Angewandte Chemie International Edition

Cover image for Vol. 55 Issue 7

Chefredakteur: Peter Gölitz, Stellvertreter: Neville Compton, Haymo Ross

Online ISSN: 1521-3773

Associated Title(s): Angewandte Chemie, Chemistry - A European Journal, Chemistry – An Asian Journal, ChemistryOpen, ChemPlusChem, Zeitschrift für Chemie

Upcoming VIPs

The following papers are very important in the opinion of two referees.

You are invited to comment on published VIPs. Please use the link given at the end of each such abstract. Scientific comments may be forwarded to the authors by the editorial office and may be posted on this page. Kindly let us know if your comments are for the editorial office only, the author, or the public as well.

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Structure and Composition of the 200 K-Superconducting Phase of H2S at Ultrahigh Pressure: The Perovskite (SH)(H3S+)

Elijah E. Gordon, Ke Xu, Prof. Dr. Hongjun Xiang, Prof. Dr. Annette Bussmann-Holder, Dr. Reinhard K. Kremer, Prof. Dr. Arndt Simon, Prof. Dr. Jürgen Köhler and Prof. Dr. Myung-Hwan Whangbo

Structure and Composition of the 200 K-Superconducting Phase of H2S at Ultrahigh Pressure: The Perovskite (SH−)(H3S+)

Under ultrahigh pressure (>110 GPa), H2S is converted into a metallic phase that becomes superconducting with a record Tc of approximately 200 K. It is proposed that in this phase a dissociation of 2 H2S into H3S+ and SH is present, leading to the perovskite structure (SH)(H3S+). This phase consists of corner-sharing SH6 octahedra with SH ions at the center of each S8 cube.

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Charge-Induced Unzipping of Isolated Proteins to a Defined Secondary Structure

Ana Isabel González Flórez, Eike Mucha, Dr. Doo-Sik Ahn, Sandy Gewinner, Dr. Wieland Schöllkopf, Prof. Dr. Kevin Pagel and Dr. Gert von Helden

Charge-Induced Unzipping of Isolated Proteins to a Defined Secondary Structure

Ultracold gas-phase IR spectroscopy reveals that highly charged protein ions adopt highly ordered, regular secondary structures that are characterized by intramolecular C5 hydrogen bonds. This transition in secondary structure is supported by a simple electrostatic model and is most likely universal for isolated proteins.

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Superparamagnetic Reduced Graphene Oxide with Large Magnetoresistance: A Surface Modulation Strategy

Jing Peng, Yuqiao Guo, Haifeng Lv, Xinyu Dou, Qi Chen, Jiyin Zhao, Prof. Changzheng Wu, Xiaojiao Zhu, Yue Lin, Prof. Wei Lu, Prof. Xiaojun Wu and Prof. Yi Xie

Superparamagnetic Reduced Graphene Oxide with Large Magnetoresistance: A Surface Modulation Strategy

Beneath the surface: Modification of graphene oxide with thiol groups results in ferromagnetic reduced graphene oxide; subsequent mild oxidation and partial thiol group removal produces superparamagnetic reduced graphene oxide. The magnetic domains are reduced to a critical size and the number of unpaired spins decreased to result in a superparamagnetic structure. This material shows large negative low-field magnetoresistance at ambient temperature.

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Layered Black Phosphorus: Strongly Anisotropic Magnetic, Electronic, and Electron-Transfer Properties

Prof. Dr. Zdeněk Sofer, Prof. Dr. David Sedmidubský, Dr. Štěpán Huber, Jan Luxa, Daniel Bouša, Dr. Chris Boothroyd and Prof. Dr. Martin Pumera

Layered Black Phosphorus: Strongly Anisotropic Magnetic, Electronic, and Electron-Transfer Properties

A shift in direction: The electrical, magnetic, and electrochemical properties of black phosphorus display an anomalous anisotropy. These unusual observations were interpreted by means of calculations, which manifested the metallic character of the edge plane and the semiconductivity of the basal plane, indicating that black phosphorus belongs to a group of materials known as topological insulators.

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Enzyme Selectivity Fine-Tuned through Dynamic Control of a Loop

Dr. Beat Vögeli, Dr. Stefan Bibow and Dr. Celestine N. Chi

Enzyme Selectivity Fine-Tuned through Dynamic Control of a Loop

In the loop: Modification of flexible loops induces structural equilibrium redistribution of an enzyme active site. A ligand-selective change of binding affinity to the active site of cyclophilin is achieved by tuning of the dynamics of a highly flexible loop. This system may serve as a model system for studying the effects of various time scales of loop motion on protein function tuned by mutations.

