Isolated Ni Atoms Enable Near-Unity CH 4 Selectivity for Photothermal CO 2 Hydrogenation

作者：Fazal Raziq, Chengyang Feng, H. Miao, Shouwei Zuo, Mohammad Ziaur Rahman, Yayu Yan, Qiaohong Li, Jorge Gascón, Huabin Zhang · 发表于：Journal of the American Chemical Society · 年份：2024 · DOI：10.1021/jacs.4c05873 · 被引用次数：163 · 研究领域：CO2 Reduction Techniques and Catalysts、Advanced Photocatalysis Techniques、Carbon dioxide utilization in catalysis

Photothermal hydrogenation of carbon dioxide (CO 2 ) into value-added products is an ideal solution for addressing the energy crisis and mitigating CO 2 emissions. However, achieving high product selectivity remains challenging due to the simultaneous occurrence of numerous competing intermediate reactions during CO 2 hydrogenation. We present a novel approach featuring isolated single-atom nickel (Ni) anchored onto indium oxide (In 2 O 3 ) nanocrystals, serving as an effective photothermal catalyst for CO 2 hydrogenation into methane (CH 4 ) with a remarkable near-unity (∼99%) selectivity. Experiments and theoretical simulations have confirmed that isolated Ni sites on the In 2 O 3 surface can effectively stabilize the intermediate products of the CO 2 hydrogenation reaction and reduce the transition state energy barrier, thereby changing the reaction path to achieve ultrahigh selective methanation. This study provides comprehensive insights into the design of single-atom catalysts for the highly selective photothermal catalytic hydrogenation of CO 2 to methane.