Autor: |
Liu, Haibing, Qiu, Yanbin, Gan, Wenxiu, Zhuang, Guoxin, Chen, Fei-Fei, Yang, Chengkai, Yu, Yan |
Zdroj: |
Science China Materials; 20240101, Issue: Preprints p1-10, 10p |
Abstrakt: |
Regulating charge transfer and reaction pathways are effective strategies for boosting photocatalytic CO2reduction. Herein, Co3O4/ZrO2mesoporous octahedrons are synthesized through facile pyrolysis of UIO-66@ZIF-67 core/shell octahedrons. The as-obtained Co3O4/ZrO2mesoporous octahedrons are assembled by highly dispersive and small-sized nanoparticles, with 13 nm average particle size and 5.8 nm pore width, leading to a high specific surface area of 43.11 m2g−1. Benefiting from active-site engineering, the charge-transfer kinetics and CO2adsorption are successfully enhanced. In addition, density functional theory calculations reveal that ZrO2tailors the reaction pathway of CO2reduction by promoting CO2activation to *CO2and intermediate formation (*COOH and *CO), as well as decreasing the energy barrier of the rate-limiting step (*CO→CO). Thus, the Co3O4/ZrO2mesoporous octahedrons afford a turnover frequency of 28.82 h−1, 16.95-fold larger than pure Co3O4. |
Databáze: |
Supplemental Index |
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