Atmosphere engineering of metal-free Te/C_(3)N_(4) p-n heterojunction for nearly 100% photocatalytic converting CO_(2) to CO  

作　　者：Huange Liao Kai Huang Weidong Hou Huazhang Guo Cheng Lian Jiye Zhang Zheng Liu Liang Wang 

机构地区：[1]Institute of Nanochemistry and Nanobiology,School of Environmental and Chemical Engineering,Shanghai University,Shanghai 200444,China [2]State Key Laboratory of Chemical Engineering,Shanghai Engineering Research Center of Hierarchical Nanomaterials,and School of Chemistry and Molecular Engineering,East China University of Science and Technology,Shanghai 200237,China [3]School of Materials Science and Engineering,Shanghai University,Shanghai 200444,China [4]School of Materials Science and Engineering,Nanyang Technological University,50 Nanyang Avenue,639798,Singapore

出　　处：《Advanced Powder Materials》2024年第6期81-90,共10页先进粉体材料(英文)

基　　金：funded by China Postdoctoral Science Foundation(2023T160406);Shanghai Pujiang Program(21PJD022);This project was also supported by Singapore Ministry of Education AcRF Tier 2(MOE-MOET2EP10121-0006)and AcRF Tier 1(RG7/21);This work is Supported by Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University.

摘　　要：Carbon nitride(CN)-based heterojunction photocatalysts hold promise for efficient carbon dioxide(CO_(2))reduction.However,suboptimal production yields and limited selectivity in CO_(2)conversion pose significant barriers to achieving efficient CO_(2)conversion.Here,we present the construction of a p-n heterojunction between ultrasmall Te NPs and CN nanosheet using a novel tandem hydrothermal-calcination synthesis strategy.Through ammonia-assisted calcination,ultrasmall Te NPs are grown in-situ on the CN nanosheets’surface,resulting in the generation of a robust p-n heterojunction.The synthesized heterojunction exhibits increased specific surface area,reinforced visible light absorption,intensive CO_(2)adsorption capacity,and efficient charge transfer.The optimum Te/CN-NH_(3)demonstrates superior photocatalytic CO_(2)reduction activity and durability,with nearly 100%selectivity for CO and a yield as high as 92.0μmol g^(-1)h^(-1),a fourfold increase compared to pure CN.Experimental and theoretical calculations unravel that the strong built-in electric field of the Te/CN-NH_(3)p-n heterojunction accelerates the migration of photogenerated electrons from Te NPs to the N site on CN nanosheets,thereby promoting CO_(2)reduction.This study provides a promising material design approach for the construction of highperformance p-n heterojunction photocatalysts.

关 键 词：p-n heterojunction Carbon nitride Built-in electric field Photocatalytic carbon dioxide reduction Heterojunction photocatalysts 

分 类 号：TB3[一般工业技术—材料科学与工程]