Version of Record online: 19 MAY 2017 | DOI: 10.1002/adma.201701073

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      By enhancing the crystalline quality of the simple and widely used MAPbI3 perovskite through additive engineering, unprecedented photovoltaic performance and thermal stability are achieved. A certified efficiency of 19.19% is obtained for devices with active area over 1 cm2, and the high-performing devices show unprecedented durability, maintaining >80% of the initial efficiency after 500 h of thermal aging at 85 °C.

  10. Progress Reports

    1. Towards Efficient Spectral Converters through Materials Design for Luminescent Solar Devices

      Barry McKenna and Rachel C. Evans

      Version of Record online: 19 MAY 2017 | DOI: 10.1002/adma.201606491

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      Sspectral converters can be applied to finished solar cells to overcome intrinsic non-absorption and thermalization losses and improve the device efficiency. Recent progress in the development of new materials for spectral conversion through luminescent downshifting, luminescent solar concentration, and upconversion is reviewed, with emphasis placed on their integration with emerging technologies, including perovskite, organic, and dye-sensitized solar cells.

  11. Communications

    1. Tuning of the Optical, Electronic, and Magnetic Properties of Boron Nitride Nanosheets with Oxygen Doping and Functionalization

      Qunhong Weng, Dmitry G. Kvashnin, Xi Wang, Ovidiu Cretu, Yijun Yang, Min Zhou, Chao Zhang, Dai-Ming Tang, Pavel B. Sorokin, Yoshio Bando and Dmitri Golberg

      Version of Record online: 19 MAY 2017 | DOI: 10.1002/adma.201700695

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      Intense oxygen doping and functionalization of hexagonal boron nitride (h-BN) nanosheets narrow the bandgap of the material from ≈5.5 to 2.1 eV in experiments, and lead to the appearance of paramagnetism and photoluminescence properties, which are not seen in h-BN. These findings pave a new way for the engineering of the optical, electronic, and magnetic properties of BN nanosheets.

    2. Bioinspired Composite Microfibers for Skin Adhesion and Signal Amplification of Wearable Sensors

      Dirk-M. Drotlef, Morteza Amjadi, Muhammad Yunusa and Metin Sitti

      Version of Record online: 19 MAY 2017 | DOI: 10.1002/adma.201701353

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      Strong adhesion of wearable sensors to dry and wet skin is proposed by a novel approach. Micropatterned adhesive films are composed of microfibers decorated with mushroom-shaped vinylsiloxane tips. Crosslinking the viscous tips directly on the skin significantly enhances the adhesion performance due to their great shape adaptation, which in turn highly increases the output signal quality of wearable strain sensors.

    3. Biphasic Supramolecular Self-Assembly of Ferric Ions and Tannic Acid across Interfaces for Nanofilm Formation

      Beom Jin Kim, Sol Han, Kyung-Bok Lee and Insung S. Choi

      Version of Record online: 19 MAY 2017 | DOI: 10.1002/adma.201700784

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      The biphasic interfacial supramolecular self-assembly of ferric ions (FeIII) and tannic acid in a heterogeneous system provides a powerful method for the formation of uniform and stable nanofilms in one step. The versatility of the synthetic strategy is demonstrated under various experimental settings (water–oil, hydrogel–water, and cell–water biphasic systems).

    4. Bioinspired Ultratough Hydrogel with Fast Recovery, Self-Healing, Injectability and Cytocompatibility

      Sara Azevedo, Ana M. S. Costa, Amanda Andersen, Insung S. Choi, Henrik Birkedal and João F. Mano

      Version of Record online: 19 MAY 2017 | DOI: 10.1002/adma.201700759

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      Inspired by the mussel byssus attachment system, a self-healable, ultratough and strong hydrogel is reported. The mild conditions employed during the fabrication process, as well as the use of nature-based materials, make it a prospective candidate for a wide range of applications including in the biomedical field.

