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Regulating CO2 hydrogenation pathways to methanol over Cu-based catalysts via Y modification
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K
H
周
奚
DOI：10.1002/aic.70528.png)
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Abstract
En 中文
Precise modulation of Cu-based catalysts is crucial yet challenging. Herein, Y was introduced into Cu-ZnO catalysts to tune their electronic and structural features. Characterizations including in situ XRD, N2O titration, and TEM-EDS revealed that Y addition reduced metallic Cu nanoparticle size and enhanced dispersion within a Y-modified ZnO matrix, suggesting increased density of Cu+–O–Znδ+ interfacial sites. Quasi-in situ XPS revealed that Y incorporation induces charge transfer, decreasing the electron density on surface Cu0 and Cu+. In situ DRIFTS analysis identified the *CO pathway on Cu0 and the formate pathway on Cu+–O–Znδ+ sites. The reduced charge density of Cu0 suppressed the *CO pathway, while electron–deficient Cu+ promoted the transformation of bidentate formate into a more active monodentate configuration. Consequently, Y-induced electronic modification enhanced methanol turnover frequency from 15.3 to 19.2 h−1 by regulating CO2 hydrogenation pathways. This strategy may guide rational catalyst design and provide insights into CO2 hydrogenation.
Keywords:
CO2 hydrogenation
Cu+–O–Znδ+ interfaces
monodentate formate pathway
oxygen vacancy
yttrium modification
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4
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1.1W
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2.9W
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