Precisely designed cobalt single atom on ZrO ₂ support for chemical CO ₂ fixation Neha Choudhary 1 , Shan Jiang 2 , Hien Pham 3 , Abhaya Datye 3 , Jeffrey T. Miller 2 , Shaikh M. Mobin 1,4 1 Department of Chemistry, Indian Institute of Technology-Indore, Simrol, India, 2 Davidson School of Chemical Engineering, Purdue University, West Lafayette, United States, 3 Department of Chemical Biological Engineering and Center for Micro engineered Materials, University of New Mexico, United States, 4 Center for Electric Vehicle and Intelligent Transport Systems, Indian Institute of Technology-Indore, Simrol, India The presence of single atoms as active sites on a metal oxide support can dramatically enhance catalytic activity. Here, we demonstrate that Cobalt doped ZrO 2 constitutes a single atom catalyst where each Co +2 ion is active for CO 2 fixation. The synthesized Co/ZrO 2 catalyst was characterized by EXAFS and STEM to confirm the presence of isolated Co +2 on the ZrO 2 support. The STEM-EDS data showed uniform distribution of Co over the surface of the ZrO 2 support. The catalytic results reveal that Co active sites on ZrO 2 enhance catalytic performance and provide 100% conversion into carbonate products in the presence of trace amounts of tetrabutylammonium bromide (TBAB). When undoped ZrO 2 and Co 3 O 4 impregnated ZrO 2 catalyst was utilized for comparison, less than 50% conversion of epoxides was obtained. The single atom catalyst (SAC) showed a broad substrate scope, solvent-free reaction and higher catalytic activity and selectivity. References 1. A. Wang, J. Li, T. Zhang, Heterogeneous single-atom catalysis, Nat Rev Chem. 2 (2018) 65–81. https://doi.org/10.1038/ s41570-018-0010-1. 2. N.H.M. Dostagir, R. Rattanawan, M. Gao, J. Ota, J. Hasegawa, K. Asakura, A. Fukouka, A. Shrotri, Co Single Atoms in ZrO2 with Inherent Oxygen Vacancies for Selective Hydrogenation of CO2 to CO, ACS Catal. 11 (2021) 9450–9461. https://doi. org/10.1021/acscatal.1c02041. 3. Q. Yang, C.-C. Yang, C.-H. Lin, H.-L. Jiang, Metal–Organic-Framework-Derived Hollow N-Doped Porous Carbon with Ultrahigh Concentrations of Single Zn Atoms for Efficient Carbon Dioxide Conversion, Angewandte Chemie International Edition. 58 (2019) 3511–3515. https://doi.org/10.1002/anie.201813494. 4. Xu et al, Strong Electronic Metal–Support Interaction between Iridium Single Atoms and a WO3 Support Promotes Highly Efficient and Robust CO2 Cycloaddition, Advanced Materials. 34 (2022) 2206991. https://doi.org/10.1002/adma.202206991.
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