    5. Synergistic Phase and Disorder Engineering in 1T-MoSe2 Nanosheets for Enhanced Hydrogen-Evolution Reaction

      Ying Yin, Yumin Zhang, Tangling Gao, Tai Yao, Xinghong Zhang, Jiecai Han, Xianjie Wang, Zhihua Zhang, Ping Xu, Peng Zhang, Xingzhong Cao, Bo Song and Song Jin

      Version of Record online: 19 MAY 2017 | DOI: 10.1002/adma.201700311

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      Synergistic regulation of crystal phase and disorder engineering in partially crystallized 1T phase MoSe2 nanosheets that are directly hydrothermally synthesized enhances catalytic activity toward the hydrogen-evolution reaction (HER). The optimized MoSe2 nanosheets exhibit a record-high HER catalytic activity, with η = 152 mV versus RHE for j = −10 mA cm−2 and a Tafel slope of 52 mV dec−1.

    6. Mushrooms as Efficient Solar Steam-Generation Devices

      Ning Xu, Xiaozhen Hu, Weichao Xu, Xiuqiang Li, Lin Zhou, Shining Zhu and Jia Zhu

      Version of Record online: 18 MAY 2017 | DOI: 10.1002/adma.201606762

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      Mushrooms can, surprisingly, enable efficient solar steam generation (≈78% under 1 sun illumination), as their natural structures possess the excellent properties of light absorption, thermal management with minimized heat loss, efficient water supply, and vapor escape.

    7. Core–Shell and Layer-by-Layer Assembly of 3D DNA Crystals

      Ronald McNeil Jr. and Paul J. Paukstelis

      Version of Record online: 18 MAY 2017 | DOI: 10.1002/adma.201701019

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      Multifunctional DNA-based biomaterial solids are generated through core–shell and layer-by-layer crystal growth. The isothermal self-assembly properties of the DNA crystal allow stepwise incorporation of functionally modified oligonucleotides to create layered periodic arrays of “guest” molecules, with each layer differentiated by the identity of the tethered guest molecules.

    8. An All-Plastic Field-Effect Nanofluidic Diode Gated by a Conducting Polymer Layer

      Gonzalo Pérez-Mitta, Waldemar A. Marmisollé, Christina Trautmann, María Eugenia Toimil-Molares and Omar Azzaroni

      Version of Record online: 18 MAY 2017 | DOI: 10.1002/adma.201700972

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      The integration of conductive poly(3,4-ethylenedioxythiophene) (PEDOT) into asymmetric solid-state nanopores leads the way to the construction of all-plastic field-effect nanofluidic diodes. The conducting layer acts as a gate electrode by changing its electrochemical state upon the application of different voltages. PEDOT-based electrochemically addressable nanofluidic devices display three well-defined voltage-controlled transport regimes: cation-rectifying, nonrectifying, and anion rectifying regimes.

    9. Regulating Water-Reduction Kinetics in Cobalt Phosphide for Enhancing HER Catalytic Activity in Alkaline Solution

      Kun Xu, Hui Ding, Mengxing Zhang, Min Chen, Zikai Hao, Lidong Zhang, Changzheng Wu and Yi Xie

      Version of Record online: 17 MAY 2017 | DOI: 10.1002/adma.201606980

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      Developing highly efficient electrocatalysts in an alkaline electrolyte for the hydrogen-evolution reaction (HER) is significant for realizing efficient overall water splitting. The coordinative effect of engineering a water dissociation step and the hydrogen adsorption free energy in Co2P by oxygen incorporation can lead to 15 times enhancement of the HER catalytic activity in alkaline solution. A new strategy for the design of advanced alkaline HER electrocatalysts is thus provided.

    10. Self-Adjusting, Polymeric Multilayered Roll that can Keep the Shapes of the Blood Vessel Scaffolds during Biodegradation

      Shiyu Cheng, Yu Jin, Nuoxin Wang, Feng Cao, Wei Zhang, Wei Bai, Wenfu Zheng and Xingyu Jiang

      Version of Record online: 17 MAY 2017 | DOI: 10.1002/adma.201700171

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      A method to fabricate a self-adjusting, blood vessel-mimicking, multilayered structure with two polymers, poly(ε-caprolactone) (PCL) and poly(dl-lactide-co-glycolide) (PLGA), by combining electrospinning, stress-induced rolling membrane, and microfluidic techniques is reported. This structure can sustain the geometry of the artificial blood vessel over long periods of in vitro/in vivo culture due to the counteraction and mechanical balance of the PCL/PLGA layers.

