Matched micro-geometrical configuration leading to hetero-interfacial intimate contact of MoS_(2)@UiO-66-NH_(2) Z-scheme heterojunction for efficient photocatalytic CO_(2) reduction  

作　　者：Xin Yang Tianyu Wang Huiyang Ma Weiliang Shi Zhengqiang Xia Qi Yang Pan Zhang Ren Ma Gang Xie Sanping Chen 

机构地区：[1]Key Laboratory of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education,College of Chemistry and Materials Science,Northwest University,Xi’an 710127,China [2]Shaanxi Key Laboratory for Carbon Neutral Technology,Carbon Neutrality College(Yulin),Northwest University,Xi’an 710069,China

出　　处：《Journal of Materials Science & Technology》2024年第15期210-219,共10页材料科学技术（英文版）

基　　金：supported by the National Natural Science Founda-tion of China(Nos.22273073,22173072,21973074,and 21965037;the Innovation Capability Support Program of Shaanxi Province(No.2022TD-32)。

摘　　要：Z-scheme heterojunction is an effective strategy in photocatalysis,when hetero-interfacial intimate con-tact is the center of high-performance Z-scheme heterojunction structure.Here,x-MoS_(2)[x=plate(p),flower(f),and solid sphere(s)]with extensive optical absorption and high conductivity and stable UiO-66-NH_(2)(y)(y=100,300,and 500 nm)with rich Lewis’s acid sites were integrated to a series of x-MoS_(2)@UiO-66-NH_(2)(y)Z-scheme heterojunctions,which were fully characterized and used for photocat-alytic reduction of CO_(2)(pCO_(2)RR)into CH_(4) and CO.In response to the difficult modification of MoS_(2)and loose contact of composite bulk materials,the micro-geometric configurations on the size of UiO-66-NH_(2)and the morphology of MoS_(2)were optimized to achieve an intimate contact.The Z-scheme heterojunc-tion f-MoS_(2)@UiO-66-NH_(2)(100 nm)with perfectly matched micro-geometric configuration exhibited an excellent electron consumption rate(Rele)of 263.78μmol g^(-1)h^(-1)and a high CH_(4) yield of 27.18μmol g^(-1)h^(-1)with a selectivity of 82.44%,being far superior to most MoS_(2)-and MOFs-based heterojunctions.Com-prehensive investigations with extensive photoelectric characterizations,control experiments,and den-sity functional theory(DFT)calculations demonstrate that the excellent photocatalytic performance of f-MoS_(2)@UiO-66-NH_(2)(100 nm)could be attributed to that(i)the low size of UiO-66-NH_(2)strengthens mutual alignment and increases outer surface to maximize heterointerface contact with MoS_(2),acceler-ating the interfacial charge transfer;(ii)the hierarchical structure of f-MoS_(2)with optimal basal plane curvature greatly reduces contact barriers to present a high charge throughput with a charge excita-tion rate of 1.967 mV,smooth initiating the 8-electron CO_(2)methanation.Additionally,the durability of f-MoS_(2)@UiO-66-NH_(2)(100 nm)was also investigated.

关 键 词：HETEROJUNCTION PHOTOCATALYSIS Carbon dioxide reduction Metal-organic frameworks 

分 类 号：X701[环境科学与工程—环境工程] O643.36[理学—物理化学] O644.1[理学—化学]