Abstract
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-MoS2[x=plate(p),flower(f),and solid sphere(s)]with extensive optical absorption and high conductivity and stable UiO-66-NH2(y)(y=100,300,and 500 nm)with rich Lewis's acid sites were integrated to a series of x-MoS2@UiO-66-NH2(y)Z-scheme heterojunctions,which were fully characterized and used for photocat-alytic reduction of CO2(pCO2RR)into CH4 and CO.In response to the difficult modification of MoS2 and loose contact of composite bulk materials,the micro-geometric configurations on the size of UiO-66-NH2 and the morphology of MoS2 were optimized to achieve an.intimate contact.The Z-scheme heterojunc-tion f-MoS2@UiO-66-NH2(100 nm)with perfectly matched micro-geometric configuration exhibited an excellent electron consumption rate(Rele)of 263.78 μmol g-1 h-1 and a high CH4 yield of 27.18 μmol g-1 h-1 with a selectivity of 82.44％,being far superior to most MoS2-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-MoS2@UiO-66-NH2(100 nm)could be attributed to that(ⅰ)the low size of UiO-66-NH2 strengthens mutual alignment and increases outer surface to maximize heterointerface contact with MoS2,acceler-ating the interfacial charge transfer;(ⅱ)the hierarchical structure of f-MoS2 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 CO2 methanation.Additionally,the durability of f-MoS2@UiO-66-NH2(100 nm)was also investigated.
基金项目
国家自然科学基金(22273073)
国家自然科学基金(22173072)
国家自然科学基金(21973074)
国家自然科学基金(21965037)
Innovation Capability Support Program of Shaanxi Province(2022TD-32)
NETL
NSTL
万方数据