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Liquid Fluxional Ga Single Atom Catalysts for Efficient Electrochemical CO2 Reduction |
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| Authors: | Dr Zedong Zhang Jiexin Zhu Dr Shenghua Chen Prof Wenming Sun Prof Dingsheng Wang |
| Institution: | 1. Department of Chemistry, Tsinghua University, Beijing, 100084 China
These authors contributed equally to this work.;2. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070 Hubei, China These authors contributed equally to this work.;3. Department of Chemistry, Tsinghua University, Beijing, 100084 China;4. Department of Chemistry, Beijing Key Laboratory for Optical Materials and Photonic Devices, Capital Normal University, Beijing, 100048 China |
| Abstract: | Precise design and tuning of the micro-atomic structure of single atom catalysts (SACs) can help efficiently adapt complex catalytic systems. Herein, we inventively found that when the active center of the main group element gallium (Ga) is downsized to the atomic level, whose characteristic has significant differences from conventional bulk and rigid Ga catalysts. The Ga SACs with a P, S atomic coordination environment display specific flow properties, showing CO products with FE of ≈92 % at ?0.3 V vs. RHE in electrochemical CO2 reduction (CO2RR). Theoretical simulations demonstrate that the adaptive dynamic transition of Ga optimizes the adsorption energy of the *COOH intermediate and renews the active sites in time, leading to excellent CO2RR selectivity and stability. This liquid single atom catalysts system with dynamic interfaces lays the foundation for future exploration of synthesis and catalysis. |
| Keywords: | CO2RR Fluxional Single Atom Catalysts Liquid Metal Ga |