Gan Guoqiang, Xu Fengquan, Li Xinyong, Fan Shiying, Bai Chunpeng, Zhao Qidong, Tadé Moses O, Liu Shaomin, Zhang Wenjun
State Key Laboratory of Fine Chemicals, Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, China.
Center of Super-Diamond and Advanced Films (COSDAF), Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon 999077, Hong Kong, China.
ACS Appl Mater Interfaces. 2023 Feb 8;15(5):6631-6638. doi: 10.1021/acsami.2c17561. Epub 2023 Jan 27.
CuFeO spinel has been considered as a promising catalyst for the electrochemical reaction, while the nature of the crystal phase on its intrinsic activity and the kind of active site need to be further explored. Herein, the crystal phase-dependent catalytic behavior and the main active sites of CuFeO spinel for electrochemical dechlorination of 1,2-dichloroethane are carefully studied based on the combination of experiments and theoretical calculations. Cubic and tetragonal CuFeO are successfully prepared by a facile sol-gel method combined with high temperature calcination. Impressively, CuFeO with the cubic phase shows a higher activity and ethylene selectivity compared to CuFeO with the tetragonal phase, suggesting a significant facilitation of electrocatalytic performance by the cubic crystal structure. Moreover, the octahedral Fe atom on the surface of cubic CuFeO(311) is the active site responsible to produce ethylene with the energy barrier of 0.40 eV. This work demonstrates the significance of crystal phase engineering for the optimization of electrocatalytic performance and offers an efficient strategy for the development of advanced electrocatalysts.
铜铁氧体尖晶石被认为是一种有前景的电化学反应催化剂，但其晶相本质对其本征活性的影响以及活性位点的种类仍需进一步探索。在此，基于实验和理论计算相结合的方法，对铜铁氧体尖晶石用于1,2 - 二氯乙烷电化学脱氯的晶相依赖性催化行为及主要活性位点进行了细致研究。通过简便的溶胶 - 凝胶法结合高温煅烧成功制备了立方相和四方相的铜铁氧体。令人印象深刻的是，与四方相铜铁氧体相比，立方相铜铁氧体表现出更高的活性和乙烯选择性，表明立方晶体结构对电催化性能有显著促进作用。此外，立方相CuFeO(311)表面的八面体铁原子是产生乙烯的活性位点，其能垒为0.40 eV。这项工作证明了晶相工程对优化电催化性能的重要性，并为开发先进电催化剂提供了一种有效策略。
