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A Stable and Conductive Metallophthalocyanine Framework for Electrocatalytic Carbon Dioxide Reduction in Water

Angewandte Chemie 2020年第38期132卷

作者： Huang N. Lee K.H. Yue Y. Xu X. Irle S. Jiang Q. Jiang D. Department of Chemistry Faculty of Science National University of Singapore 3 Science Drive 3 Singapore 117543 Singapore MOE Key Laboratory of Macromolecular Synthesis and Functionalization State Key Laboratory of Silicon Materials Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China Bredesen Centre for Interdisciplinary Research and Graduate Education University of Tennessee Knoxville TN 37996 United States Computational Sciences and Engineering Division & Chemical Sciences Division Oak Ridge National Laboratory Oak Ridge TN 37831 United States Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University Binhai New City Fuzhou 350207 China

Transformation of carbon dioxide to high value-added chemicals becomes a significant challenge for clean energy studies. Here a stable and conductive covalent organic framework was developed for electrocatalytic carbon dioxide reduction to carbon monoxide in aqueous solution. The cobalt(II) phthalocyanine catalysts are topologically connected via robust phenazine linkage into a two-dimensional tetragonal framework that is stable under boiling water, acid, or base conditions. The 2D lattice enables full π conjugation along x and y directions as well as π conduction along the z axis across the π columns. With these structural features, the electrocatalytic framework exhibits a faradaic efficiency of 96 %, an exceptional turnover number up to 320 000, and a long-term turnover frequency of 11 412 hour−1, which is a 32-fold improvement over molecular catalyst. The combination of catalytic activity, selectivity, efficiency, and durability is desirable for clean energy production. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

关键词： 2D polymers CO2 reduction covalent organic frameworks electrocatalysis π conjugation

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A Mini Review on Nanocarbon-Based 1D Macroscopic Fibers:Assembly Strategies and Mechanical Properties

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Nano-Micro Letters 2017年第4期9卷 175-192页

作者： Liang Kou Yingjun Liu Cheng Zhang Le Shao Zhanyuan Tian Zengshe Deng Chao Gao Shaanxi Coal and Chemical Technology Institute Co. Ltd MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Donghua University

Nanocarbon-based materials, such as carbon nanotubes(CNTs) and graphene have been attached much attention by scientific and industrial community. As two representative nanocarbon materials, one-dimensional CNTs and twodimensional graphene both possess remarkable mechanical properties. In the past years, a large amount of work have been done by using CNTs or graphene as building blocks for constructing novel, macroscopic, mechanically strong fibrous materials. In this review, we summarize the assembly approaches of CNT-based fibers and graphene-based fibers in chronological order, respectively. The mechanical performances of these fibrous materials are compared, and the critical influences on the mechanical properties are discussed. Personal perspectives on the fabrication methods of CNT-and graphene-based fibers are further presented.

关键词： One dimensional Macroscopic architectures Carbon nanotubes Graphene fibers Assembly strategies Mechanical performance

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Dual-Emissive Platinum(II) Metallacage with a Sensitive Oxygen Response for Imaging of Hypoxia and Imaging-Guided Chemotherapy

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Angewandte Chemie 2020年第45期132卷

作者： Zhu H. Li Q. Shi B. Ge F. Liu Y. Mao Z. Wang S. Yu G. Huang F. Stang P.J. State Key Laboratory of Chemical Engineering Center for Chemistry of High-Performance & Novel Materials Department of Chemistry Zhejiang University Hangzhou 310027 China Department of Chemistry University of Utah Salt Lake City UT 84112 United States College of Pharmaceutical Science Zhejiang University Hangzhou 310058 China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China School of Life Sciences Tianjin University and Tianjin Engineering Center of Micro-Nano Biomaterials and Detection-Treatment Technology Tianjin 300072 China Green Catalysis Center and College of Chemistry Zhengzhou University Zhengzhou 450001 China

