Environmentally benign methane-regulated catalytic desulfurization

He, Peng ¹Li, Zhaofei ²Meng, Shijun ²Li, Yimeng ²Chang, Lo-Yueh ³Liu, Lijia ⁴Wen, Xiaodong ¹Klein, Brittney A. ⁵Michaelis, Vladimir K. ⁵Qi, Jizhen ⁶Wu, Dongchang ⁷Liu, Xi ⁸Song, Hua ²Xu, Hao²

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作者信息

1. Synfuels China Technol Co Ltd
2. Univ Calgary
3. Natl Synchrotron Radiat Res Ctr
4. Western Univ
5. Univ Alberta
6. Chinese Acad Sci
7. Shanghai Nanoport
8. Shanghai Jiao Tong Univ
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Abstract

Hydrodesulfurization is well established in the industry while costly and environmentally unfriendly due to CO2 emissions and H2S production. An alternative, cost-effective desulfurization process remains unreported. Here, we demonstrate a desulfurization process for dibenzothiophene, one of the most well-known and recalcitrant sulfur-containing model compounds against catalytic desulfurization, under the regulation of methane instead of hydrogen over a combination of two catalysts, generating a new sulfur-containing product, CS2, as an important intermediate in organic chemistry and non-polar solvent with lower environmental impact than H2S. A catalytic mechanism is proposed and supported by extensive experimental and computational evidence. It is discovered that methane acts as a critical initiator and intensifies the direct desulfurization pathway, where two catalysts must work cooperatively and a surface sulfur transfer process is indispensable. This study explores an alternative desulfurization route with unique reaction pathways towards CS2 formation, whose practical potential is also supported by the desulfurization performance over a series of real-world crude samples.

Key words

Desulfurization/Methane/Supported catalysts/Green chemistry/Carbon disulfide/CO-AROMATIZATION/MODEL-COMPOUND/CARBON-DISULFIDE/DIBENZOTHIOPHENE/HYDRODESULFURIZATION/SPECTROSCOPY/ACTIVATION/EMISSIONS/BENZENE/PROPANE

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出版年

2022

Applied Catalysis

ISSN：0926-3373

被引量8

参考文献量52

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