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Cover image for Vol. 9 Issue 8

Special Issue: Low-Dimensional Carbon Materials

April 22, 2013

Volume 9, Issue 8

Pages 1121–1410

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      Special Issue: Low-Dimensional Carbon Materials (Small 8/2013) (page 1121)

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201370043

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      This issue's cover highlights the main low-dimensional carbon materials (for example graphene and carbon nanotubes), a longstanding favorite of the Center for Nanochemistry (CNC) at Peking University. In the past 20 years, the CNC team has produced numerous exciting achievements in the synthesis, characterization, properties, and applications of low-dimensional carbon materials. This special issue was organized as the commemorative gift to the CNC's 20th birthday.

  2. Inside Front Cover

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    1. Field-Effect Transistors: Unique Role of Self-Assembled Monolayers in Carbon Nanomaterial-Based Field-Effect Transistors (Small 8/2013) (page 1122)

      Hongliang Chen and Xuefeng Guo

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201370044

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      Integrated electrical circuits are described by H. Chen and X. Guo through the combination of bottom-up self-assembly and top-down device fabrication. In each device on page 1144, self-assembled monolayers are used as active layers and carbon nanomaterials (such as single-walled carbon nanotubes or graphene) act as nanoelectrodes, forming stimuli-responsive high-performance organic field-effect transistors. In conjunction with their miniaturized dimensions, the ability to integrate these hybrid devices into current CMOS technology has the potential to create multifunctional integrated circuits as a significant step towards practical molecular devices.

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    1. Low-Dimensional Carbon Materials (Small 8/2013) (page 1412)

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201370045

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  4. Masthead

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    1. Masthead: (Small 8/2013)

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201370046

  5. Contents

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    1. Contents: (Small 8/2013) (pages 1123–1130)

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201370047

  6. Editorial

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  7. Concepts

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    1. Photo-induced Free Radical Modification of Graphene (pages 1134–1143)

      Liming Zhang, Lin Zhou, Mingmei Yang, Zhirong Liu, Qin Xie, Hailin Peng and Zhongfan Liu

      Article first published online: 20 MAR 2013 | DOI: 10.1002/smll.201203152

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      Free radicals (X·) are photogenerated under illumination from neutral Xn molecules. These radicals react with the exposed graphene surface, leading to the light-guided covalent modification of graphene.

  8. Reviews

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    1. Unique Role of Self-Assembled Monolayers in Carbon Nanomaterial-Based Field-Effect Transistors (pages 1144–1159)

      Hongliang Chen and Xuefeng Guo

      Article first published online: 4 MAR 2013 | DOI: 10.1002/smll.201202973

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      The unique role of self-assembled monolayers (SAMs) as either active or auxiliary layers in carbon nanomaterial-based field-effect transistors is highlighted for tuning the substrate effect, controlling the carrier type and density in the conducting channel, and even installing new functionalities. The combination of molecular self-assembly and molecular engineering with materials fabrication could incorporate diverse molecular functionalities into electrical nanocircuits, thus speeding the development of nanometer/molecular electronics in the future.

    2. Graphene-Based Electrochemical Sensors (pages 1160–1172)

      Shixin Wu, Qiyuan He, Chaoliang Tan, Yadong Wang and Hua Zhang

      Article first published online: 13 MAR 2013 | DOI: 10.1002/smll.201202896

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      Recently, different graphene-based materials, prepared by chemical reduction of graphene oxide (GO), solvothermal reduction of GO, electrochemical reduction of GO, etc., have been widely used for electrochemical sensing applications. In this review, the sensing performances of different graphene-based materials for detection of various biomolecules and chemicals have been summarized and compared.

    3. Graphene: A Two-Dimensional Platform for Lithium Storage (pages 1173–1187)

      Sheng Han, Dongqing Wu, Shuang Li, Fan Zhang and Xinliang Feng

      Article first published online: 13 MAR 2013 | DOI: 10.1002/smll.201203155

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      This review presents the componential and structural design for graphene-based hybrids in lithium ion batteries (LIBs) with enhanced electrochemical performance. The typical fabrication methods and structure–property relationships of these hybrids are discussed.