    11. Ultrahigh-Conductivity Polymer Hydrogels with Arbitrary Structures

      Bowen Yao, Haiyan Wang, Qinqin Zhou, Mingmao Wu, Miao Zhang, Chun Li and Gaoquan Shi

      Version of Record online: 17 MAY 2017 | DOI: 10.1002/adma.201700974

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      A poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) hydrogel treated by concentrated sulfuric acid shows an extraordinarily high conductivity of 880 S m−1. It can be fabricated into arbitrary structures for practical applications. A current-collector-free all-solid fiber supercapacitor based on dried fibers of this hydrogel exhibits a performance superior to those of previously reported counterparts.

    12. Imaging Nanoscale Morphology of Semiconducting Polymer Films with Photoemission Electron Microscopy

      Andreas Neff, Falk Niefind, Bernd Abel, Stefan C. B. Mannsfeld and Katrin R. Siefermann

      Version of Record online: 17 MAY 2017 | DOI: 10.1002/adma.201701012

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      Photoemission electron microscopy in combination with polarized laser light is presented as a tool permitting fast imaging of polymer-chain orientation and local degree of order in semicrystalline samples of semiconducting polymers. The high spatial resolution of the microscope provides insights into the nanoscale morphology, which is relevant for the material's performance in electronic devices.

    13. Oxidized Quasi-Carbon Nitride Quantum Dots Inhibit Ice Growth

      Guoying Bai, Zhiping Song, Hongya Geng, Dong Gao, Kai Liu, Shuwang Wu, Wei Rao, Liangqia Guo and Jianjun Wang

      Version of Record online: 17 MAY 2017 | DOI: 10.1002/adma.201606843

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      Oxidized quasi-carbon nitride quantum dots (OQCNs), which possess the ability to shape ice crystals and inhibit ice growth/recrystallization, are synthesized by a simple and up-scalable approach. In the cryopreservation of sheep red blood cells, OQCNs significantly improve the cell recovery to more than twice that obtained by using a commercial cryoprotectant (hydroxyethyl starch) without the addition of any organic solvents.

    14. Brain-Inspired Photonic Neuromorphic Devices using Photodynamic Amorphous Oxide Semiconductors and their Persistent Photoconductivity

      Minkyung Lee, Woobin Lee, Seungbeom Choi, Jeong-Wan Jo, Jaekyun Kim, Sung Kyu Park and Yong-Hoon Kim

      Version of Record online: 17 MAY 2017 | DOI: 10.1002/adma.201700951

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      A brain-inspired photonic neuromorphic device is demonstrated using an amorphous indium-gallium-zinc-oxide film. By utilizing the persistent photoconductivity behavior, short-term memory/long-term memory, spike-timing-dependent plasticity, and neural facilitation are emulated, which are the important synaptic functions for learning and memory. This work may open up new possibilities to realize ultrafast and massive parallel synaptic computing systems based on photonic neuromorphic devices.

    15. A Single-Molecular AND Gate Operated with Two Orthogonal Switching Mechanisms

      Na Zhang, Wai-Yip Lo, Anex Jose, Zhengxu Cai, Lianwei Li and Luping Yu

      Version of Record online: 17 MAY 2017 | DOI: 10.1002/adma.201701248

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      A single-molecule AND gate is constructed from two different switching mechanisms, the switch between conjugation to cross-conjugation by light and the shift of conducting orbitals by protonation. The two switches are orthogonal and can be switched reversibly. The switching ratio between the highest and lowest conductance states is 94.

  12. Reviews

    1. Defect Chemistry of Nonprecious-Metal Electrocatalysts for Oxygen Reactions

      Dafeng Yan, Yunxiao Li, Jia Huo, Ru Chen, Liming Dai and Shuangyin Wang

      Version of Record online: 16 MAY 2017 | DOI: 10.1002/adma.201606459

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      Defects in carbon-based metal-free electrocatalysts for the oxygen-reduction reaction (ORR) and various defects in metal oxide/selenide for the oxygen-evolution reaction (OER) are reviewed. The existence of defects has a great effect on the properties of catalysts; for example, the charge distribution and the conductibility. The strategies to generate defects, the defect–activity relationship, and the techniques to identify defects are discussed.

