期刊
ACS CATALYSIS
卷 12, 期 15, 页码 9515-9525出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02424
关键词
photocatalysis; methane; methane oxidation; oxygenates; titanium dioxide
资金
- National Key R&D Program of China [2021YFF0500702, 2021YFF0500703]
- Natural Science Foundation of China [91945301]
- Program of Shanghai Academic/Technology Research Leader [20XD1404000]
- Transformational Technologies for Clean Energy and Demonstration
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA21020600]
- Youth Innovation Promotion Association of CAS
In this study, a novel Cu and W codoped TiO2 photocatalyst was fabricated to achieve selective photooxidation of methane into oxygenates at ambient temperature, with limited formation of CO2. The Cu-W-TiO2 photocatalyst exhibited high productivity and selectivity, and its improved performance was attributed to the modulation of electronic and band structure, which facilitated methane activation and hindered overoxidation of oxygenates.
Direct selective methane photooxidation to liquid oxygenates with high productivity and selectivity under mild reaction conditions is highly urgent but remains challenging. Herein, a Cu and W codoped TiO2 (Cu-W-TiO2) photocatalyst was fabricated to enable aerobic oxidation of methane into oxygenates with limited formation of CO(2 )under ambient temperature. A high oxygenate productivity of 34.5 mmol g(-1) with a remarkable selectivity of 97.1% was achieved over the Cu-W- TiO2 photocatalyst. Based on structural characterizations and mechanism studies, it was suggested that the Cu species acted as hole traps, while oxygen vacancies and the W6+-dopant state worked as electron traps. The inhibited recombination of photogenerated carriers contributed to enhanced photocatalytic efficiency. The modulated electronic and band structure promoted the activation of methane and hindered the overoxidation of oxygenates.
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