期刊
ACS CATALYSIS
卷 8, 期 2, 页码 987-996出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.7b02617
关键词
iron nickel sulfide; pentlandite; surface composition; hydrogen evolution; electrocatalysis; electrochemistry; HER
资金
- Fonds of the Chemical Industry (Liebig grant)
- Deutsche Forschungsgemeinschaft (Emmy Noether grant) [AP242/2-1]
- Deutsche Forschungsgemeinschaft [EXC 1069]
Inspired by our recent finding that Fe4.5Ni4.5S8 rock is a highly active electrocatalyst for HER, we set out to explore the influence of the Fe:Ni ratio on the performance of the catalyst. We herein describe the synthesis of (FexNi1-x)(9)S-8 (x = 0-1) along with a detailed elemental composition analysis. Furthermore, using linear sweep voltammetry, we show that the increase in the iron or nickel content, respectively, lowers the activity of the electrocatalyst toward HER Electrochemical surface area analysis (ECSA) clearly indicates the highest amount of active sites for a Fe:Ni ratio of 1:1 on the electrode surface pointing at an altered surface composition of iron and nickel for the other materials. Specific metal-metal interactions seem to be of key importance for the high electrocatalytic HER activity, which is supported by DFT calculations of several surface structures using the surface energy as a descriptor of catalytic activity. In addition, we show that a temperature increase leads to a significant decrease of the overpotential and gain in HER activity. Thus, we showcase the necessity to investigate the material structure, composition and reaction conditions when evaluating electrocatalysts.
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