    4. A Review of Carbon Nanotube- and Graphene-Based Flexible Thin-Film Transistors (pages 1188–1205)

      Dong-Ming Sun, Chang Liu, Wen-Cai Ren and Hui-Ming Cheng

      Article first published online: 21 MAR 2013 | DOI: 10.1002/smll.201203154

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      The progress of carbon nanotube- and graphene-based flexible thin-film transistors from material preparation, device fabrication techniques to transistor performance control is reviewed. State-of-the-art fabrication techniques of thin-film transistors are divided into three categories and possible scale-up approaches to achieve realistic production of flexible nanocarbon-based transistors are discussed. The recent progress in flexible all-carbon nanomaterial transistor research is highlighted.

    5. Graphene: A Platform for Surface-Enhanced Raman Spectroscopy (pages 1206–1224)

      Weigao Xu, Nannan Mao and Jin Zhang

      Article first published online: 26 MAR 2013 | DOI: 10.1002/smll.201203097

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      Graphene is a unique platform for surface-enhanced Raman spectroscopy (SERS). The multi-role of graphene played in SERS is overviewed, including as a Raman probe, as a substrate, as an additive, and as a building block of a flat surface for SERS. Apart from versatile improvements on SERS performance towards applications, graphene-involved SERS studies are also expected to shed light on the fundamental mechanism of the SERS effect.

    6. Carbon Nanotube Photoelectronic and Photovoltaic Devices and their Applications in Infrared Detection (pages 1225–1236)

      Leijing Yang, Sheng Wang, Qingsheng Zeng, Zhiyong Zhang and Lian-Mao Peng

      Article first published online: 26 MAR 2013 | DOI: 10.1002/smll.201203151

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      Carbon nanotube (CNT)-based photovoltaic cells and photodetectors are reviewed with a focus on the particular type of CNT diodes fabricated via a doping-free process. The photovoltage multiplication effect of CNT and its potential application for constructing high-performance CNT-based infrared detectors are also reviewed.

    7. The Road for Nanomaterials Industry: A Review of Carbon Nanotube Production, Post-Treatment, and Bulk Applications for Composites and Energy Storage (pages 1237–1265)

      Qiang Zhang, Jia-Qi Huang, Wei-Zhong Qian, Ying-Ying Zhang and Fei Wei

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201203252

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      The mass production engineering principles and advances in carbon nanotube (CNT) purification, dispersion, as well as bulk applications for nanocomposite and energy storage are reviewed. The environmental, health, and safety considerations of CNTs, and the recent progress on CNT commercialization are also included. The gap between the basic scientific research and industrial development should be bridged by multidisciplinary research for the rapid growth of CNT nano-industry.

    8. Graphene in Light: Design, Synthesis and Applications of Photo-active Graphene and Graphene-Like Materials (pages 1266–1283)

      Hang-Xing Wang, Qiang Wang, Kai-Ge Zhou and Hao-Li Zhang

      Article first published online: 2 APR 2013 | DOI: 10.1002/smll.201203040

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      Combining the unique electrical and mechanic properties of graphene with the excellent optical properties of various photo-active moieties, functionalized graphene has true potential for photodetectors, optoelectronics, photovoltaics, and photocatalysis.

    9. Spectroscopic Characterization of the Chiral Structure of Individual Single-Walled Carbon Nanotubes and the Edge Structure of Isolated Graphene Nanoribbons (pages 1284–1304)

      Daqi Zhang, Juan Yang and Yan Li

      Article first published online: 26 MAR 2013 | DOI: 10.1002/smll.201202986

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      The chiral structure of single-walled carbon nanotubes and the edge structure of graphene nanoribbons are key issues in determining their electronic structures and properties. The fundamental principles and the applications of various spectroscopic methods, including resonance Raman, photoluminescence, and Rayleigh scattering spectroscopies, in the structural determination of these sp2 carbon-based materials are reviewed. The challenges in this area are also discussed.

