Operando Spectroscopy Observation of Mo Clusters-Ti3 C2 TX Catalyst/Support Interface's Dynamic Evolution in Hydrogen Evolution Reaction.
Operando Spectroscopy Observation of Mo Clusters-Ti3 C2 TX Catalyst/Support Interface's Dynamic Evolution in Hydrogen Evolution Reaction.
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DOI：
10.1002/smll.202306716
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发表时间：
2023-10
期刊：
影响因子：
13.3
通讯作者：
Peng Fei Wu;Yu Qi Yang;Hong Yan Xi;Yang Si;Yong Heng Chu;X. Su;Wensheng Yan;Ting Ting You-Ting;Y. Gao;Yu Wang;Wen Xing Chen;Yu Ying Huang;P. Yin
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文献类型：
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作者：
Peng Fei Wu;Yu Qi Yang;Hong Yan Xi;Yang Si;Yong Heng Chu;X. Su;Wensheng Yan;Ting Ting You-Ting;Y. Gao;Yu Wang;Wen Xing Chen;Yu Ying Huang;P. Yin
催化剂和载体之间的相互作用在电催化析氢过程中起着重要作用，这可能是通过相变或结构重塑来解释性能改善的原因。然而，这些催化剂的内在行为（偏压下界面的动态演变、结构/形态转变、稳定性）尚未被清楚地监测，而操作技术在真实的时间内很好地捕捉反应过程中的动态变化以确定实际的活性位点。本文以Ti_3C_2TX上的氮掺杂钼原子团簇（MoACs /N-Ti_3C_2 TX）为模型催化剂，研究了MoACs在Ti_3C_2TX上的动态演化过程.操作X射线吸收结构（XAS）理论计算和原位拉曼光谱表明，在工作条件下，Mo原子簇结构向6配位的单原子Mo结构演变，暴露出更多的活性中心，从而提高了催化性能。它显示出与商业Pt/C相当的优异HER性能，包括在10 mA cm-2下60 mV的过电位、小的Tafel斜率（56 mV dec-1）以及高活性和耐久性。该研究为研究电还原过程中物种的演化、界面迁移机制和活性增强化合物的来源提供了独特的视角。
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 Ti3 C2 TX (MoACs /N-Ti3 C2 TX ) is used as a model catalyst to reveal the dynamic evolution of MoAcs on Ti3 C2 TX 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.