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Selective Reduction of CO2on Ti2C(OH)2MXene through Spontaneous Crossing of Transition States

Parui, A and Srivastava, P and Singh, AK (2022) Selective Reduction of CO2on Ti2C(OH)2MXene through Spontaneous Crossing of Transition States. In: ACS Applied Materials and Interfaces .

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Official URL: https://doi.org/10.1021/acsami.2c10213


Direct reduction of gas-phase CO2 to renewable fuels and chemical feedstock without any external energy source or rare-metal catalyst is one of the foremost challenges. Here, using density functional theory and ab initio molecular dynamics (AIMD) simulations, we predict Ti2C(OH)2 MXene as an efficient electron-coupled proton donor exhibiting simultaneously high reactivity and selectivity for CO2 reduction reaction (CRR) by yielding valuable chemicals, formate, and formic acid. This is caused by CO2 spontaneously crossing the activation barrier involved in the formation of multiple intermediates. Metallic Ti2C(OH)2 contains easily donatable protons on the surface and high-energy electrons near the Fermi level that leads to its high reactivity. High selectivity arises from low activation barrier for CRR as predicted by proposed mechanistic interpretations. Furthermore, H vacancies generated during the product formation can be replenished by exposure to moisture, ensuring the uninterrupted formation of the products. Our study provides a single-step solution for CRR to valuable chemicals without necessitating the expensive electrochemical or low-efficiency photochemical cells and hence is of immense interest for recycling the carbon. © 2022 American Chemical Society.

Item Type: Journal Article
Publication: ACS Applied Materials and Interfaces
Publisher: American Chemical Society
Additional Information: The copyright for this article belongs to the American Chemical Society.
Keywords: Catalysts; Chemical activation; Density functional theory; Molecular dynamics; Reaction kinetics; Reduction; Titanium compounds, reductions; Ab initio molecular dynamics; CO 2 reduction; CO2 reduction; CO2activation; Density-functional-theory; Gaseous CO2reduction; Mxene; Reduction reaction; Spontaneous reduction, Carbon dioxide
Department/Centre: Division of Chemical Sciences > Materials Research Centre
Date Deposited: 06 Oct 2022 10:58
Last Modified: 06 Oct 2022 10:58
URI: https://eprints.iisc.ac.in/id/eprint/77247

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