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Synergistic Cascade Hydrogen Evolution Boosting via Integrating Surface Oxophilicity Modification with Carbon Layer Confinement
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2021-10-14 , DOI: 10.1002/adfm.202108991
Feixiang Bao 1 , Zhilong Yang 1 , Yuliang Yuan 1 , Penglin Yu 1 , Gangming Zeng 1 , Yi Cheng 2 , Yangfan Lu 3 , Jiawei Zhang 1 , Hongwen Huang 1
Affiliation  

The lack of highly efficient catalysts severely hinders large-scale application of electrochemical hydrogen evolution reaction (HER) for hydrogen production from water. Herein, synergistic cascade hydrogen evolution boosting by combining the strategies of carbon layer confinement and surface oxophilicity modification is realized. The carbon layers confined ultrafine RuCr nanoparticles (RuCr@C) exhibit outstanding HER activity (j10 = 19 mV, turnover frequency = 4.25 H2 s-1), surpassing the benchmark Pt/C and most of the reported HER catalysts. Combined experimental verifications and theoretical simulations reveal that surface adsorption modification and electronic structure regulation synergistically boosts the HER kinetics over the RuCr@C catalyst. The Volmer step is accelerated by stabilizing the final state of water dissociation (*H and *OH) through Cr doping, and the Heyrovsky step is promoted via carbon layers confinement. As such, this work highlights a synergistic cascade strategy to boost HER kinetics which is of fundamental importance to accelerate future advances in electrocatalysis.

中文翻译:

通过将表面亲氧性改性与碳层限制相结合的协同级联析氢促进

缺乏高效催化剂严重阻碍了电化学析氢反应(HER)在水制氢中的大规模应用。在此,通过结合碳层限制和表面亲氧性改性的策略,实现了协同级联析氢助推。碳层限制的超细RuCr纳米颗粒(RuCr@C)表现出出色的HER活性(j 10 = 19 mV,转换频率= 4.25 H 2 s -1),超过了基准 Pt/C 和大多数报道的 HER 催化剂。结合实验验证和理论模拟表明,表面吸附改性和电子结构调节协同提高了 RuCr@C 催化剂的 HER 动力学。通过 Cr 掺杂稳定水解离的最终状态(*H 和 *OH)来加速 Volmer 步骤,并通过碳层限制促进 Heyrovsky 步骤。因此,这项工作强调了一种协同级联策略来提高 HER 动力学,这对于加速电催化的未来发展至关重要。
更新日期:2021-10-14
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