  9. Frontispiece

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    1. Nanotube Arrays: Sorting out Semiconducting Single-Walled Carbon Nanotube Arrays by Washing off Metallic Tubes Using SDS Aqueous Solution (Small 8/2013) (page 1305)

      Yue Hu, Yabin Chen, Pan Li and Jin Zhang

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201370048

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      S-SWNT (red tubes) arrays are sorted on a quartz surface by J. Zhang and co-workers, who explain on page 1306 how to wash off the m-SWNTs (green tubes) using SDS (yellow particles) aqueous solution. The SDS molecules selectively adsorb onto m-SWNTs. The SDS coating layer then minimizes the interactions between m-SWNTs and the quartz substrate, thus allowing the m-SWNTs to be easily washed off by the assistance of ultrasonication while the s-SWNT arrays remain securely on the substrate.

  10. Communications

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    1. Sorting out Semiconducting Single-Walled Carbon Nanotube Arrays by Washing off Metallic Tubes Using SDS Aqueous Solution (pages 1306–1311)

      Yue Hu, Yabin Chen, Pan Li and Jin Zhang

      Article first published online: 18 MAR 2013 | DOI: 10.1002/smll.201202940

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      Semiconducting single-walled carbon nanotube (s-SWNT) arrays are produced via a procedure analogous to a surfactant-assisted decontamination process. Aligned individual SWNT arrays grow on a quartz surface as a mixture of metallic SWNTs (m-SWNTs) and s-SWNTs. They are immersed in a sodium dodecyl sulfate (SDS) solution, and the SDS molecules selectively adsorb onto m-SWNTs. This SDS coating minimizes the interaction between m-SWNTs and the substrate, thus the m-SWNTs are easily washed off during ultrasonication while the s-SWNT arrays remain on the substrate. The percentage of s-SWNTs in the arrays can be higher than 90%.

    2. Solvatochromic Effect on the Photoluminescence of MoS2 Monolayers (pages 1312–1315)

      Nannan Mao, Yanfeng Chen, Dameng Liu, Jin Zhang and Liming Xie

      Article first published online: 26 FEB 2013 | DOI: 10.1002/smll.201202982

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      The effect of surrounding solvents on the photoluminescence (PL) of MoS2 monolayers on Si/SiO2 substrates is studied. A redshift (up to −60 meV) is observed for MoS2 monolayers with nonhalogenated solvent surroundings. A blueshift (up to 60 meV) and intensity increase (2–50 times) are observed for monolayers with halogenated solvent surroundings.

    3. Synthesis of Boron-Doped Graphene Monolayers Using the Sole Solid Feedstock by Chemical Vapor Deposition (pages 1316–1320)

      Huan Wang, Yu Zhou, Di Wu, Lei Liao, Shuli Zhao, Hailin Peng and Zhongfan Liu

      Article first published online: 6 MAR 2013 | DOI: 10.1002/smll.201203021

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      Substitutionally boron-doped monolayer graphene film is grown on a large scale by using a sole phenylboronic acid as the source in a low-pressure chemical vapor deposition system. The B-doped graphene film is a homogeneous monolayer with high crystalline quality, which exhibits a stable p-type doping behavior with a considerably high room-temperature carrier mobility of about 800 cm2 V−1 s−1.

    4. Nickel Sulfide/Nitrogen-Doped Graphene Composites: Phase-Controlled Synthesis and High Performance Anode Materials for Lithium Ion Batteries (pages 1321–1328)

      Nasir Mahmood, Chenzhen Zhang and Yanglong Hou

      Article first published online: 12 MAR 2013 | DOI: 10.1002/smll.201203032

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      Phase-controlled nickel sulfide (Ni3S4 and NiS1.03) nanoparticle (NP)/nitrogen-doped graphene (NG) composites are prepared through a facile one-pot hydrothermal process. The composites show ultrahigh capacity retentions of 98.87% and 95.94% for Ni3S4/NG and NiS1.03/NG electrodes, respectively, as anode materials for lithium ion batteries.

