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Radiolytic approach for efficient, selective and catalyst‐free CO2 conversion at room temperature

Abstract : The present study proposes a new approach for direct CO$_2$ conversion using primary radicals from water irradiation. In order to ensure reduction of CO$_2$ into CO$_2^{-•}$ by all the hydrated electrons, we use formate ions to scavenge simultaneously the parent oxidizing radicals H$^•$ and OH$^•$ producing the same transient CO$_2^{-•}$ radicals. Conditions are optimized to obtain the highest conversion yield of CO$_2$. The goal is achieved under mild conditions of room temperature, neutral pH and 1 atm of CO$_2$ pressure. All the available radicals are exploited for selectively converting CO$_2$ into oxalate that is accompanied by H$_2$ evolution. The mechanism presented accounts for the results and also sheds light on the data in the literature. The radiolytic approach is a mild and scalable route of direct CO$_2$ capture at the source in industry and the products, oxalate salt and H$_2$, can be easily separated.
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Submitted on : Thursday, July 15, 2021 - 4:36:44 PM
Last modification on : Tuesday, January 4, 2022 - 6:42:25 AM
Long-term archiving on: : Saturday, October 16, 2021 - 6:54:58 PM

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Changjiang Hu, Sarah Al Gharib, Yunlong Wang, Pingping Gan, Qiuhao Li, et al.. Radiolytic approach for efficient, selective and catalyst‐free CO2 conversion at room temperature. ChemPhysChem, Wiley-VCH Verlag, 2021, 22 (18), pp.1900-1906. ⟨10.1002/cphc.202100378⟩. ⟨cea-03287511⟩

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