  13. Communications

    1. Tuning Up or Down the Critical Thickness in LaAlO3/SrTiO3 through In Situ Deposition of Metal Overlayers

      Diogo Castro Vaz, Edouard Lesne, Anke Sander, Hiroshi Naganuma, Eric Jacquet, Jacobo Santamaria, Agnès Barthélémy and Manuel Bibes

      Version of Record online: 15 MAY 2017 | DOI: 10.1002/adma.201700486

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      The possibility to tune up or down the critical thickness at which a 2D electron gas appears at the LaAlO3/SrTiO3 interface, by capping the LaAlO3 with different metals is demonstrated. Besides electrostatic effects, X-ray photoemission spectroscopy reveals the importance of the partial oxidation of the metal on the properties of the gas.

    2. A Microfluidic Ion Pump for In Vivo Drug Delivery

      Ilke Uguz, Christopher M. Proctor, Vincenzo F. Curto, Anna-Maria Pappa, Mary J. Donahue, Magali Ferro, Róisín M. Owens, Dion Khodagholy, Sahika Inal and George G. Malliaras

      Version of Record online: 15 MAY 2017 | DOI: 10.1002/adma.201701217

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      A microfluidic ion pump is developed, which is capable of delivering a drug without a solvent. In vitro characterization shows low-voltage operation, high drug-delivery capacity, and high ON/OFF ratio. Cortical delivery in an animal model shows that this device represents a significant step forward toward the development of implantable drug-delivery systems.

    3. Photosensitization Priming of Tumor Microenvironments Improves Delivery of Nanotherapeutics via Neutrophil Infiltration

      Dafeng Chu, Xinyue Dong, Qi Zhao, Jingkai Gu and Zhenjia Wang

      Version of Record online: 15 MAY 2017 | DOI: 10.1002/adma.201701021

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      Active delivery of nanotherapeutics to tumor is mediated by neutrophil infiltration after the tumor is photosensitized to induce acute inflammation. Anti-CD11b antibody-decorated nanoparticles are specifically internalized by activated neutrophils in vivo that mediate the tumor deposition of NPs. Photothermal therapy using this approach dramatically improves the cancer treatment in mice.

    4. Ultrahigh Thermal Conductive yet Superflexible Graphene Films

      Li Peng, Zhen Xu, Zheng Liu, Yan Guo, Peng Li and Chao Gao

      Version of Record online: 12 MAY 2017 | DOI: 10.1002/adma.201700589

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      An atomic crystal-folding principle is proposed for designing highly thermal-conductive yet superflexible graphene film. Debris-free, giant graphene sheets and folded atomic thin crystals afford macroscopic assembled graphene film a high thermal conductivity 1940 W m−1 K−1 and fracture elongation 16%, respectively. This principle opens the door for high-performance yet flexible inorganic/ceramic macroscopic materials and devices.

    5. In Situ Probing of Ion Ordering at an Electrified Ionic Liquid/Au Interface

      Wattaka Sitaputra, Dario Stacchiola, James F. Wishart, Feng Wang and Jerzy T. Sadowski

      Version of Record online: 12 MAY 2017 | DOI: 10.1002/adma.201606357

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      Reconfiguration of electric-double-layer ion ordering at electrified ionic liquid/solid interfaces involves complex restructuring of ions. Motion of oppositely charged ions during rearrangement is observed in real time using photoemission electron microscopy. This first step toward novel operando studies of ionic-liquid electrolyte dynamics opens up experimental possibilities for correlating functional properties with local ionic measurements at electrolyte/electrode interfaces.

    6. Superlubricity between MoS2 Monolayers

      He Li, Jinhuan Wang, Song Gao, Qing Chen, Lianmao Peng, Kaihui Liu and Xianlong Wei

      Version of Record online: 12 MAY 2017 | DOI: 10.1002/adma.201701474

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      A method for friction tests between atomic layers of 2D materials is developed based on in situ scanning electron microscope technique. Friction tests on the sliding between MoS2 monolayers give an ultralow friction coefficient of ≈10−4, providing the first direct experimental evidence for the superlubricity between atomic layers of hexagonal MoS2.