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    1. Graphene Sheets: Gram-Scale Synthesis of Graphene Sheets by a Catalytic Arc-Discharge Method (Small 8/2013) (page 1329)

      Liping Huang, Bin Wu, Jianyi Chen, Yunzhou Xue, Dechao Geng, Yunlong Guo, Gui Yu and Yunqi Liu

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201370049

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      Gram-scale amounts of high-quality graphene sheets are synthesized on page 1330 through an arc-discharge method. An arc, which is generated between two graphite rods when a high voltage is applied by Y. Liu and co-workers, can cause the graphite layers to separate into graphene sheets via a high-temperature exfoliation, or even broken into small clusters/atoms, which then form graphene sheets by catalytic growth, demonstrating that two mechanisms exist in an arc discharge process simultaneously.

  12. Communications

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    1. Gram-Scale Synthesis of Graphene Sheets by a Catalytic Arc-Discharge Method (pages 1330–1335)

      Liping Huang, Bin Wu, Jianyi Chen, Yunzhou Xue, Dechao Geng, Yunlong Guo, Gui Yu and Yunqi Liu

      Article first published online: 6 MAR 2013 | DOI: 10.1002/smll.201202802

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      Flake graphite is used as carbon source and ZnO or ZnS as catalyst in the synthesis of high-quality graphene sheets. A catalytic growth mechanism for cathode-part graphene synthesis in the arc-discharge apparatus and an exfoliation mechanism for wall-part graphene synthesis are introduced. N-doped cathode-part graphene and undoped wall-part graphene are formed simultaneously.

    2. Photocatalytic Engineering of Single-Walled Carbon Nanotubes: From Metal-to-Semiconductor Conversion to Cutting and Patterning (pages 1336–1341)

      Yufeng Nie, Liming Zhang, Di Wu, Yubin Chen, Guoming Zhang, Qin Xie and Zhongfan Liu

      Article first published online: 12 MAR 2013 | DOI: 10.1002/smll.201203066

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      With a TiO2-based photocatalytic approach, both an arbitrary geometry tailoring of single-walled carbon nanotubes (SWCNTs) on various substrates and the conversion of metallic to semiconducting SWCNTs are demonstrated. Taking advantage of the selectivity on the diameter and metallicity of SWCNTs, 100% depletable SWCNT-based field-effect transistors are achieved, with Ion/Ioff improvements up to five orders of magnitude.

    3. High-Performance Supercapacitor Electrode Materials Prepared from Various Pollens (pages 1342–1347)

      Long Zhang, Fan Zhang, Xi Yang, Kai Leng, Yi Huang and Yongsheng Chen

      Article first published online: 13 MAR 2013 | DOI: 10.1002/smll.201202943

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      Supercapacitors based on activated carbon prepared from various pollens show good specific capacitance (207 F g−1) and large gravimetric and volumetric energy density (∼88 Wh kg−1 and ∼44 Wh L−1, respectively) in ionic liquid electrolytes, which are much better than those of RP20 (commercial activated carbon) or graphene-based supercapacitors.

    4. Photoinduced Methylation of Graphene (pages 1348–1352)

      Lei Liao, Zehao Song, Yu Zhou, Huan Wang, Qin Xie, Hailin Peng and Zhongfan Liu

      Article first published online: 20 MAR 2013 | DOI: 10.1002/smll.201203069

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      Covalent grafting of methyl groups onto the basal plane of graphene is achieved through a photochemical reaction between graphene and di-tert-butyl peroxide. The methylation of graphene is found to be reversible. The edge of single-layer graphene shows the largest methylation reactivity, which provides a route to tailor the edge state of graphene.

