State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, China.
School of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot, 010000, China.
Small. 2023 May;19(21):e2207146. doi: 10.1002/smll.202207146. Epub 2023 Feb 11.
Developing high-performance electrocatalysts toward hydrogen evolution reaction (HER) is important for clean and sustainable hydrogen energy, yet still challenging. Herein, an α-MoC induced redispersing strategy to construct a superior HER electrocatalyst (Pt/CNTs-N + α-MoC ) by mechanical mixing of α-MoC with Pt/CNTs-N followed by thermal reduction is reported. It is found that thermo-activation treatment enables partial Pt atoms to redisperse on α-MoC substrate from carbon nanotubes, which creates dual active interfaces of Pt species dispersed over carbon nanotubes and α-MoC . Benefiting from the strong electronic interaction between the Pt atom and α-MoC , the utilization efficiency of the Pt atom and the zero-valence state of Pt is evidently enhanced. Consequently, Pt/CNTs-N + α-MoC catalyst exhibits excellent HER activity with low overpotentials of 17 and 34 mV to achieve a current density of 10 mA cm in acidic and alkaline electrolytes, respectively. Density functional theory calculations further reveal that the synergistic effect between Pt and α-MoC makes it accessible for the dissociation of water molecules and subsequent desorption of hydrogen atoms. This work reveals the crucial roles of α-MoC additives, providing practical solutions to enhance platinum dispersion, and thereby enhance the catalytic activity in HER.
开发用于析氢反应(HER)的高性能电催化剂对于清洁可持续的氢能至关重要,但仍然具有挑战性。本文报道了一种通过α-MoC 与 Pt/CNTs-N 机械混合,随后热还原来构建具有优异 HER 电催化剂(Pt/CNTs-N+α-MoC)的α-MoC 诱导再分散策略。研究发现,热激活处理使部分 Pt 原子从碳纳米管上重新分散在α-MoC 载体上,从而在碳纳米管和α-MoC 上形成 Pt 物种分散的双活性界面。得益于 Pt 原子与α-MoC 之间的强电子相互作用,Pt 原子的利用率和 Pt 的零价态明显提高。因此,Pt/CNTs-N+α-MoC 催化剂在酸性和碱性电解液中分别表现出优异的 HER 活性,其达到 10 mA cm-2 的电流密度时所需的过电位仅为 17 mV 和 34 mV。密度泛函理论计算进一步表明,Pt 和α-MoC 之间的协同效应使得水分子的解离和随后的氢原子脱附变得容易。这项工作揭示了α-MoC 添加剂的关键作用,为增强铂的分散提供了实用的解决方案,从而提高了 HER 中的催化活性。