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Non-Interacting Ni and Fe Dual-Atom Pair Sites in N-Doped Carbon Catalysts for Efficient Concentrating Solar-Driven Photothermal CO2 Reduction |
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| Authors: | Shengpeng Mo Xinya Zhao Shuangde Li Lili Huang Xin Zhao Quanming Ren Mingyuan Zhang Ruosi Peng Yanan Zhang Xiaobin Zhou Yinming Fan Prof. Qinglin Xie Prof. Yanbing Guo Prof. Daiqi Ye Prof. Yunfa Chen |
| Affiliation: | 1. College of Environment Science and Engineering, Guilin University of Technology, Guilin, 541004 P. R. China These authors contributed equally to this work.;2. Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China These authors contributed equally to this work.;3. State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190 P. R. China These authors contributed equally to this work.;4. College of Environment Science and Engineering, Guilin University of Technology, Guilin, 541004 P. R. China;5. School of Environment and Energy, South China University of Technology, Guangzhou, 510006 P. R. China;6. College of Geology and Environment, Xi'an University of Science and Technology, Xi'an, 710054 P. R. China;7. School of Environment and Civil Engineering, Dongguan University of Technology, Dongguan, 523808 P. R. China;8. Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental and Applied Chemistry, College of Chemistry, Central China Normal University, Wuhan, 430079 P. R. China;9. State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing, 100190 P. R. China |
| Abstract: | Solar-to-chemical energy conversion under weak solar irradiation is generally difficult to meet the heat demand of CO2 reduction. Herein, a new concentrated solar-driven photothermal system coupling a dual-metal single-atom catalyst (DSAC) with adjacent Ni−N4 and Fe−N4 pair sites is designed for boosting gas-solid CO2 reduction with H2O under simulated solar irradiation, even under ambient sunlight. As expected, the (Ni, Fe)−N−C DSAC exhibits a superior photothermal catalytic performance for CO2 reduction to CO (86.16 μmol g−1 h−1), CH4 (135.35 μmol g−1 h−1) and CH3OH (59.81 μmol g−1 h−1), which are equivalent to 1.70-fold, 1.27-fold and 1.23-fold higher than those of the Fe−N−C catalyst, respectively. Based on theoretical simulations, the Fermi level and d-band center of Fe atom is efficiently regulated in non-interacting Ni and Fe dual-atom pair sites with electronic interaction through electron orbital hybridization on (Ni, Fe)−N−C DSAC. Crucially, the distance between adjacent Ni and Fe atoms of the Ni−N−N−Fe configuration means that the additional Ni atom as a new active site contributes to the main *COOH and *HCO3 dissociation to optimize the corresponding energy barriers in the reaction process, leading to specific dual reaction pathways (COOH and HCO3 pathways) for solar-driven photothermal CO2 reduction to initial CO production. |
| Keywords: | CO2 Reduction Dual-Single-Atom Catalyst Electronic Interaction Reaction Mechanism Solar |