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A Triatomic Silicon(0) Cluster Stabilized by a Cyclic Alkyl(amino) Carbene

Dr. Kartik Chandra Mondal, Dr. Sudipta Roy, Priv.-Doz. Dr. Birger Dittrich, Dr. Diego M. Andrada, Prof. Dr. Gernot Frenking and Prof. Dr. Herbert W. Roesky

A Triatomic Silicon(0) Cluster Stabilized by a Cyclic Alkyl(amino) Carbene

Three-sided: Reaction of potassium graphite with a cyclic alkyl(amino) carbene tetrachlorosilane adduct results in the formation of a stable and isolable carbene-stabilized triatomic silicon(0) cluster (see figure). The triangular compound was characterized by single crystal X-ray structural crystallography, and its bonding and electron density distributions were studied by quantum chemical calculations.

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Elemental-Sulfur-Mediated Facile Synthesis of a Covalent Triazine Framework for High-Performance Lithium–Sulfur Batteries

Dr. Siddulu Naidu Talapaneni, Tae Hoon Hwang, Sang Hyun Je, Dr. Onur Buyukcakir, Prof. Jang Wook Choi and Prof. Ali Coskun

Elemental-Sulfur-Mediated Facile Synthesis of a Covalent Triazine Framework for High-Performance Lithium–Sulfur Batteries

Elemental stabilization: A covalent triazine framework (CTF) with chemically embedded polymeric sulfur (S-CTF) was synthesized under catalyst- and solvent-free reaction conditions from 1,4-dicyanobenzene and elemental sulfur. This material was used as a robust cathode for high-performance lithium–sulfur batteries with very good cycling stabilities.

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Cooperative Reductive Elimination: The Missing Piece in the Oxidative-Coupling Mechanistic Puzzle

Ignacio Funes-Ardoiz and Prof. Feliu Maseras

Cooperative Reductive Elimination: The Missing Piece in the Oxidative-Coupling Mechanistic Puzzle

Joint effort: The reaction between benzoic acid and methylphenylacetylene to form an isocoumarin is catalyzed by Cp*Rh(OAc)2 in the presence of Cu(OAc)2(H2O) as the oxidant. Its mechanism was elucidated by DFT calculations with the B97D functional, which showed that the overall transformation proceeds by cooperative reductive elimination with a transition state containing both rhodium and copper centers.

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Total Synthesis of Ileabethoxazole, Pseudopteroxazole, and seco-Pseudopteroxazole

Dr. Ming Yang, Xiaowen Yang, Prof. Dr. Hongbin Sun and Prof. Dr. Ang Li

Total Synthesis of Ileabethoxazole, Pseudopteroxazole, and seco-Pseudopteroxazole

The antituberculosis diterpenoids ileabethoxazole, pseudopteroxazole, and seco-pseudopteroxazole were prepared by total synthesis. An important triene intermediate was obtained by an alkyne carbopalladation/Stille reaction cascade and then subjected to a one-pot 6π electrocyclization/aromatization process to assemble the multisubstituted aromatic core.

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Noninvasive Staging of Kidney Dysfunction Enabled by Renal-Clearable Luminescent Gold Nanoparticles

Dr. Mengxiao Yu, Dr. Jiancheng Zhou, Bujie Du, Xuhui Ning, Craig Authement, Leah Gandee, Prof. Dr. Payal Kapur, Prof. Dr. Jer-Tsong Hsieh and Prof. Dr. Jie Zheng

Noninvasive Staging of Kidney Dysfunction Enabled by Renal-Clearable Luminescent Gold Nanoparticles

A noninvasive, inexpensive method for the noninvasive staging of kidney dysfunction is based on the use of renal-clearable near-infrared-emitting gold nanoparticles as imaging agents for in vivo fluorescence imaging. The various stages of kidney dysfunction could thus be readily differentiated in a unilateral-ureteral-obstruction mouse model.

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Light-Harvesting Systems Based on Organic Nanocrystals To Mimic Chlorosomes

Dr. Peng-Zhong Chen, Prof. Dr. Yu-Xiang Weng, Dr. Li-Ya Niu, Dr. Yu-Zhe Chen, Prof. Dr. Li-Zhu Wu, Prof. Dr. Chen-Ho Tung and Prof. Dr. Qing-Zheng Yang

Light-Harvesting Systems Based on Organic Nanocrystals To Mimic Chlorosomes

Daylight saving: Uniform nanocrystals of organic difluoroboron chromophores with controlled donor/acceptor ratios were prepared by simple coassembly of the donors and acceptors in water. The light-harvesting system funneled the excitation energy with an energy transfer efficiency of 95 % at a donor/acceptor ratio as high as 1000:1. The acceptor was found to have a significant fluorescence at donor/acceptor ratios of up to 200 000:1.

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Catalytically Active Rh Sub-Nano Clusters on TiO2 for CO Oxidation at Cryogenic Temperatures

Hongling Guan, Dr. Jian Lin, Dr. Botao Qiao, Dr. Xiaofeng Yang, Dr. Lin Li, Dr. Shu Miao, Prof. Jingyue Liu, Prof. Aiqin Wang, Prof. Xiaodong Wang and Prof. Tao Zhang

Catalytically Active Rh Sub-Nano Clusters on TiO2 for CO Oxidation at Cryogenic Temperatures

Supported catalysts: A catalyst with unique configuration of Rh sub-nano clusters supported on a TiO2 surface was prepared. This catalyst exhibited an unprecedentedly high activity for CO oxidation at cryogenic temperatures.