    5. Facile Synthesis of Large-Area Ultrathin Hexagonal BN Films via Self-Limiting Growth at the Molten B2O3 Surface (pages 1353–1358)

      Xiaoxia Yang, Zixuan Guan, Min Zeng, Jiake Wei, Wenlong Wang and Xuedong Bai

      Article first published online: 15 MAR 2013 | DOI: 10.1002/smll.201203126

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      A self-limiting growth process based on the interface-controlled reaction of molten boron oxide (B2O3) with ammonia (NH3) is demonstrated for the facile and lost-cost synthesis of ultrathin (20–30 nm) crystalline hexagonal boron nitride (h-BN) films over large areas. The as-grown h-BN films are of high quality, being densely continuous, uniform and smooth, and highly transparent over a broad wavelength range.

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    1. Graphene: Single and Polycrystalline Graphene on Rh(111) Following Different Growth Mechanisms (Small 8/2013) (page 1359)

      Mengxi Liu, Yabo Gao, Yanfeng Zhang, Yu Zhang, Donglin Ma, Qingqing Ji, Teng Gao, Yubin Chen and Zhongfan Liu

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201370050

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      The atomic resolution of scanning tunneling microscope (STM) images is exploited to identify graphene on metal substrates. The growth of graphene on a Rh(111) substrate is examined under different growth conditions, and diverse surface characteristics and growth mechanisms are discovered. On page 1360, the versatile atomic structures and different stacking geometries of graphene on Rh(111) are described by Z. F. Liu and co-workers.

  14. Full Papers

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    1. Single and Polycrystalline Graphene on Rh(111) Following Different Growth Mechanisms (pages 1360–1366)

      Mengxi Liu, Yabo Gao, Yanfeng Zhang, Yu Zhang, Donglin Ma, Qingqing Ji, Teng Gao, Yubin Chen and Zhongfan Liu

      Article first published online: 25 FEB 2013 | DOI: 10.1002/smll.201202962

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      Using ultrahigh vacuum and atmospheric pressure chemical vapor deposition (UHVCVD and APCVD) methods, single crystalline and polycrystalline, monolayer and few-layer graphene is synthesized on a substrate of Rh(111). With scanning tunneling microscope, atomic-scale images of the samples are obtained. This work may provide atomic-scale proofs for some fundamental issues in graphene growth.

    2. Aligned Carbon Nanotubes for High-Efficiency Schottky Solar Cells (pages 1367–1372)

      Jiangtao Di, Zhenzhong Yong, Xinhe Zheng, Baoquan Sun and Qingwen Li

      Article first published online: 6 MAR 2013 | DOI: 10.1002/smll.201202995

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      Carbon nanotube (CNT)–Si Schottky solar cells are fabricated using an aligned CNT film drawn directly from a CNT array. The power conversion efficiency (PCE) is 10.5%, much higher than that of the solar cells fabricated using pristine and random CNT films. The fabrication is scalable, and the solar cells fabricated in one batch show very small PCE fluctuations.

    3. Widely Tunable Carrier Mobility of Boron Nitride-Embedded Graphene (pages 1373–1378)

      Jinying Wang, Ruiqi Zhao, Zhongfan Liu and Zhirong Liu

      Article first published online: 20 MAR 2013 | DOI: 10.1002/smll.201202978

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      The intrinsic carrier mobility of boron nitride-embedded graphene (BNG) is investigated under a phonon scattering mechanism. The mobility increases with carbon content and is tunable from 103 to 105 cm2 V−1 s−1 when the bandgap is between 0.38 and 1.39 eV. Some BNG materials even show ultrahigh mobility comparable to that of graphene. BNG is thus a promising material for electronic devices.

