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M/BiOCl-(M = Pt, Pd, and Au) Boosted Selective Photocatalytic CO 2 Reduction to C 2 Hydrocarbons via *CHO Intermediate Manipulation.
- Source :
-
Advanced science (Weinheim, Baden-Wurttemberg, Germany) [Adv Sci (Weinh)] 2024 Sep; Vol. 11 (35), pp. e2400934. Date of Electronic Publication: 2024 Jul 18. - Publication Year :
- 2024
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Abstract
- Selective CO <subscript>2</subscript> photoreduction to C <subscript>2</subscript> hydrocarbons is significant but limited by the inadequate adsorption strength of the reaction intermediates and low efficiency of proton transfer. Herein, an ameliorative *CO adsorption and H <subscript>2</subscript> O activation strategy is realized via decorating bismuth oxychloride (BiOCl) nanostructures with different metal (Pt, Pd, and Au) species. Experimental and theoretical calculation results reveal that distinct *CO binding energies and *H acquisition abilities of the metal cocatalysts mediate the CO <subscript>2</subscript> reduction activity and hydrocarbon selectivity. The relatively moderate *CO adsorption and *H supply over Pd/BiOCl endows it with the lowest free energy to generate *CHO, leading to its highest activity of hydrocarbon production. Specifically, the Pt cocatalyst can efficiently participate in H <subscript>2</subscript> O dissociation to deliver more *H for facilitating the protonation of the *CHO and *CHOH, thereby favoring CH <subscript>4</subscript> production with 76.51% selectivity. A lower *H supply over Pd/BiOCl and Au/BiOCl results in a large energy barrier for *CHO or *CHOH protonation and thus a more thermodynamically favored OC─CHO coupling pathway, which endows them with vastly increased C <subscript>2</subscript> hydrocarbon selectivity of 81.21% and 92.81%, respectively. The understanding of efficient C <subscript>2</subscript> hydrocarbon production in this study sheds light on how materials can be engineered for photocatalytic CO <subscript>2</subscript> reduction.<br /> (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)
Details
- Language :
- English
- ISSN :
- 2198-3844
- Volume :
- 11
- Issue :
- 35
- Database :
- MEDLINE
- Journal :
- Advanced science (Weinheim, Baden-Wurttemberg, Germany)
- Publication Type :
- Academic Journal
- Accession number :
- 39022985
- Full Text :
- https://doi.org/10.1002/advs.202400934