Non-Interacting Ni and Fe Dual-Atom Pair Sites in N-Doped Carbon Catalysts for Efficient Concentrating Solar-Driven Photothermal CO2 Reduction

作者：Mo, Shengpeng; Zhao, Xinya; Li, Shuangde; Huang, Lili; Zhao, Xin; Ren, Quanming; Zhang, Mingyuan; Peng, Ruosi; Zhang, Yanan; Zhou, Xiaobin; Fan, Yinming; Xie, Qinglin^*; Guo, Yanbing^*; Ye, Daiqi^*; Chen, Yunfa

来源：Angewandte Chemie - International Edition, 2023, 62(50).

DOI：10.1002/anie.202313868

• CO2 Reduction
• Dual-Single-Atom Catalyst
• Electronic Interaction
• Reaction Mechanism
• Solar

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-N-4 and Fe-N-4 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 mu mol g(-1) h(-1)), CH4 (135.35 mu mol g(-1) h(-1)) and CH3OH (59.81 mu mol 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.

• 单位
  桂林理工大学; 东莞理工学院; 中国科学院