无定形固体
氧气
电子转移
化学工程
材料科学
光化学
化学
化学物理
结晶学
有机化学
工程类
作者
Zhongming Wang,Hang Yuan,Siting Chen,Yong Jia,Lina Guo,Hong Wang,Wenxin Dai
标识
DOI:10.1016/j.cej.2024.152394
摘要
The progressive transfer of photogenerated electrons between the catalyst components and reactants is of great significance for photocatalysis. Amorphous Pd (PdA) and oxygen vacancies (VOs) were simultaneously introduced in Pd-In2O3 exploiting hydrogen-induced amorphization effects; 0.6 wt% Pd-In2O3 exhibited a 4.5-fold increase in activity and a 3.2-fold higher selectivity toward CH3OH + CO (63.62 %) compared with In2O3. Multiple in situ techniques and theoretical calculations revealed that intercomponent electron transfer channels were established via various interface structures formed between PdA or crystalline Pd (PdC) and In2O3; PdA acted as electronic pump, facilitating the transfer and separation of photogenerated electrons, resulting in their subsequent enrichment on the surface of PdA. Simultaneously, PdA acted as electron-donating adsorption site for H2O, increasing the number of electrons received by H2O, further inhibiting the competitive adsorption of H2O and CO2 on VO sites, and promoting the hydrogen evolution reaction. Additionally, the electronic coupling between PdC and VOs could significantly decrease the electron-donating ability of VOs, reducing the number of electrons received by CO2, thus effectively regulating the degree of CO2 reduction. This study employs PdA/PdC and VOs to synergistic optimize the progressive transfer of photogenerated electrons, and presents a novel approach for elucidating the catalytic mechanism.
科研通智能强力驱动
Strongly Powered by AbleSci AI