Imaging of hypoxia in vivo helps with accurate cancer diagnosis and evaluation of therapeutic outcomes. A PtII metallacage with oxygen-responsive red phosphorescence and steady fluorescence for in vivo hypoxia imaging and chemotherapy is reported. The therapeutic agent and diagnostic probe were integrated into the metallacage through heteroligation-directed self-assembly. Nanoformulation by encapsulating the metallacage into nanoparticles greatly enhanced its stability the in physiological environment, rendering biomedical applications feasible. Apart from enhanced red phosphorescence upon hypoxia, the ratio between red and blue emissions, which only varies with intracellular oxygen level, provides a more precise standard for hypoxia imaging and detection. Moreover, in vivo explorations demonstrate the promising potential applications of the metallacage-loaded nanoparticles as theranostic agents for tumor hypoxia imaging and chemotherapy. © 2020 Wiley-VCH GmbH

关键词： hypoxia imaging metallacages platinum self-assembly supramolecular chemistry

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Special Photophysical Properties of Poly(2,11-diquinoxalinopyrene)s

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Chinese Journal of Polymer Science 2017年第9期35卷 1097-1109页

作者： Ming-jian Jiang Xin-yuan Li Lei-tao Sun Xiao-long Niu Qiu-min Liang Xiao-qiang Cai Jin-chang Huang 凌军莫越奇 College of Materials Science andEngineering South China University of Technology Guangzhou 510640 China Ministry of Education Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou 31002 7 China

A diquinoxalinopyrene （DQP） derivative and the corresponding oligomers （PDQPs） with Mn of ca. 3300, 4200, 5600, and 7300 have been synthesized. It is found that the band gaps and highest occupied molecular orbital （HOMO）/lowest unoccupied molecular orbital （LUMO） levels between DQP and its homopolymers only have a slight difference, implying a limited conjugation extension achieved from unimer to heptamer. The DFT calculation is in accordance with the experimental results. It reveals that the nodal planes are across the 2,11-positions in the LUMO and/or HOMO of DQP, dimer and trimer, which can be used to explain this special phenomenon.

关键词： Polydiquinoxalinopyrene Photophysical properties Nodal

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Engineered Coatings via the Assembly of Amino-Quinone Networks

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Angewandte Chemie 2020年第5期133卷

作者： Qi-Zhi Zhong Dr. Joseph J. Richardson Ai He Dr. Tian Zheng Dr. René P. M. Lafleur Dr. Jianhua Li Dr. Wen-Ze Qiu Denzil Furtado Dr. Shuaijun Pan Prof. Zhi-Kang Xu Prof. Ling-Shu Wan Prof. Frank Caruso MOE Key Laboratory of Macromolecular Synthesis and Functionalization Key Laboratory of Adsorption and Separation Materials & Technologies of Zhejiang Province Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China ARC Centre of Excellence in Convergent Bio-Nano Science and Technology and the Department of Chemical Engineering The University of Melbourne Parkville Victoria 3010 Australia

Engineering coatings with precise physicochemical properties allows for control over the interface of a material and its interactions with the surrounding environment. However, assembling coatings with well-defined properties on different material classes remains a challenge. Herein, we report a co-assembly strategy to precisely control the structure and properties (e.g., thickness, adhesion, wettability, and zeta potential) of coatings on various materials (27 substrates examined) using quinone and polyamine building blocks. By increasing the length of the amine building blocks from small molecule diamines to branched amine polymers, we tune the properties of the films, including the thickness (from ca. 5 to ca. 50 nm), interfacial adhesion (0.05 to 5.54 nN), water contact angle (130 to 40°), and zeta potential (−42 to 28 mV). The films can be post-functionalized through the in situ formation of diverse nanostructures, including nanoparticles, nanorods, and nanocrystals. Our approach provides a platform for the rational design of engineered, substrate-independent coatings for various applications.

关键词： nanostructures quinones self-assembly surface modification thin films

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Shape change of calcite single crystals to accommodate interfacial curvature:Crystallization in presence of Mg2+ions and agarose gel-networks

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Chinese Chemical Letters 2017年第4期28卷 857-862页

作者： Tao Ye Xin-Yi Jin Liao Chen Chong Hu Jie Ren Yu-Jing Liu Gang Wu Lu-Jian Chen Hong-Zheng Chen Han-Ying Li MOE Key Laboratory of Macromolecular Synthesis and Functionalization State Key Laboratory of Silicon MaterialsDepartment of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China Department of Electronic Engineering School of Information Science and EngineeringXiamen UniversityXiamen 361005China

