Enhanced Dissociation Activation of CO2 on the Bi/Cu(111) interface by the synergistic effect
Enhanced Dissociation Activation of CO2 on the Bi/Cu(111) interface by the synergistic effect
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协同效应增强Bi/Cu(111)界面上CO2的解离活化
DOI：
10.1016/j.jcat.2022.04.001
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发表时间：
2022-04
影响因子：
7.3
通讯作者：
Fei Song
中科院分区：
文献类型：
--
作者：
Huan Zhang;Zhaofeng Liang;Chaoqin Huang;Lei Xie;Hongbing Wang;Jinping Hu;Zheng Jiang;Fei Song
热催化CO2还原反应（CO2 RR）是一种很有前途的CO2减排技术。同时，了解CO2在催化剂表面的还原机理，对于推进催化剂设计和最终实现温和条件下的工业化具有重要意义。本文采用近常压X射线光电子能谱（NAP-XPS）、常压扫描隧道显微镜（NAP-STM）和密度泛函理论（DFT）等方法，详细研究了铋/铜界面对CO2 RR的催化作用.结果表明，Bi在Cu上的初始沉积导致了Bi-Cu异质结构的形成，而在较厚的覆盖层处界面被掩埋。在CO2暴露后，由于CO2对Cu位点的活化和随后的氧向Bi的迁移，Bi在界面处被氧化，而Cu+随后在退火中被诱导作为进一步的解离位点。与纯Cu（111）相比，Bi/Cu界面上包括晶格氧和缺陷氧的氧化分数显著更高，表明Bi-Cu界面在CO2活化中的协同效应。因此，我们的工作清楚地揭示了Bi-Cu异质结构的解离位点的演变，并可能促进用于提高热催化CO2 RR的Cu基催化剂的设计。
Thermocatalytic CO2reduction reaction (CO2RR) is one of the promising strategies to mitigate CO2emissions. Meanwhile, understanding the reduction mechanism of CO2on the catalyst surface is imperative for advancing catalyst design and the eventual industrialization under mild conditions. In this work, the catalytic role of bismuth/copper interface towards CO2RR is elaborately investigated via a combination of near ambient-pressure X-ray photoelectron spectroscopy (NAP-XPS), ambient-pressure scanning tunneling microscopy (NAP-STM) and density function theory (DFT). It is demonstrated that the initial deposition of Bi on Cu results in the formation of Bi-Cu heterogenous structure, while the interface is buried at the thick coverage. Upon CO2exposure, Bi is oxidized at interface due to the activation of CO2on Cu sites and subsequent migration of oxygen to Bi, while Cu+is induced afterwards in annealing acting as the further dissociation site. Compared with the pure Cu(1 1 1), the fraction of oxidation including both lattice and defective oxygen is significantly higher on the Bi/Cu interface, indicating the synergistic effect of Bi-Cu interface in the activation of CO2. Thus, our work clearly reveals the dissociation site evolution of the Bi-Cu bimetallic heterostructure and might promote the design of Cu-based catalysts for advancing thermocatalytic CO2RR.
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