过电位
催化作用
纳米片
氢溢流
无定形固体
材料科学
电化学
氢
拉曼光谱
电解质
可逆氢电极
无机化学
结晶学
化学
纳米技术
物理化学
电极
工作电极
有机化学
物理
光学
作者
Yue Liu,Gui Liu,Xiangyu Chen,Chuang Xue,Mingke Sun,Yifei Liu,Jianxin Kang,Xiujuan Sun,Xiaotian Wang
标识
DOI:10.1007/s40820-024-01420-6
摘要
Abstract Single-atom (SA) catalysts with nearly 100% atom utilization have been widely employed in electrolysis for decades, due to the outperforming catalytic activity and selectivity. However, most of the reported SA catalysts are fixed through the strong bonding between the dispersed single metallic atoms with nonmetallic atoms of the substrates, which greatly limits the controllable regulation of electrocatalytic activity of SA catalysts. In this work, Pt–Ni bonded Pt SA catalyst with adjustable electronic states was successfully constructed through a controllable electrochemical reduction on the coordination unsaturated amorphous Ni(OH) 2 nanosheet arrays. Based on the X-ray absorption fine structure analysis and first-principles calculations, Pt SA was bonded with Ni sites of amorphous Ni(OH) 2 , rather than conventional O sites, resulting in negatively charged Pt δ − . In situ Raman spectroscopy revealed that the changed configuration and electronic states greatly enhanced absorbability for activated hydrogen atoms, which were the essential intermediate for alkaline hydrogen evolution reaction. The hydrogen spillover process was revealed from amorphous Ni(OH) 2 that effectively cleave the H–O–H bond of H 2 O and produce H atom to the Pt SA sites, leading to a low overpotential of 48 mV in alkaline electrolyte at −1000 mA cm −2 mg −1 Pt , evidently better than commercial Pt/C catalysts. This work provided new strategy for the controllable modulation of the local structure of SA catalysts and the systematic regulation of the electronic states.
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