Synthetic calcite single crystals,due to their strong crystal habit,tend to grow into characteristic *** the nature,biogenic calcite crystals form composites together with biomacromolecular materials,spurring investigations of how the growing calcite single crystals change their habit to satisfy the curvature of the organic *** this work,we examine calcite crystallization on a flat surface of glass slide and a curved surface of polystyrene（PS） *** crystals exhibit tiny contact area onto the glass substrate that is averagely only 15%of their projected area on the *** sharp contrast,the contact area greatly increase to above 75%of the projected area,once magnesium ions or agarose gel networks are introduced into the crystallization ***,the calcite crystals form rough and step-like interfaces with a curved ***,the interfaces become smooth and curved as the crystals grow in presence of magnesium ions or agarose gel *** discrepancy between the interfacial structures implies kinetic effects of the additives on the crystallization around the *** work may provide implications for understanding the formation mechanisms of single-crystal composite materials.

关键词： Calcite Single crystal Gel-incorporation Magnesium Interface

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Long-range ordering of composites for organic electronics:TIPS-pentacene single crystals with incorporated nano-fibers

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Chinese Chemical Letters 2017年第11期28卷 2121-2124页

作者： Huanbin Li Guobiao Xue Jiake Wu Wenqiang Zhang Zhuoting Huang Zengqi Xie Huolin L.Xin Gang Wu Hongzheng Chen Hanying Li State Key Laboratory of Silicon Materials MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Institute of Polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and Devices South China University of Technology Center for Functional Nanomaterials Brookhaven National Laboratory

Multi-component active materials are widely used for organic electronic devices, with every component contributing complementary and synergistic optoelectronic functions. Mixing these components generally leads to lowered crystallinity and weakened charge transport. Therefore, preparing the active materials without substantially disrupting the crystalline lattice is highly desired. Here, we show that crystallization of TIPS-pentacene from solutions in the presence of fluorescent nanofibers of a perylene bisimide derivative （PBI） leads to formation of composites with nanoflber guest incorporated in the crystal host. In spite of the binary composite structure, the TIPS-pentacene maintains the single- crystalline nature. As a result, the incorporation of the PB1 guest introduces additional fluorescence function but does not significantly reduce the charge transport property of the TIPS-pentacene host, exhibiting field-effect mobility as high as 3.34 cm^2 V^-1 s^-1 even though 26.4% of the channel area is taken over by the guest. As such, this work provides a facile approach toward high-performance multifunctional organic electronic materials.

关键词： Organic Electronics Single Crystals Composites High Mobility Field-Effect Transistors

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Electron Beam Lithography: CO2-Based Dual-Tone Resists for Electron Beam Lithography (Adv. Funct. Mater. 13/2021)

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Advanced Functional Materials 2021年第13期31卷

作者： Xin-Yu Lu Hao Luo Kai Wang Yao-Yao Zhang Xiao-Feng Zhu Dongxue Li Bingze Ma Shisheng Xiong Paul F. Nealey Qiang Li Guang-Peng Wu MOE Laboratory of Macromolecular Synthesis and Functionalization Adsorption and Separation Materials and Technologies of Zhejiang Province Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China State Key Laboratory of Modern Optical Instrumentation College of Optical Science and Engineering Zhejiang University Hangzhou 310027 China Pritzker School of Molecular Engineering University of Chicago Chicago IL 60637 USA Materials Science Division Argonne National Laboratory 9700 S Cass Avenue Argonne IL 60439 USA School of Information Science and Technology Fudan University Shanghai 200433 China State Key Lab of ASIC and System School of Microelectronics Fudan University Shanghai 200433 China

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Macroscopic Assembled Graphene for Silicon Mid-Infrared Photodetectors

