文献类型：期刊文献

英文题名：Engineering the grain boundary and surface sites of binary Cu-Mn catalysts to boost CO oxidation

作者：Zhang, Xiangxue[1];Chao, Xinyi[1];Fei, Nina[1];Chen, Wenyao[1];Qian, Gang[1];Zhang, Jing[1];Chen, De[2];Duan, Xuezhi[1];Zhou, Xinggui[1];Yuan, Weikang[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, NO-7491 Trondheim, Norway

年份：2024

卷号：9

期号：10

起止页码：2659

外文期刊名：REACTION CHEMISTRY & ENGINEERING

收录：;EI(收录号：20243116781413);WOS:【SCI-EXPANDED(收录号:WOS:001275625900001)】；

基金：This work was financially supported by the National Key R&D Program of China (2022YFA1503503 and 2022YFA1503504), the Natural Science Foundation of China (22038003, 22178100, 22178101, U22B20141 and 22008066), the Shanghai Pilot Program for Basic Research (22TQ1400100-15), the Fundamental Research Funds for the Central Universities, the Innovation Program of Shanghai Municipal Education Commission, the Program of Shanghai Academic/Technology Research Leader (21XD1421000), and the Shanghai Science and Technology Innovation Action Plan (22JC1403800). We thank the staff at the BL14W1 XAFS beamline of Shanghai Synchrotron Radiation Facility (SSRF) for the beam time and assistance in the experiments.

语种：英文

外文关键词：Binary alloys - Catalyst activity - Catalytic oxidation - Copper - Economic and social effects - Grain boundaries - Lattice mismatch - Manganese oxide - Nanorods

摘要：The catalytic oxidation of CO over Cu-based catalysts has garnered significant interest due to their promising potential in addressing environmental pollution and enhancing industrial processes. Herein, we report a dual-stimuli strategy to boost the catalytic performance of CO oxidation via synergistically harnessing active Cu+ species with oxygen vacancies by engineering the grain boundary of Cu-Mn catalysts. Nanorod-like MnO2 with a tunnel structure was prepared by a hydrothermal method and employed as the catalyst support, where different amounts of Cu were further introduced via impregnation to obtain Cu/MnO2 catalysts. It is found that apart from the highly dispersed Cu species within the MnO2 lattice to create lattice mismatch and distortion, some Cu are present as oxidized nanoparticles over the MnO2 surface, thus sparking off increased dislocations and grain boundaries. A combination of characterization methods demonstrates that the proportion of active Cu+ species decreases with increasing amount of Cu, presenting an inverse relationship to the abundance of oxygen vacancies over the catalyst surface. Correspondingly, both Cu+ species and oxygen vacancies are identified as the main active sites for the adsorption and activation of CO and O2, respectively. Therefore, a trade-off between the percentage of active Cu+ species and oxygen vacancies for the 15% Cu/MnO2 catalyst with a moderate Cu introduction contributes to its highest catalytic activity, with T50 and T90 reaching 66 degrees C and 89 degrees C, respectively. This investigation highlights the potential of synergistically harnessing active Cu+ species with oxygen vacancies via grain boundary engineering for enhanced catalytic performance in CO oxidation applications. A dual-stimuli strategy is proposed to boost the catalytic performance of CO oxidation via synergistically harnessing active Cu+ species with oxygen vacancies by engineering the grain boundary of Cu-Mn catalysts.