{"title":"Optimization of CO2 Mass Transfer and Modulation of Reaction Kinetics for Efficient CO2 Conversion via a Three‐Phase Photocatalytic Flow System","authors":"Hui Fu, Yuli Lei, Qianqian Zhang, Yuanyuan Liu, Zhaoke Zheng, Hefeng Cheng, Baibiao Huang, Haibo Ma, Peng Wang","doi":"10.1002/adfm.202515361","DOIUrl":null,"url":null,"abstract":"The design of a photocatalytic system with conducive CO<jats:sub>2</jats:sub> mass transfer, reaction kinetics, and product venting is crucial for achieving stable and efficient photocatalytic CO<jats:sub>2</jats:sub> reduction reaction (CO<jats:sub>2</jats:sub>RR). Herein, a three‐phase photocatalytic flow system is developed to optimize the CO<jats:sub>2</jats:sub> mass transfer and modulate the reaction kinetics, and prepare single‐atom‐based photocatalyst to boost the performance of CO<jats:sub>2</jats:sub>RR. Kinetic calculations present that the flow system optimizes the first‐order reaction of the conventional non‐flow system to zero‐order reaction, which facilitates the efficient and long‐lasting photocatalytic CO<jats:sub>2</jats:sub>RR. Ab initio quantum chemical simulations of both the ground and excited states reveal that the enhanced performance stems from charge transfer photoexcitation associated with the doped single Co atom, which facilitates proton adsorption, reduces the energy barrier, and promotes C–OH bond cleavage. Taking advantage of the three‐phase flow system and single‐atom catalyst, the CO generation rate increases to 2.35 µmol h<jats:sup>−1</jats:sup> with a selectivity of 97.8%. This work opens a new avenue for the rational design of high‐efficiency CO<jats:sub>2</jats:sub> conversion systems and holds promise for other photocatalytic applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"11 1","pages":""},"PeriodicalIF":18.5000,"publicationDate":"2025-07-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Functional Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/adfm.202515361","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The design of a photocatalytic system with conducive CO2 mass transfer, reaction kinetics, and product venting is crucial for achieving stable and efficient photocatalytic CO2 reduction reaction (CO2RR). Herein, a three‐phase photocatalytic flow system is developed to optimize the CO2 mass transfer and modulate the reaction kinetics, and prepare single‐atom‐based photocatalyst to boost the performance of CO2RR. Kinetic calculations present that the flow system optimizes the first‐order reaction of the conventional non‐flow system to zero‐order reaction, which facilitates the efficient and long‐lasting photocatalytic CO2RR. Ab initio quantum chemical simulations of both the ground and excited states reveal that the enhanced performance stems from charge transfer photoexcitation associated with the doped single Co atom, which facilitates proton adsorption, reduces the energy barrier, and promotes C–OH bond cleavage. Taking advantage of the three‐phase flow system and single‐atom catalyst, the CO generation rate increases to 2.35 µmol h−1 with a selectivity of 97.8%. This work opens a new avenue for the rational design of high‐efficiency CO2 conversion systems and holds promise for other photocatalytic applications.
期刊介绍:
Firmly established as a top-tier materials science journal, Advanced Functional Materials reports breakthrough research in all aspects of materials science, including nanotechnology, chemistry, physics, and biology every week.
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