Cascade electrocatalysis via integrating ruthenium clusters and yttrium single atoms for boosted alkaline hydrogen evolution

IF 32.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Haotian Zhang, Haoran Guo, Fuhui Zhang, Jinyang Zhang, Yizhuo Cheng, Yanqing Ma, Lei Ma, Limin Qi
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引用次数: 0

Abstract

Anion-exchange-membrane water electrolysis (AEMWE) has emerged as a highly prospective technology for large-scale hydrogen production. However, its widespread application is severely restricted by the sluggish kinetics of alkaline hydrogen evolution reaction (HER). Inspired by enzymatic cascade reactions, this work proposes a novel cascade electrocatalysis mechanism for alkaline HER on a supported metal catalyst comprising Ru clusters and Y single atoms simultaneously immobilized on a N-doped carbon support (Ru-YNC). Specifically, oxophilic Y single atoms serve as preferential water adsorption and dissociation centers, and the generated hydrogen adsorption intermediates are promptly captured and reduced by adjacent Ru clusters owing to the different adsorption properties of Ru and Y species, thereby remarkably accelerating the alkaline HER kinetics. Consequently, the Ru-YNC exhibits an overpotential of only 22 mV at 10 mA cm-2 in 1.0 M KOH. The assembled AEMWE electrolyzer delivers a current density of 1000 mA cm-2 and a remarkable noble metal mass activity of 52.07 A mgnoble metal-1 at a cell voltage of 1.87 V. Furthermore, it shows outstanding durability over 1000 h at 500 mA cm-2 with a degradation rate of only 40 μV h-1. This work provides new insights into catalyst design and mechanism exploration for electrochemical alkaline HER.
通过整合钌簇和钇单原子的级联电催化促进碱性氢的析出
阴离子交换膜电解(AEMWE)是一种极具发展前景的大规模制氢技术。然而,碱性析氢反应(HER)动力学缓慢严重制约了其广泛应用。受酶级联反应的启发,本研究提出了一种新型的碱性HER级联电催化机制,该机制在负载金属催化剂上由Ru簇和Y单原子同时固定在n掺杂碳载体(Ru- ync)上。具体来说,亲氧的Y单原子作为优先的水吸附和解离中心,由于Ru和Y两种物质的不同吸附性质,生成的氢吸附中间体被相邻的Ru团簇迅速捕获和还原,从而显著加快了碱性HER动力学。因此,在1.0 M KOH条件下,Ru-YNC在10 mA cm-2下的过电位仅为22 mV。组装的AEMWE电解槽在1.87 V的电池电压下,电流密度为1000 mA cm-2,贵金属质量活性为52.07 a mg -1。此外,在500 mA cm-2条件下,该材料的耐久时间超过1000 h,降解率仅为40 μV h-1。本研究为电化学碱性HER的催化剂设计和机理探索提供了新的思路。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Energy & Environmental Science
Energy & Environmental Science 化学-工程:化工
CiteScore
50.50
自引率
2.20%
发文量
349
审稿时长
2.2 months
期刊介绍: Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences." Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).
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