    4. Chirality-Dependent Reactivity of Individual Single-Walled Carbon Nanotubes (pages 1379–1386)

      Bilu Liu, Hua Jiang, Arkady V. Krasheninnikov, Albert G. Nasibulin, Wencai Ren, Chang Liu, Esko I. Kauppinen and Hui-Ming Cheng

      Article first published online: 15 MAR 2013 | DOI: 10.1002/smll.201202761

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      The intrinsic chemical reactivity of individual and suspended single-walled carbon nanotubes is investigated using electron diffraction. The results reveal that the reactivity of nanotubes is not only related to their diameters and electronic properties, but also to their chiral angles. Simple air treatment at medium temperatures may selectively enrich large-diameter and high-chiral-angle semiconducting carbon nanotubes.

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    1. Free Radicals: Free Radical Reactions in Two Dimensions: A Case Study on Photochlorination of Graphene (Small 8/2013) (page 1387)

      Lin Zhou, Lushan Zhou, Mingmei Yang, Di Wu, Lei Liao, Kai Yan, Qin Xie, Zhirong Liu, Hailin Peng and Zhongfan Liu

      Article first published online: 12 APR 2013 | DOI: 10.1002/smll.201370051

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      Graphene is a 2D giant polycyclic aromatic molecule that provides opportunities for studying chemical reactions in two dimensions. H. Peng, Z. Liu, and co-workers have systematically investigated the influence of specific features of 2D molecules, such as their thickness, stacking order, single- and double-side upon graphene's radical reactivity by utilizing a free radical photochlorination as a probe. The result, described on page 1388, can contribute to a deeper understanding of dimensionality effects for the chemistry of 2D graphene.

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    1. Free Radical Reactions in Two Dimensions: A Case Study on Photochlorination of Graphene (pages 1388–1396)

      Lin Zhou, Lushan Zhou, Mingmei Yang, Di Wu, Lei Liao, Kai Yan, Qin Xie, Zhirong Liu, Hailin Peng and Zhongfan Liu

      Article first published online: 19 MAR 2013 | DOI: 10.1002/smll.201202969

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      Graphene provides a perfect platform for studying free radical reaction chemistry in two-dimensions. Free-radical photochlorination of graphene is used as an example to investigate the thickness, stacking order, and single- and double-side dependent reactivity of graphene. Anomalously low reactivity is observed in the photochlorination of AB-stacked bilayer graphene in comparison with that of few-layer graphene.

      Corrected by:

      Corrigendum: Corrigendum: Free Radical Reactions in Two Dimensions: A Case Study on Photochlorination of Graphene

      Vol. 9, Issue 15, 2485, Article first published online: 6 AUG 2013

    2. Edge-to-Edge Assembled Graphene Oxide Aerogels with Outstanding Mechanical Performance and Superhigh Chemical Activity (pages 1397–1404)

      Huan Huang, Pengwan Chen, Xuetong Zhang, Yun Lu and Wanchu Zhan

      Article first published online: 20 MAR 2013 | DOI: 10.1002/smll.201202965

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      Chemically crosslinked graphene oxide (GO) 3D aerogels with large specific surface area, outstanding mechanical performance, and superhigh chemical activity are fabricated by assembling 2D GO sheets edge-to-edge into uniform, 3D hydrogel networks with subsequent supercritical fluid drying. These aerogels are superior to 3D frameworks assembled via partial overlapping of the basal planes of the 2D building blocks.

    3. Universal Rule on Chirality-Dependent Bandgaps in Graphene Antidot Lattices (pages 1405–1410)

      Xiaofei Liu, Zhuhua Zhang and Wanlin Guo

      Article first published online: 26 MAR 2013 | DOI: 10.1002/smll.201202988

      Thumbnail image of graphical abstract

      Graphene with periodically patterned antidots represents a facile route to open a bandgap for graphene electronics. It's found that bandgaps in graphene antidot lattices are well defined by a chirality vector R = na1+ma2. The bandgap opens when (n-m)mod3 is 0 but remains to be closed when (n-m)mod3 is ±1, reminiscent of the gap-chirality rule in carbon nanotubes.

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