4.8 Article

Boosting Selective Oxidation of Ethylene to Ethylene Glycol Assisted by In situ Generated H2O2 from O2 Electroreduction

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WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202302466

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Electrocatalysis; Ethylene Oxidation; In Situ H2O2; Integrated System; ORR

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We have established an integrated pathway for oxidizing ethylene into ethylene glycol using mesoporous carbon catalyst and titanium silicalite-1 catalyst. This pathway exhibits remarkable activity, achieving 86% H2O2 conversion, 99% ethylene glycol selectivity, and a production rate of 51.48 mmol g(ecat)(-1) h(-1) at 0.4 V vs. reversible hydrogen electrode. In addition to using generated H2O2 as an oxidant, there is also an (OOH)-O-center dot intermediate that eliminates the step of absorbing and dissociating H2O2, showing faster reaction kinetics compared to the ex situ approach. This work not only provides a new idea for ethylene glycol synthesis but also demonstrates the advantage of in situ generated H2O2 in the tandem route.
Ethylene glycol is a useful organic compound and chemical intermediate for manufacturing various commodity chemicals of industrial importance. Nevertheless, the production of ethylene glycol in a green and safe manner is still a long-standing challenge. Here, we established an integrated, efficient pathway for oxidizing ethylene into ethylene glycol. Mesoporous carbon catalyst produces H2O2, and titanium silicalite-1 catalyst would subsequently oxidize ethylene into ethylene glycol with the in situ generated H2O2. This tandem route presents a remarkable activity, i.e., 86 % H2O2 conversion with 99 % ethylene glycol selectivity and 51.48 mmol g(ecat)(-1) h(-1) production rate at 0.4 V vs. reversible hydrogen electrode. Apart from generated H2O2 as an oxidant, there exists (OOH)-O-center dot intermediate which could omit the step of absorbing and dissociating H2O2 over titanium silicalite-1, showing faster reaction kinetics compared to the ex situ one. This work not only provides a new idea for yielding ethylene glycol but also demonstrates the superior of in situ generated H2O2 in tandem route.

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