Isolated Ni Atoms Enable Near-Unity CH4Selectivity for Photothermal CO2Hydrogenation

Autor: Raziq, Fazal, Feng, Chengyang, Hu, Miao, Zuo, Shouwei, Rahman, Mohammad Ziaur, Yan, Yayu, Li, Qiao-Hong, Gascon, Jorge, Zhang, Huabin
Zdroj: Journal of the American Chemical Society; July 2024, Vol. 146 Issue: 30 p21008-21016, 9p
Abstrakt: Photothermal hydrogenation of carbon dioxide (CO2) into value-added products is an ideal solution for addressing the energy crisis and mitigating CO2emissions. However, achieving high product selectivity remains challenging due to the simultaneous occurrence of numerous competing intermediate reactions during CO2hydrogenation. We present a novel approach featuring isolated single-atom nickel (Ni) anchored onto indium oxide (In2O3) nanocrystals, serving as an effective photothermal catalyst for CO2hydrogenation into methane (CH4) with a remarkable near-unity (∼99%) selectivity. Experiments and theoretical simulations have confirmed that isolated Ni sites on the In2O3surface can effectively stabilize the intermediate products of the CO2hydrogenation 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 CO2to methane.
Databáze: Supplemental Index