1. Key Laboratory for Green Chemical Technology of Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China 2. School of Materials Science and Engineering, National Institute for Advanced Materials, TKL of Metal and Molecule-Based Material Chemistry, Nankai University, Tianjin 300350, China 3. Zhejiang Institute of Tianjin University, Ningbo 315201, China 4. Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, China
The Fe-Mn bimetallic catalyst is a potential candidate for the conversion of CO2 into value-added chemicals. The interaction between the two metals plays a significant role in determining the catalytic performance, however which remains controversial. In this study, we aim to investigate the impact of tuning the proximity of Fe-Mn bimetallic catalysts with similar nanoparticle size. And its effect on the physicochemical properties of the catalysts and corresponding performance were investigated. It was found that closer Fe-Mn proximity resulted in enhanced CO2 hydrogenation activity and inhibited CH4 formation. The physiochemical properties of prepared catalysts were characterized using X-ray diffraction, H2 temperature programmed reduction, and X-ray photoelectron spectroscopy, revealing that a closer Fe-Mn distance promoted electron transfer from Mn to Fe, thereby facilitating Fe carburization. The adsorption behavior of CO2 and the identification of reaction intermediates were analyzed using CO2-temperature programed desorption and in situ Fourier transform infrared spectroscopy, confirming the intimate Fe-Mn sites contributed to CO2 adsorption and the formation of HCOO* species, ultimately leading to increased CO2 conversion and hydrocarbon production. The discovery of a synergistic effect at the intimate Fe-Mn sites in this study provides valuable insights into the relationship between active sites and promoters.
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