Chen Hanlin, Si Jincheng, Lyu Siliu, Zhang Tianyu, Li Zhongjian, Lei Chaojun, Lei Lecheng, Yuan Chris, Yang Bin, Gao Liguo, Hou Yang
Key Laboratory of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, 38 Zhejiang University Road, Hangzhou 310027, China.
State Key Laboratory of Fine Chemicals, School Petroleum and Chemical Engineering, Dalian University of Technology, 2 Tai Gong Road, Panjin 124221, China.
ACS Appl Mater Interfaces. 2020 Jun 3;12(22):24675-24682. doi: 10.1021/acsami.9b15039. Epub 2020 May 19.
Developing highly efficient transition metal dichalcogenide electrocatalysts would be significantly beneficial for the electrocatalytic hydrogen evolution reaction (HER) from water splitting. Herein, we reported novel ultrathin tantalum disulfide nanosheets (TaS NSs) prepared by electrochemically exfoliating bulk TaS with an alternating voltage in an acidic electrolyte. The obtained TaS NS electrocatalyst possessed an ultrathin structure with a lateral size of 2 μm and a thickness of ∼3 nm. Owing to the unique 2D structure, the achieved TaS NSs displayed remarkable electrocatalytic activity toward the HER by a small overpotential of 197 mV at 10 mA cm and a small Tafel slope of 100 mV dec in acidic solution, much lower than those of TaS (>547 mV and 216 mV dec, respectively) and other reported TaS-based HER electrocatalysts. Furthermore, highly efficient full water splitting could be realized with two electrodes in which TaS NSs acted as the cathode while Ir/C served as the anode, with help of two AA size batteries or solar cells. By replacing the oxygen evolution reaction with the urea oxidation reaction (UOR), bifunctional TaS NSs enabled an energy-effective HER process in the cathode and UOR process in the anode with decreased applied potential.
开发高效的过渡金属二硫属化物电催化剂对于水分解的电催化析氢反应（HER）将具有显著的益处。在此，我们报道了通过在酸性电解质中用交变电压对块状TaS进行电化学剥离制备的新型超薄二硫化钽纳米片（TaS NSs）。所获得的TaS NS电催化剂具有超薄结构，横向尺寸为2μm，厚度约为3nm。由于独特的二维结构，所制备的TaS NSs在酸性溶液中对HER表现出显著的电催化活性，在10 mA cm时过电位仅为197 mV，塔菲尔斜率为100 mV dec，远低于TaS（分别为>547 mV和216 mV dec）以及其他报道的基于TaS的HER电催化剂。此外，借助两个AA尺寸电池或太阳能电池，以TaS NSs作为阴极，Ir/C作为阳极的双电极体系可实现高效的全水分解。通过用尿素氧化反应（UOR）替代析氧反应，双功能TaS NSs在阴极实现了节能的HER过程，在阳极实现了UOR过程，同时降低了外加电位。
