详细信息
Optimizing water dissociation dehydrogenation process via Sn single atom incorporation for boosting photocatalytic CO2 methanation
文献类型:期刊文献
英文题名:Optimizing water dissociation dehydrogenation process via Sn single atom incorporation for boosting photocatalytic CO2 methanation
作者:Li, Mingyang[1,2];He, Chengxuan[1,2];Yang, Xiao[1,2];Liu, Zhiguo[1,2];Li, Jiaying[1,2];Wang, Lingzhi[1,2];Wu, Shiqun[1,2];Zhang, Jinlong[1,2]
机构:[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalysi, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Joint Int Res Lab Precis Chem & Mol Engn,Sch Chem, Shanghai 200237, Peoples R China
年份:2023
卷号:3
期号:10
外文期刊名:CHEM CATALYSIS
收录:WOS:【ESCI(收录号:WOS:001097337200001)】;
基金:This work was supported by the National Key R & D Program of China (2022YFE0107900 and 2022YFB3803600), the National Natural Science Foundation of China (21972040, 21673073, and 22202070), the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), the Science and Technology Commission of Shanghai Municipality (22230780200 and 20DZ2250400), the Project supported by the Shanghai Municipal Science and Technology Major Project(2018SHZDZX03), the Program of Introducing Talents of Discipline to Universities (no. B20031 and B16017), the Postdoctoral Innovative Talent Support Program (BX20220107), the Shanghai Rising-Star Program (22YF1410200), and the Fundamental Research Funds for the Central Universities(222201717003). Thanks to the Shanghai Synchrotron Radiation Facility (SSFR; beamline BL14W1) for providing beam time. Thanks to the Research Center of Analysis and Test of East China University of Science and Technology for the help on the characterizations. We thank the Anhui Absorption Spectroscopy Analysis Instrument Co., Ltd. for XAFS measurements and analysis.
语种:英文
摘要:The conversion of CO2 into value-added methane (CH4) via light -driven processes represents a promising strategy for mitigating en-ergy scarcity and curtailing CO2 pollution. However, the intricate re-action kinetics of multiple electron-proton coupling processes remain a significant challenge. During the CO2 photoreduction pro-cess, the promotion of proton production from water dissociation for CH4 generation has been overlooked. Herein, Co3O4 is modified by Sn single atoms to realize selective CH4 production from CO2 photoreduction. The introducing of Sn induces generation of oxy-gen vacancy and adjacent low-valence Co (Co2+), which favors CO2 adsorption and activation by virtue of the reduced steric hindrance and enriched electrons at Co2+ sites. Specifically, Sn single atoms serve as H2O dissociation sites, accelerating the production of pro-tons and reducing the energy barrier of the rate-determining step. Our work endows a guideline for controlling CO2 photoreduction products' selectivity through the delicate design of active sites in catalysts and reaction kinetics optimization.
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