Minmin Wang, Chao Feng, Wanliang Mi, Mengdi Guo, Zekun Guan, Min Li, Hsiao-Chien Chen, Yunqi Liu, Yuan Pan
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引用次数: 0
摘要
通过自组装-热解策略从煤沥青中获得了一种锚定铂单原子(SAs)和纳米团簇(NCs)的具有丰富空位缺陷(NSC)的 N、S 共掺杂碳,并提出了一种基于铂 SAs-Pt NCs/NSC 催化剂的缺陷诱导电子再分布效应,用于电催化氢进化反应(HER)。优化后的催化剂具有 Pt-N3S1 SAs 和 Pt NCs 双活性位点,表现出优异的氢进化反应活性,在电流密度为 400 mA cm-2 时过电位为 192 mV,在过电位为 150 mV 时翻转频率为 30.1 s-1,质量活性为 13716 mA mgPt-1,是 20% Pt/C 催化剂的 7.4 倍。原位拉曼显示催化剂的缺陷结构与反应过程中的氢吸附直接相关。密度泛函理论计算表明,Pt-N3S1 SAs 和 Pt NCs 之间存在缺陷诱导的电子再分布。电子从 Pt NCs 转移到 Pt SAs,从而增加了 Pt SAs 表面的电子数,增强了对 H+ 的吸附能力。同时,H* 在铂 NCs 上的解离能力也得到了提高,从而协同促进了 HER 过程。
Defect-Induced Electron Redistribution between Pt-N3S1 Single Atomic Sites and Pt Clusters for Synergistic Electrocatalytic Hydrogen Production with Ultra-High Mass Activity
A N, S co-doped carbon with abundant vacancy defects (NSC) anchored Pt single atoms (SAs) and nanoclusters (NCs) derived from coal pitch by a self-assembly-pyrolysis strategy is reported and a defect-induced electron redistribution effect based on Pt SAs-Pt NCs/NSC catalyst is proposed for electrocatalytic hydrogen evolution reaction (HER). The optimized catalyst featuring Pt-N3S1 SAs and Pt NCs dual active sites exhibit excellent HER activity with an overpotential of 192 mV at a current density of 400 mA cm−2, a turnover frequency of 30.1 s−1 at an overpotential of 150 mV, which the mass activity is 13716 mA mgPt−1, 7.4 times higher than that of 20% Pt/C catalyst. In situ Raman revealsa direct correlation between the defect structure of the catalyst and hydrogen adsorption during the reaction process. Density functional theory calculation shows the defect-induced electron redistribution between Pt-N3S1 SAs and Pt NCs. The electrons are transferred from Pt NCs to Pt SAs, which increases the number of electrons on the surface of Pt SAs and enhances the adsorption ability of H+. Meanwhile, the dissociation ability of H* on the Pt NCs is promoted, thus synergistically promoting the HER process.
期刊介绍:
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