Nature Communications ( IF 14.7 ) Pub Date : 2023-07-14 , DOI: 10.1038/s41467-023-39963-8 Xiaozhong Zheng 1 , Xiaoyun Shi 1 , Honghui Ning 1 , Rui Yang 1 , Bing Lu 1 , Qian Luo 1 , Shanjun Mao 1 , Lingling Xi 1 , Yong Wang 1, 2
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-HxWO3 catalyst is readily synthesized and exhibits enhanced performance for neutral hydrogen evolution reaction. HxWO3 support is functioned as proton sponge to create a local acid-like microenvironment around Ir metal sites by spontaneous injection of protons to WO3, as evidenced by spectroscopy and electrochemical analysis. Rationalize revitalized lattice-hydrogen species located in the interface are coupled with Had atoms on metallic Ir surfaces via thermodynamically favorable Volmer-Tafel steps, and thereby a fast kinetics. Elaborated Ir-HxWO3 demonstrates acid-like activity with a low overpotential of 20 mV at 10 mA cm−2 and low Tafel slope of 28 mV dec−1, 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.
中文翻译:
定制局部类酸微环境以有效释放中性氢
中性介质中的电化学析氢反应由于动力学缓慢而被列为能源催化领域最困难的挑战。在此,Ir-H x WO 3催化剂易于合成并且表现出增强的中性析氢反应性能。H x WO 3载体充当质子海绵,通过向WO 3自发注入质子,在Ir金属位点周围创建局部类酸微环境,如光谱学和电化学分析所证明。合理化位于界面的再生晶格氢物种与 H ad耦合通过热力学有利的 Volmer-Tafel 步骤,金属 Ir 表面上的原子,从而实现快速动力学。精心设计的Ir-H x WO 3表现出类酸活性,在10 mA cm -2下具有20 mV的低过电势和28 mV dec -1的低塔菲尔斜率,甚至可以与酸性环境中的活性相媲美。这项工作中例证的概念为定制局部反应微环境以调节催化活性和途径提供了可能性。