过电位
塔菲尔方程
X射线吸收光谱法
催化作用
材料科学
拉曼光谱
钼
过渡金属
吸收光谱法
扩展X射线吸收精细结构
化学工程
结晶学
物理化学
化学
电化学
生物化学
物理
电极
量子力学
光学
冶金
工程类
作者
Peng Wu,Yu Yang,Xiang Hong,Yang Si,Yong Heng Chu,Xiao Zhi Su,Wen Yan,Ting You,Yu Gao,Yu Wang,Wen Xing Chen,Yuying Huang,Penggang Yin
出处
期刊:Small
[Wiley]
日期:2023-10-20
被引量:2
标识
DOI:10.1002/smll.202306716
摘要
Abstract The interaction between catalyst and support plays an important role in electrocatalytic hydrogen evolution (HER), which may explain the improvement in performance by phase transition or structural remodeling. However, the intrinsic behavior of these catalysts (dynamic evolution of the interface under bias, structural/morphological transformation, stability) has not been clearly monitored, while the operando technology does well in capturing the dynamic changes in the reaction process in real time to determine the actual active site. In this paper, nitrogen‐doped molybdenum atom‐clusters on Ti 3 C 2 T X (Mo ACs /N‐Ti 3 C 2 T X ) is used as a model catalyst to reveal the dynamic evolution of Mo Acs on Ti 3 C 2 T X during the HER process. Operando X‐ray absorption structure (XAS) theoretical calculation and in situ Raman spectroscopy showed that the Mo cluster structure evolves to a 6‐coordinated monatomic Mo structure under working conditions, exposing more active sites and thus improving the catalytic performance. It shows excellent HER performance comparable to that of commercial Pt/C, including an overpotential of 60 mV at 10 mA cm −2 , a small Tafel slope (56 mV dec −1 ), and high activity and durability. This study provides a unique perspective for investigating the evolution of species, interfacial migration mechanisms, and sources of activity‐enhancing compounds in the process of electroreduction.
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