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Highly selective aerobic oxidation of methane to methanol over gold decorated zinc oxide via photocatalysis
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2020-06-05 , DOI: 10.1039/d0ta02793f
Wencai Zhou 1, 2, 3, 4, 5 , Xueying Qiu 1, 2, 3, 4, 5 , Yuheng Jiang 1, 2, 3, 4, 5 , Yingying Fan 1, 2, 3, 4, 5 , Shilei Wei 6, 7, 8, 9, 10 , Dongxue Han 6, 7, 8, 9, 10 , Li Niu 6, 7, 8, 9, 10 , Zhiyong Tang 1, 2, 3, 4, 5
Affiliation  

Photodriven CH4 conversion has been regarded as a promising green strategy for fabrication of value-added commodity chemicals, in particular methanol. However, due to the incomplete transformation of intermediates or the overoxidation of products, a good selectivity of methanol is hard to achieve. Here, we present a highly selective transformation of methane to methanol using gold modified zinc oxide as a photocatalyst under full light spectrum irradiation at atmospheric temperature. The selectivity of methanol can reach 99.1% with a productivity of 1371 μmol g−1. Fine tuning the loading amount of gold nanoparticles (0.75 wt%) and inputting an appropriate light energy are the pivotal factors for selectivity improvement. Besides, in contrast to the reported photocatalytic aerobic CH4 oxidation on gold modified zinc oxide, we find that both oxygen and water, rather than only molecular oxygen, provide the O-source for methanol formation. This result is verified through 18O-isotope tests (18O2 and H218O), leading to a disparate mechanism.

中文翻译:

在金装饰的氧化锌上通过光催化将甲烷选择性地好氧氧化为甲醇

光驱动的CH 4转化被认为是制造增值商品化学品(特别是甲醇)的有前途的绿色战略。然而,由于中间体的不完全转化或产物的过度氧化,难以实现良好的甲醇选择性。在这里,我们介绍了在大气温度下全光谱照射下,使用金改性的氧化锌作为光催化剂,将甲烷高度选择性地转化为甲醇的过程。甲醇的选择性可以达到99.1%,产率为1371μmolg -1。微调金纳米颗粒的负载量(0.75重量%)并输入适当的光能是提高选择性的关键因素。此外,与报道的光催化好氧CH相反在金修饰的氧化锌上进行4氧化时,我们发现氧气和水(而不是仅分子氧)都为形成甲醇提供了O源。通过18个O同位素测试( 18 O 2和H 2 18 O)验证了该结果,从而得出了不同的机理。
更新日期:2020-07-07
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