Advanced Materials and Catalysis Group, Center of Chemistry for Frontier Technologies, State Key Laboratory of Clean Energy Utilization, Institute of Catalysis, Department of Chemistry, Zhejiang University, 310028, Hangzhou, P. R. China.
College of Chemistry and Molecular Engineering, Zhengzhou University, 450001, Zhengzhou, China.
Nat Commun. 2023 Jul 14;14(1):4209. doi: 10.1038/s41467-023-39963-8.
Electrochemical hydrogen evolution reaction in neutral media is listed as the most difficult challenges of energy catalysis due to the sluggish kinetics. Herein, the Ir-HWO catalyst is readily synthesized and exhibits enhanced performance for neutral hydrogen evolution reaction. HWO support is functioned as proton sponge to create a local acid-like microenvironment around Ir metal sites by spontaneous injection of protons to WO, as evidenced by spectroscopy and electrochemical analysis. Rationalize revitalized lattice-hydrogen species located in the interface are coupled with H atoms on metallic Ir surfaces via thermodynamically favorable Volmer-Tafel steps, and thereby a fast kinetics. Elaborated Ir-HWO demonstrates acid-like activity with a low overpotential of 20 mV at 10 mA cm and low Tafel slope of 28 mV dec, which are even comparable to those in acidic environment. The concept exemplified in this work offer the possibilities for tailoring local reaction microenvironment to regulate catalytic activity and pathway.
电化学中性介质中的析氢反应因其动力学缓慢而被列为能源催化中最具挑战性的难题之一。在此,我们制备了 Ir-HWO 催化剂,该催化剂在中性析氢反应中表现出了增强的性能。HWO 载体通过自发向 WO 注入质子,起到质子海绵的作用,在 Ir 金属位点周围创造局部类似酸的微环境,这一点可以通过光谱和电化学分析得到证明。合理化的晶格氢物种位于界面处,并通过热力学有利的 Volmer-Tafel 步骤与金属 Ir 表面上的 H 原子耦合,从而实现快速动力学。详细研究表明,Ir-HWO 具有类似酸的活性,在 10 mA cm 处的过电势低至 20 mV,Tafel 斜率低至 28 mV dec,这与在酸性环境中的性能相当。这项工作中举例说明的概念为调节催化活性和途径提供了定制局部反应微环境的可能性。