Research Square

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Research Square 2020年

作者： Gao, Chao Peng, Li Du, Sichao Liu, Lixiang Bodepudi, Srikrishna Chanakya Li, Lingfei Liu, Wei Cong, Xin Lai, Runchen Fang, Wenzhang Cao, Xiaoxue Liu, Xinyu Abid, Muhammad Lv, Jianhang Liu, Junxue Jin, Shengye Wu, Kaifeng Zhou, Qiaohui Zhu, Haiming Lin, Miao-Ling Tan, Ping-Heng Xiong, Qihua Wang, Xiaomu Hu, Weida Duan, Xiangfeng Yu, Bin Yin, Wenyan Xu, Zhen Xu, Yang MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University Hangzhou310027 China Colleges of ISEE and Microelectronics State Key Laboratories of Modern Optical Instrumentation and Silicon Materials Hangzhou Global Scientific and Technological Innovation Center ZJU-UIUC Joint Institute Zhejiang University Hangzhou310027 China State Key Laboratory of Superlattices and Microstructures Institute of Semiconductors Chinese Academy of Sciences Beijing100083 China State Key Laboratory of Molecular Reaction Dynamics and Dynamics Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian116023 China Department of Chemistry Zhejiang University Hangzhou310027 China Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University 637371 Singapore National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced Microstructure School of Electronic Science and Engineering Nanjing University Nanjing210093 China National Laboratory for Infrared Physics Shanghai Institute of Technical Physics Chinese Academy of Sciences Shanghai200083 China Department of Chemistry and Biochemistry California Nanosystems Institute University of California Los Angeles90095 United States

Graphene with linear energy dispersion and weak electron-phonon interaction is highly anticipated to harvest hot-electrons in a broad wavelength range from ultraviolet to terahertz1,2. However, the limited absorption (~2.3%) and serious backscattering of hot-electrons associated with single-layer graphene result in inadequate quantum yields3-5, impeding their practically broadband photodetection, especially in the mid-infrared range. Here, we report a macroscopic assembled graphene (MAG)/silicon heterojunction for ultrafast mid-infrared photodetection. The highly crystalline 2-inch scale MAG with tunable thickness from 10 to 60 nm is produced by scalable wet-assembly of commercial graphene oxide followed by thermal annealing. The MAG/Si Schottky diode exhibits broadband photodetection capability in 1-10 μm at room temperature with fast response (120-130 ns, 4 mm2 window) and high detectivity (1011 to 106 Jones), outperforming single-layer graphene/Si photodetectors by 2 to 8 orders in transient photocurrent. This optoelectronic performance is attributed to the superior advantages of MAG (~40% of light absorption, ~23 ps of carrier relaxation time, and high quasi-equilibrated hot-carrier-multiplication gain), atomic-scale contact interface of MAG and silicon, and impact-ionization avalanche gain (~102 times) from silicon. The MAG provides a long-range platform to understand the hot-carrier dynamics in stacked 2D materials, leading to next-generation broadband silicon-based image sensors. © 2020, CC BY.

关键词： Graphene

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A-D-A small molecule donors based on pyrene and diketopyrrolopyrrole for organic solar cells

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Science China Chemistry 2017年第4期60卷 561-569页

作者： Jing-Qi Xu Wenqing Liu Shi-Yong Liu Jun Ling Jiangquan Mai Xinhui Lu Chang-Zhi Li Alex K.-Y. Jen Hongzheng Chen Key Laboratory of Macromolecular Synthesis and Functionalization Ministry of Education State Key Laboratory of Silicon Materials Department of Polymer Science and Engineering Zhejiang University Hangzhou 310027 China Department of Physics Chinese University of Hong Kong New Territories China Department of Materials Science & Engineering University of Washington Seattle Washington 98195 USA

Three new electron donating small molecules （SMs）, Pyr（EH-DPP）2, Pyr（HD-DPP）2 and PyrA（EH-DPP）2, are designed and synthesized through coupling electron rich pyrene core with electron deficient diketopyrrolopyrrole （DPP） terminals, of which the derived organic solar cells （OSCs） exhibit interesting structure-performance correlation. It shows that the tune of their solubilizing side chains and n-bridge for the acceptor-donor-acceptor （A-D-A） SMs can significantly alter the resultant short-circuit current density and power conversion efficiency （PCE） in OSCs. The Pyr（EH-DPP）2 with short side chains displays broader absorption and higher hole mobility than the Pyr（HD-DPP）2 with long side chains. Although showing planar structure, the acetylene bridge-incorporated PyrA（EH-DPP）2 adapts an undesired edge-on packing and strong aggregation in film, leading to non-ideal morphology and poor miscibility with fullerene acceptors. As a result, the PCE of the solar cell based on Pyr（EH-DPP）2 is several times higher than those based on Pyr（HD-DPP）： and PyrA（EH-DPP）2, indicating the A-D-A combination of polyaromatics with DPP would be the promising skeleton for developing photovoltaic semiconductors.

关键词： solution-processed small molecules diketopyrrolopyrrole pyrene organic solar cells

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