TU Darmstadt, Graduate School of Excellence Energy Science and Engineering, Otto-Berndt-Str. 3, 64287, Darmstadt, Germany.
TU Darmstadt, Department of Chemistry, Otto-Berndt-Str. 3, 64287, Darmstadt, Germany.
Chemistry. 2018 Aug 27;24(48):12480-12484. doi: 10.1002/chem.201802684. Epub 2018 Jul 25.
Today, metal-N- as well as metal-S-doped carbon materials are known to catalyze the hydrogen evolution reaction (HER). However, especially N- and S-co-doped catalysts reach highest activity, but it remains unclear if the activity is related to MN or MS (M=metal) sites. In this work we apply a simple method for multi-heteroatom doping and investigate the effect of cobalt content on the HER in acidic medium. The CoN and CoS sites were evidenced on the basis of structural characterization by Raman, X-ray induced photoelectron spectroscopy, and TEM. The presence of sulfur enables the formation of a larger number of CoN sites. Structure-performance relationship proves that the HER activity is dominated by CoN rather than CoS sites. The most active catalysts also exhibit an excellent stability under galvanostatic conditions making them of interest for electrolyser application.
如今，已知金属-N 和金属-S 掺杂的碳材料可以催化析氢反应（HER）。然而，特别是 N 和 S 共掺杂的催化剂达到了最高的活性，但仍不清楚这种活性是否与 MN 或 MS（M=金属）位点有关。在这项工作中，我们应用了一种简单的多杂原子掺杂方法，并研究了钴含量对酸性介质中 HER 的影响。根据拉曼、X 射线光电子能谱和 TEM 的结构表征，证明了 CoN 和 CoS 位点的存在。硫的存在使得形成更多数量的 CoN 位点成为可能。结构-性能关系证明，HER 活性主要由 CoN 而不是 CoS 位点决定。最活跃的催化剂在恒电流条件下也表现出优异的稳定性，这使得它们在电解槽应用中具有吸引力。
