塔菲尔方程
过电位
X射线光电子能谱
催化作用
钯
氢溢流
材料科学
价(化学)
纳米颗粒
氧化物
可逆氢电极
电化学
化学工程
化学
纳米技术
物理化学
电极
工作电极
有机化学
冶金
工程类
作者
Zhongmiao Gong,Zhigang Chen,Hao Li,Guang Yang,Min Yuan,Zhi-Yun Li,Xueying Wan,Yi Cui
标识
DOI:10.1016/j.jechem.2023.11.033
摘要
Surface-supported isolated atoms in single-atom catalysts (SACs) grant maximum utilization of metals in heterogeneous catalysis. Herein, we report a feasible pyrolysis strategy to synthesize Pd single atoms by thermally melting Pd nanoparticles on an oxygen-vacancy-rich tungsten-oxide matrix at reduction atmosphere. Near ambient pressure X-ray photoelectron spectroscopy was used to monitor the formation of zero-valence Pd single atoms and the increased metallic feature of WO3−x substrate. Accordingly, the as-obtained zero-valence Pd single-atom catalyst exhibits a markedly boosted HER activity with a low overpotential (η10 = 70 mV) at the current density of 10 mA/cm2 and a small Tafel slope (b = 68 mV/dec), nearly 150 mV and a 3.0-fold enhancement than those of Pd nanoparticles (η10 = 220 mV, b = 133 mV/dec) under the same conditions. In addition, quasi in situ XPS results suggest the hydrogen spillover effect is more likely to occur on Pd single atoms during the electrochemical process. Our work may pave an interesting route for the rational design of highly-efficient single-atom catalyst, and the elucidation of corresponding enhanced reaction mechanisms by the utilization of advanced characterization techniques.
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