Enhancing Photocatalytic CO 2 Conversion through Oxygen‐Vacancy‐Mediated Topological Phase Transition
Abstract Weak adsorption of gas reactants and strong binding of intermediates present a significant challenge for most transition metal oxides, particularly in the realm of CO 2 photoreduction. Herein, we demonstrate that the adsorption can be fine‐tuned by phase engineering of oxide catalysts. An o...
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Published in | Angewandte Chemie Vol. 136; no. 11 |
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Main Authors | , , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
11.03.2024
|
Online Access | Get full text |
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Summary: | Abstract
Weak adsorption of gas reactants and strong binding of intermediates present a significant challenge for most transition metal oxides, particularly in the realm of CO
2
photoreduction. Herein, we demonstrate that the adsorption can be fine‐tuned by phase engineering of oxide catalysts. An oxygen vacancy mediated topological phase transition in Ni‐Co oxide nanowires, supported on a hierarchical graphene aerogel (GA), is observed from a spinel phase to a rock‐salt phase. Such in situ phase transition empowers the Ni‐Co oxide catalyst with a strong internal electric field and the attainment of abundant oxygen vacancies. Among a series of catalysts, the in situ transformed spinel/rock‐salt heterojunction supported on GA stands out for an exceptional photocatalytic CO
2
reduction activity and selectivity, yielding an impressive CO production rate of 12.5 mmol g
−1
h
−1
and high selectivity of 96.5 %. This remarkable performance is a result of the robust interfacial coupling between two topological phases that optimizes the electronic structures through directional charge transfer across interfaces. The phase transition process induces more Co
2+
in octahedral site, which can effectively enhance the Co‐O covalency. This synergistic effect balances the surface activation of CO
2
molecules and desorption of reaction intermediates, thereby lowering the energetic barrier of the rate‐limiting step. |
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ISSN: | 0044-8249 1521-3757 |
DOI: | 10.1002/ange.202317957 |