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Filtration Shell Mediated Power Density Independent Orthogonal Excitations–Emissions Upconversion Luminescence

Dr. Xiaomin Li, Zhenzhen Guo, Tiancong Zhao, Yang Lu, Lei Zhou, Prof. Dongyuan Zhao and Prof. Fan Zhang

Filtration Shell Mediated Power Density Independent Orthogonal Excitations–Emissions Upconversion Luminescence

A different light: Lanthanide-doped nanoparticles (NPs) with a filtration shell that separates two different luminescence processes and prevents them from interfering with each other are prepared. The filtration effects allow the core-multishell upconversion NPs to show power density independent orthogonal excitations-emissions luminescence and be used in anti-counterfeiting and imaging-guided combined therapy.

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Target-induced and Equipment-free DNA Amplification with a Simple Paper Device

Dr. Meng Liu, Christy Y. Hui, Dr. Qiang Zhang, Jimmy Gu, Dr. Balamurali Kannan, Dr. Sana Jahanshahi-Anbuhi, Prof. Dr. Carlos D. M. Filipe, Prof. Dr. John D. Brennan and Prof. Dr. Yingfu Li

Target-induced and Equipment-free DNA Amplification with a Simple Paper Device

DNA amplification is better on paper: A highly functional, “all-in-one” DNA amplification-based paper device allows for visual detection of DNA and microRNA with minimal human intervention, making this method particularly suitable for bioassays used in resource-poor settings.

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First Principles Calculations for Hydrogenation of Acrolein on Pd and Pt: Chemoselectivity Depends on Steric Effects on the Surface

Sakari Tuokko, Prof. Dr. Petri M. Pihko and Dr. Karoliina Honkala

First Principles Calculations for Hydrogenation of Acrolein on Pd and Pt: Chemoselectivity Depends on Steric Effects on the Surface

Run for cover: Acrolein is reduced chemoselectively on Pt(111) and Pd(111) surfaces at the C[DOUBLE BOND]C bond and not at the C[DOUBLE BOND]O bond because reaction steps involving C[DOUBLE BOND]O reduction become energetically unfavorable with increasing steric repulsion.

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Oxyhydroxide Nanosheets with Highly Efficient Electron–Hole Pair Separation for Hydrogen Evolution

Junheng Huang, Qichao Shang, Dr. Yuanyuan Huang, Fumin Tang, Prof. Qun Zhang, Dr. Qinghua Liu, Shan Jiang, Fengchun Hu, Wei Liu, Prof. Yi Luo, Dr. Tao Yao, Dr. Yong Jiang, Dr. Zhiyun Pan, Dr. Zhihu Sun and Prof. Shiqiang Wei

Oxyhydroxide Nanosheets with Highly Efficient Electron–Hole Pair Separation for Hydrogen Evolution

The thickness of a layered β-CoOOH semiconductor was reduced to obtain an atomically thin two-dimensional nanostructure. Electron–hole recombination is almost suppressed in the 1.3 nm thick β-CoOOH nanosheet, which leads to excellent electron–hole separation efficiencies and superior hydrogen production rates (LD⊥: carrier diffusion length along the c axis).

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Synthesis of Iron Nanometallic Glasses and Their Application in Cancer Therapy by a Localized Fenton Reaction

Dr. Chen Zhang, Prof. Wenbo Bu, Dr. Dalong Ni, Dr. Shenjian Zhang, Dr. Qing Li, Prof. Zhenwei Yao, Prof. Jiawen Zhang, Dr. Heliang Yao, Prof. Zheng Wang and Prof. Jianlin Shi

Synthesis of Iron Nanometallic Glasses and Their Application in Cancer Therapy by a Localized Fenton Reaction

Amorphous iron nanoparticles (AFeNPs) can be used for cancer theranostics. Ionization of the AFeNPs in the mildly acidic tumor microenvironment promotes the release of ferrous ions in the tumor; these induce H2O2 disproportionation, which in turn leads to efficient .OH generation and significant tumor growth inhibition.

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Electrocatalytic Generation of Amidyl Radicals for Olefin Hydroamidation: Use of Solvent Effects to Enable Anilide Oxidation

Lin Zhu, Peng Xiong, Zhong-Yi Mao, Yong-Heng Wang, Prof. Dr. Xiaomei Yan, Prof. Dr. Xin Lu and Prof. Dr. Hai-Chao Xu

Electrocatalytic Generation of Amidyl Radicals for Olefin Hydroamidation: Use of Solvent Effects to Enable Anilide Oxidation

Easy access to­ N-arylamidyl radicals: The first electrocatalytic method for the generation of amidyl radicals from anilides has been developed using ferrocene (Cp2Fe) as a highly reactive, yet chemoselective redox catalyst. Based on this radical-generating method, a highly chemo- and diastereoselective olefin hydroamidation reaction has been developed.

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