    7. Ambient Protection of Few-Layer Black Phosphorus via Sequestration of Reactive Oxygen Species

      Sumeet Walia, Sivacarendran Balendhran, Taimur Ahmed, Mandeep Singh, Christopher El-Badawi, Mathew D. Brennan, Pabudi Weerathunge, Md. Nurul Karim, Fahmida Rahman, Andrea Rassell, Jonathan Duckworth, Rajesh Ramanathan, Gavin E. Collis, Charlene J. Lobo, Milos Toth, Jimmy Christopher Kotsakidis, Bent Weber, Michael Fuhrer, Jose M. Dominguez-Vera, Michelle J. S. Spencer, Igor Aharonovich, Sharath Sriram, Madhu Bhaskaran and Vipul Bansal

      Version of Record online: 12 MAY 2017 | DOI: 10.1002/adma.201700152

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      Few-layer black phosphorous (BP) has recently emerged as a promising elemental analog to graphene. This study reports a chemical sequestration approach that allows BP to remain stable without requiring its isolation from the ambient environment. The strategy allows BP to remain stable for over 13 weeks, while retaining its key electronic characteristics.

    8. Self-Assembled Au/CdSe Nanocrystal Clusters for Plasmon-Mediated Photocatalytic Hydrogen Evolution

      Run Shi, Yinhu Cao, Yanjun Bao, Yufei Zhao, Geoffrey I. N. Waterhouse, Zheyu Fang, Li-Zhu Wu, Chen-Ho Tung, Yadong Yin and Tierui Zhang

      Version of Record online: 12 MAY 2017 | DOI: 10.1002/adma.201700803

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      Highly efficient plasmon-mediated photocatalysts based on Au/CdSe nanocrystal clusters (NCs) are successfully fabricated through an emulsion-based self-assembly approach. The Au/CdSe NCs synergistically harness the excellent visible-light-absorption properties of CdSe quantum dots and Au nanoparticles, affording a remarkable H2 evolution rate of inline image in aqueous solution under visible-light illumination and excellent operational stability.

    9. Laser-Induced Graphene in Controlled Atmospheres: From Superhydrophilic to Superhydrophobic Surfaces

      Yilun Li, Duy Xuan Luong, Jibo Zhang, Yash R. Tarkunde, Carter Kittrell, Franklin Sargunaraj, Yongsung Ji, Christopher J. Arnusch and James M. Tour

      Version of Record online: 12 MAY 2017 | DOI: 10.1002/adma.201700496

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      The modification of graphene-based materials has been an important topic, and this study aims to expand the properties of laser-induced graphene (LIG). With a controlled atmosphere chamber, both superhydrophobic and superhydrophilic LIG surfaces can be obtained. Characterizations show that the different wetting properties result from surface morphology and chemical composition. Applications are demonstrated in oil/water separation, anti-icing, as well as microsupercapacitors.

    10. Semiconducting Nanowire-Based Optoelectronic Fibers

      Wei Yan, Yunpeng Qu, Tapajyoti Das Gupta, Arouna Darga, Dang Tùng Nguyên, Alexis Gérald Page, Mariana Rossi, Michele Ceriotti and Fabien Sorin

      Version of Record online: 12 MAY 2017 | DOI: 10.1002/adma.201700681

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      High-quality monocrystalline semiconducting nanowire-based optoelectronic devices, for the first time, are integrated into the tip of a polymer optical fiber and along the fiber length. The fiber-integrated devices, fabricated via a combination of simple and scalable approaches, exhibit unprecedented optoelectronic properties. The opportunities of this approach in advanced fibers and textiles are highlighted via an all-fiber-integrated fluorescence imaging system.

