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Identification of active sites for formaldehyde oxidation on mesoporous Pt/CeO2 catalyst at ambient temperature and low humidity

Journal 2025 · IF 7.5 · 发表于 2025 年 3 月 3 日
作者: Ruichen Wang,Chao Yu,Juanjuan Gong,Qingfa Su,Hui Chen,Canyan Yang,Shaodi Sun,Zhiwei Huang,Huazhen Shen,Huawang Zhao,Bihong Lv,Xiaomin Wu,Guohua Jing
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摘要

Identification of active sites governing the performance of indoor formaldehyde (HCHO) oxidation at ambient temperature and low humidity is crucial for developing improved catalysts, but remains challenging. It has recently been discovered that the effective dissociation of water is of importance for HCHO oxidation at low humidity. Here, we have elaborately designed a Pt supported on three-dimensionally ordered mesoporous CeO 2 catalyst (Pt/kit-CeO 2 ). The Pt/kit-CeO 2 catalyst achieves ∼ 95 % CO 2 yield for a long time. The results indicate that the abundant oxygen vacancies and single coordination-unsaturated Ce sites on mesoporous CeO 2 enhance H 2 O dissociation, leading to the generation of a substantial amount of terminal hydroxyl groups (OH t ). These OH t groups promote the oxidation of intermediate dioxymethylene (DOM) and formate species, thereby regulating the catalytic activity. Additionally, the dispersed Pt facilitates the activation of O 2 , generating active oxygen species (O*) that work synergistically with OH t groups to promote the conversion of formates into CO 2 . The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) further elucidated the mechanism of catalyst promoting HCHO oxidation: HCHO (+O*) → DOM (+OH t ) → HCOO – /HCOOH (+OH t /O*) → CO 3 2– → CO 2 . We anticipate that this knowledge will inspire the development of Pt-based catalysts specifically tailored for low humidity.

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