光催化
催化作用
醋酸
化学吸附
水溶液
选择性
二氧化碳
产量(工程)
溶解度
甲烷
材料科学
无机化学
光化学
化学
化学工程
有机化学
冶金
工程类
作者
Ning Liu,Na Lu,Kun Zhao,Pengxiao Liu,ZhuMei Sun,Jing Lü
标识
DOI:10.1016/j.cej.2024.150690
摘要
The conversion of methane (CH4) and carbon dioxide (CO2) into high-value products under mild conditions is crucial for addressing the greenhouse effect and advancing C1 chemistry. In this study, Cu/ZnO catalysts were prepared through a one-step wet reduction process, and the catalytic conversion of CH4 and CO2 into acetic acid molecules (CH3COOH) was achieved via photon activation at ambient temperature. The yield of acetic acid was 411.6 μmol/Lgcat−1h−1 with a selectivity of 89.5 % under optimal conditions (100 mWcm−2 light intensity, 25 ± 2 °C, 2 MPa pressure, and a 1:1 CH4:CO2 volume ratio). Enhanced solubility of CH4 in aqueous under increased pressure and temperature was observed to improve acetic acid production. Additionally, the catalytic mechanism involved surface chemisorption of CH4 and CO2, facilitated by ZnO and Cu in the catalyst, leading to C-C coupling and subsequent acetic acid formation, driven by photogenerated electron-hole migration. This study provides a foundational understanding for the synthesis of value-added chemicals through CH4 and CO2 conversion via C-C coupling in mild environments.
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