通过 Ru-Sn 双金属位和新型羟基溢出效应实现高效碱性氢进化

IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Analytical Chemistry Pub Date : 2024-09-28 DOI:10.1002/adma.202411942
Zhen-Tong Yan, Shi Tao, Juan Wang, Xiu-Li Lu, Tong-Bu Lu
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引用次数: 0

摘要

碱性氢进化反应(HER)在实际制氢中具有巨大潜力,但仍受限于活性和稳定性电催化剂的缺乏。本文首次在一种名为 Ru-Sn/SnO2 NS 的协同电催化剂上实现了高效的水解离过程、吸附羟基的快速转移和优化的氢吸附,该催化剂基于多孔 Ru 纳米片构建了 Ru-Sn 双金属位点和 SnO2 异质结。密度泛函理论(DFT)计算和原位红外光谱表明,Ru-Sn双金属位点能优化水的解离过程和氢的吸附,而SnO2的存在能诱导独特的羟基溢出效应,加速羟基转移过程,避免活性位点中毒。研究结果表明,Ru-Sn/SnO2 NS 具有显著的碱性 HER 性能,过电位极低(10 mA cm-2 时为 12 mV),稳定性强(650 h),远优于 Ru NS(10 mA cm-2 时为 27 mV,稳定性为 90 h)和 Ru-Sn NS(10 mA cm-2 时为 16 mV,稳定性为 120 h)。这项研究为设计高效的碱性 HER 电催化剂提供了新的思路。
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Unlocking Efficient Alkaline Hydrogen Evolution Through Ru–Sn Dual Metal Sites and a Novel Hydroxyl Spillover Effect
Alkaline hydrogen evolution reaction (HER) has great potential in practical hydrogen production but is still limited by the lack of active and stable electrocatalysts. Herein, the efficient water dissociation process, fast transfer of adsorbed hydroxyl and optimized hydrogen adsorption are first achieved on a cooperative electrocatalyst, named as Ru–Sn/SnO2 NS, in which the Ru–Sn dual metal sites and SnO2 heterojunction are constructed based on porous Ru nanosheet. The density functional theory (DFT) calculations and in situ infrared spectra suggest that Ru–Sn dual sites can optimize the water dissociation process and hydrogen adsorption, while the existence of SnO2 can induce the unique hydroxyl spillover effect, accelerating the hydroxyl transfer process and avoiding the poison of active sites. As results, Ru–Sn/SnO2 NS display remarkable alkaline HER performance with an extremely low overpotential (12 mV at 10 mA cm−2) and robust stability (650 h), much superior to those of Ru NS (27 mV at 10 mA cm−2 with 90 h stability) and Ru–Sn NS (16 mV at 10 mA cm−2 with 120 h stability). The work sheds new light on designing of efficient alkaline HER electrocatalyst.
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来源期刊
Analytical Chemistry
Analytical Chemistry 化学-分析化学
CiteScore
12.10
自引率
12.20%
发文量
1949
审稿时长
1.4 months
期刊介绍: Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.
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