Journal
CHEMICAL ENGINEERING JOURNAL
Volume 452, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.139505
Keywords
Selective methane oxygenation; Chlorine radicals; Hydrogen peroxide; Photocatalysis
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In this study, a chlorine-mediated pathway was used to selectively partially oxidize methane to methanol under mild conditions via photocatalysis. The results showed that the synergy effect of chlorine radicals and H2O2 achieved high productivity of methanol.
Selective partial oxidation of methane to methanol under mild conditions remains a great challenge in activating the first C-H bond of CH4 and inhibiting overoxidation. Chlorine-mediated pathway arises as a promising strategy to obtain high CH4 conversion under mild conditions. Herein, a considerable CH3OH production rate of 180.75 mu mol center dot gcat- 1 center dot h-1 with 80.07 % selectivity is achieved when the BiOCl with oxygen vacancies is irradiated by visible light in NaCl solution with H2O2 addition. Experimental studies reveal that chlorine radicals are in situ produced and constrained on the surface of the catalyst, which inhibits the over halogenation. Reactive oxygen species produced by H2O2 dissociation were utilized to be the receptors of center dot CH3. The high productivity of methanol was achieved by the synergy effect of chlorine radicals and H2O2. This work provides a new feasible method to convert inert methane into high-value-added products via photocatalysis.
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