甲烷
催化作用
光热治疗
辐照
光热效应
光化学
解吸
X射线光电子能谱
电子转移
密度泛函理论
化学
化学工程
材料科学
纳米技术
物理化学
吸附
计算化学
物理
有机化学
核物理学
生物化学
工程类
作者
Zhiqiang Rao,Yuehan Cao,Zeai Huang,Zihang Yin,Wenchao Wan,Minzhi Ma,Yanxin Wu,Junbu Wang,Guidong Yang,Yi Cui,Zhongmiao Gong,Ying Zhou
标识
DOI:10.1021/acscatal.0c04826
摘要
Photothermal catalysis, which couples both solar and thermal energies, has burgeoned as a promising approach to drive catalytic reactions. However, the utilization of light irradiation to tune the reaction paths to obtain ideal product distribution in photothermal catalysis is still of tremendous challenge. Herein, we successfully regulated the relationship between two core competition reactions through light irradiation during photothermal dry reforming of methane over Ni/Ga2O3, resulting in the promotion of H2 formation and the suppression of the reverse water gas shift reaction. The increase in the H2/CO ratio from 0.55 to 0.94 could be achieved. Furthermore, the combination of density functional calculations and X-ray photoelectron spectroscopy reveals that light irradiation impelled the direction of electron transfer to be reversed from Ga2O3 to Ni to form the Ni0 sites, which provides the generation of abundant hot electrons from the electronic interband transition of Ni to boost the formation and desorption of H2. This work promotes the understanding of nonthermal behaviors of light irradiation in light-driven photochemistry, which is significant for designing catalysts with high efficiency and controllable product distribution.
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