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Author: Zhang, Hua × Type: Text ×

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    Covalent Organic Frameworks for Efficient Energy Electrocatalysis: Rational Design and Progress
    (Weinheim : Wiley-VCH, 2021) Zhang, Hua; Zhu, Minshen; Schmidt, Oliver G.; Chen, Shuillang; Zhang, Kai
    An efficient catalyst with a precisely designed and predictable structure is highly desired to optimize its performance and understand the mechanism beyond the catalytic activity. Covalent organic frameworks (COFs), as an emerging class of framework materials linked by strong covalent bonds, simultaneously allow precise structure design with predictable synthesis and show advantages of large surface areas, tunable pore sizes, and unique molecular architectures. Although the research on COF‐based electrocatalysts is at an early age, significant progress has been made. Herein, the recent significant progress in the design and synthesis of COFs as highly efficient electrocatalysts for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER) is summarized. Design principles for COFs as efficient electrocatalysts are discussed by considering essential factors for catalyzing the OER, ORR, and HER processes at the molecular level. Herein, a summary on the in‐depth understanding of the catalytic mechanism and kinetics limitations of COFs provides a general instruction for further exploring their vast potential for designing highly efficient electrocatalysts.
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    Engineering grain boundaries at the 2D limit for the hydrogen evolution reaction
    ([London] : Nature Publishing Group UK, 2020) He, Yongmin; Tang, Pengyi; Hu, Zhili; He, Qiyuan; Zhu, Chao; Wang, Luqing; Zeng, Qingsheng; Golani, Prafful; Gao, Guanhui; Fu, Wei; Huang, Zhiqi; Gao, Caitian; Xia, Juan; Wang, Xingli; Wang, Xuewen; Zhu, Chao; Ramasse, Quentin M.; Zhang, Ao; An, Boxing; Zhang, Yongzhe; Martí-Sánchez, Sara; Morante, Joan Ramon; Wang, Liang; Tay, Beng Kang; Yakobson, Boris I.; Trampert, Achim; Zhang, Hua; Wu, Minghong; Wang, Qi Jie; Arbiol, Jordi; Liu, Zheng
    Atom-thin transition metal dichalcogenides (TMDs) have emerged as fascinating materials and key structures for electrocatalysis. So far, their edges, dopant heteroatoms and defects have been intensively explored as active sites for the hydrogen evolution reaction (HER) to split water. However, grain boundaries (GBs), a key type of defects in TMDs, have been overlooked due to their low density and large structural variations. Here, we demonstrate the synthesis of wafer-size atom-thin TMD films with an ultra-high-density of GBs, up to ~1012 cm−2. We propose a climb and drive 0D/2D interaction to explain the underlying growth mechanism. The electrocatalytic activity of the nanograin film is comprehensively examined by micro-electrochemical measurements, showing an excellent hydrogen-evolution performance (onset potential: −25 mV and Tafel slope: 54 mV dec−1), thus indicating an intrinsically high activation of the TMD GBs.