    11. You have full text access to this OnlineOpen article
      Optical, Thermal, and Mechanical Characterization of Ga2Se3-Added GLS Glass

      Andrea Ravagli, Christopher Craig, Ghada A. Alzaidy, Paul Bastock and Daniel W. Hewak

      Version of Record online: 11 MAY 2017 | DOI: 10.1002/adma.201606329

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      Theresults of the addition of Se to gallium lanthanum sulfide(GLS) glass through the substitution of Ga2S3 by Ga2Se3 are described. An innovative open melting apparatus is used. The addition of selenium to GLS glass generally results in a lower glass transition temperature and an extended transmission window up to 15 µm with minor effect on the visible transmission.

    12. Vertically Aligned Niobium Nanowire Arrays for Fast-Charging Micro-Supercapacitors

      Seyed M. Mirvakili and Ian W. Hunter

      Version of Record online: 11 MAY 2017 | DOI: 10.1002/adma.201700671

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      Fast-charging micro-supercapacitors are made from vertically aligned niobium nanowire arrays. Thanks to the high electrical conductivity of the nanowires, the micro-supercapacitor exhibits a very small characteristic relaxation time constant of 8.4 ms. With 1 m sulfuric acid, cycling rates of up to 300 V s−1 are achieved while with 1-ethyl-3-methylimidazolium tetrafluoroborate an operating voltage of up to 4 V is obtained.

    13. You have full text access to this OnlineOpen article
      Optochemically Responsive 2D Nanosheets of a 3D Metal–Organic Framework Material

      Abhijeet K. Chaudhari, Ha Jin Kim, Intaek Han and Jin-Chong Tan

      Version of Record online: 10 MAY 2017 | DOI: 10.1002/adma.201701463

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      A rapid supramolecular method to synthesize the “OX-1” (Oxford University-1) nanosheet metal–organic framework (MOF), functionalized adopting the guest@MOF strategy, is reported. Nanoscale confinement of light-emitting guest molecules in the OX-1 pores yields remarkable optical, electronic, and chemical properties. Harnessing reversible host–guest interactions, photochemical sensing of volatile organic compounds and small molecules important for many practical applications is demonstrated.

  14. Reviews

    1. Recent Progress in the Design of Advanced Cathode Materials and Battery Models for High-Performance Lithium-X (X = O2, S, Se, Te, I2, Br2) Batteries

      Jiantie Xu, Jianmin Ma, Qinghua Fan, Shaojun Guo and Shixue Dou

      Version of Record online: 10 MAY 2017 | DOI: 10.1002/adma.201606454

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      Emerging Li-X (X = O2, S, Se, Te, I2, Br2) batteries with promising cathode materials open up new opportunities for the development of high-performance lithium-ion battery alternatives. Here, an overview of recent important progress in the design of advanced cathode materials and battery models for developing high-performance Li-X batteries is presented.

  15. Communications

    1. Large Modulation of Charge Carrier Mobility in Doped Nanoporous Organic Transistors

      Fengjiao Zhang, Xiaojuan Dai, Weikun Zhu, Hyunjoong Chung and Ying Diao

      Version of Record online: 10 MAY 2017 | DOI: 10.1002/adma.201700411

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      Doping of organic electronics without disrupting molecular packing is a critical challenge preventing effective modulation of charge transport properties. This paper reports on enhanced charge-transfer doping in crystalline small molecule and polymer transistors by introducing nanopores in organic semiconductors via meniscus-guided coating. Nanopores lead to dramatic increase in charge carrier mobility by promoting charge transfer reaction across the pore wall.

    2. Solvent-Free Self-Assembly to the Synthesis of Nitrogen-Doped Ordered Mesoporous Polymers for Highly Selective Capture and Conversion of CO2

      Fujian Liu, Kuan Huang, Qin Wu and Sheng Dai

      Version of Record online: 10 MAY 2017 | DOI: 10.1002/adma.201700445

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      A novel and green strategy in which no solvents are used, for the fast synthesis of nitrogen-doped ordered mesoporous polymers (N-OMPs) is developed. The N-OMPs display competitive CO2 capacities and extraordinary CO2/N2 selectivities, as well as excellent activity for catalytic conversion of CO2. The methodology can also be extended to the synthesis of N-OMP/SiO2 nanocomposites, mesoporous SiO2, TiO2, and TiPO.

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