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Intermediate stabilization for tuning photocatalytic selective oxidation of CH4 to CH3OH over Co3O4/ZnO
Journal of Catalysis ( IF 7.3 ) Pub Date : 2022-06-11 , DOI: 10.1016/j.jcat.2022.06.017
Zhen Xiao , Jinni Shen , Jiangjie Zhang , Dongmiao Li , Yi Li , Xuxu Wang , Zizhong Zhang

Artificial photocatalysis provides a promising approach for CH4 selective conversion into CH3OH under mild reaction conditions. However, the over-oxidization by the active oxygen radical species impedes for the high efficiency of photocatalytic conversion of CH4 to CH3OH. Here, we proposed a strategy of the transfer of key intermediates •CH3 from host photocatalyst surface for stability to improve CH4 conversion to CH3OH products. A Co3O4/ZnO composited photocatalyst was designed to efficiently convert CH4 to CH3OH with a rate of 366 μmol g-1h−1 under simulated sunlight irradiation, while the parent ZnO only completely overoxidized CH4 into CO2. We uncovered that Co3O4 played a new role as the active site for the adsorption of •CH3 key intermediates and the desorption of CH3OH to suppress CH4 overoxidation on ZnO surface. This work highlights cocatalyst for •CH3 intermediate stabilization to control the pathway of photocatalytic selective oxidation of CH4 into CH3OH.



中文翻译:

在 Co3O4/ZnO 上调节 CH4 光催化选择性氧化为 CH3OH 的中间稳定剂

人工光催化为在温和反应条件下将 CH 4选择性转化为 CH 3 OH提供了一种有前景的方法。然而,活性氧自由基物种的过氧化阻碍了CH 4至CH 3 OH的高效光催化转化。在这里,我们提出了一种将关键中间体•CH 3从主体光催化剂表面转移以提高稳定性以提高CH 4转化为CH 3 OH 产物的策略。设计了一种Co 3 O 4 /ZnO复合光催化剂,以366 μmol g -1的速率有效地将CH 4转化为CH 3 OHh -1在模拟太阳光照射下,而母体ZnO仅将CH 4完全过氧化成CO 2。我们发现Co 3 O 4作为吸附•CH 3关键中间体和解吸CH 3 OH的活性位点发挥了新的作用,以抑制ZnO 表面上的CH 4过氧化。这项工作重点介绍了用于 •CH 3中间体稳定化的助催化剂,以控制 CH 4光催化选择性氧化成 CH 3 OH 的途径。

更新日期:2022-06-16
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