Chen Chunjun, Sun Xiaofu, Yang Dexin, Lu Lu, Wu Haihong, Zheng Lirong, An Pengfei, Zhang Jing, Han Buxing
Beijing National Laboratory for Molecular Sciences , CAS Key Laboratory of Colloid and Interface and Thermodynamics , CAS Research/Education Center for Excellence in Molecular Sciences , Institute of Chemistry , Chinese Academy of Sciences , Beijing 100190 , P. R. China . Email:
University of Chinese Academy of Sciences , Beijing 100049 , China.
Chem Sci. 2018 Nov 26;10(6):1659-1663. doi: 10.1039/c8sc03986k. eCollection 2019 Feb 14.
The efficient electrochemical reduction of CO to CO in aqueous electrolyte is very interesting. Due to the critical electron-transfer step during the activation of CO, it is important to design efficient strategies to engineer the electronic properties of catalysts to improve the electrochemical performance. Herein cobalt phthalocyanine (CoPc) supported on ZnInS (ZIS) nanosheets was synthesized. It was found that the hybrids showed excellent performance for CO electroreduction to CO in aqueous solution. The faradaic efficiency, current density and mass activity could reach 93%, 8 mA cm and 266 mA mg , respectively. Introduction of Zn-defects resulted in dangling S bonds in the ZIS support, which interacted with Co active sites of CoPc strong Co-S interaction. Mechanistic studies revealed that the enhancement of CO production over CoPc by Co-S interaction originated from the eased CO activation.
在水性电解质中将CO高效电化学还原为CO非常有趣。由于CO活化过程中的关键电子转移步骤,设计有效的策略来调控催化剂的电子性质以改善电化学性能很重要。在此合成了负载在ZnInS(ZIS)纳米片上的钴酞菁(CoPc)。发现该杂化物在水溶液中对CO电还原为CO表现出优异的性能。法拉第效率、电流密度和质量活性分别可达93%、8 mA cm和266 mA mg。引入锌缺陷导致ZIS载体中出现悬空的S键,其与CoPc的Co活性位点相互作用——形成强Co-S相互作用。机理研究表明,Co-S相互作用增强了CoPc上CO的生成,这源于CO活化的缓解。