Light-assisted catalysis and the dynamic nature of surface species in the reverse water gas shift reaction over Cu/γ-Al2O3

Lorber, Kristijan; Arčon, Iztok; Huš, Matej; Zavašnik, Janez; Sancho-Parramon, Jordi; Prašnikar, Anže; Likozar, Blaž; Novak Tušar, Nataša; Djinović, Petar (2024) Light-assisted catalysis and the dynamic nature of surface species in the reverse water gas shift reaction over Cu/γ-Al2O3. ACS Applied Materials & Interfaces, 16 (49). pp. 67778-67790. ISSN 1944-8244

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Abstract

The reverse water gas shift (RWGS) reaction converts CO2 and H2 into CO and water. We investigated Cu/gamma-Al2O3 catalysts in both thermally driven and light-assisted RWGS reactions using visible light. When driven by combined visible light and thermal energy, the CO2 conversion rates were lower than in the dark. Light-assisted reactions showed an increase in the apparent activation energy from 68 to 87 kJ/mol, indicating that light disrupts the energetically favorable pathway active in the dark. A linear correlation between irradiance and decreasing reaction rate suggests a photon-driven phenomenon. In situ diffuse reflectance infrared Fourier transform spectroscopy and TD-DFT analyses revealed that catalyst illumination causes significant, partly irreversible surface dehydroxylation, highlighting the importance of OH groups in the most favorable RWGS pathway. This study offers a novel approach to manipulate surface species and control activity in the RWGS reaction.

Item Type:	Article
Uncontrolled Keywords:	light-assisted catalysis; reaction mechanism; in situ spectroscopy; hydroxyl; copper; RWGS
Subjects:	NATURAL SCIENCES > Chemistry
Divisions:	Division of Materials Physics
Depositing User:	Jordi Sancho Parramon
Date Deposited:	17 Apr 2025 10:50
URI:	http://fulir.irb.hr/id/eprint/9705
DOI:	10.1021/acsami.4c15849

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