Liu Changhai, Sun Lei, Luo Linlin, Wang Wenchang, Dong Huilong, Chen Zhidong
School of Materials Science and Engineering, Jiangsu Collaborative Innovation Center of Photovoltaic Science and Engineering, Changzhou University, Changzhou, Jiangsu 213164, China.
School of Petrochemical Engineering, Changzhou University, Changzhou, Jiangsu 213164, China.
ACS Appl Mater Interfaces. 2021 May 19;13(19):22646-22654. doi: 10.1021/acsami.1c04989. Epub 2021 May 11.
Although nonprecious metal catalysts based on earth-abundant 3d transition metals (TMs) are regarded as promising substitutes for a noble metal electrocatalytic hydrogen evolution reaction (HER), their large-scale application is still inhibited by their inadequate activity and durability. Here, a facile method for nonprecious metal catalysts has been developed to prepare molybdenum carbide on nitrogen-doped carbon. By optimizing the Ni doping ratio, the Ni@MoC/NC exhibits the lowest overpotential for 10 mA cm and superior stability in both acidic and alkaline media for HER application, outperforming most of the reported HER electrocatalysts. In addition, a theoretical simulation has also confirmed the possible mechanism for the synergistic effect with the regulative adsorption energy of hydrogen species with Ni doping and formation of a MoC/MoC heterojunction in the Ni@MoC/NC electrocatalyst. Therefore, this work provides a new avenue for designing two-dimensional nanostructures with an optimized electronic structure for promising TM HER electrocatalysts in a wide pH range.
尽管基于储量丰富的3d过渡金属（TMs）的非贵金属催化剂被视为贵金属电催化析氢反应（HER）的有前途的替代品，但其大规模应用仍受到活性和耐久性不足的限制。在此，已开发出一种制备非贵金属催化剂的简便方法，用于在氮掺杂碳上制备碳化钼。通过优化镍掺杂比例，Ni@MoC/NC在10 mA cm时表现出最低的过电位，并且在酸性和碱性介质中用于HER应用时均具有优异的稳定性，优于大多数已报道的HER电催化剂。此外，理论模拟还证实了Ni@MoC/NC电催化剂中镍掺杂对氢物种的调节吸附能以及MoC/MoC异质结形成的协同效应的可能机制。因此，这项工作为设计具有优化电子结构的二维纳米结构提供了一条新途径，以用于在宽pH范围内有前景的TM HER电催化剂。
