机构地区:[1]School of Environmental and Safety Engineering,Liaoning Petrochemical University,Fushun 113001,China [2]Biobased Chemistry and Technology,Wageningen University&Research,Stippeneng 4,Wageningen 6708 WE,The Netherlands [3]Laboratory of Organic Chemistry,Wageningen University&Research,Bornse Weilanden 9,Wageningen 6708 WG,The Netherlands [4]State Key Laboratory of Catalysis,Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,China [5]School of New Energy,Nanjing University of Science and Technology,Jiangyin 214000,China
出 处:《Nano Research》2023年第3期3730-3740,共11页纳米研究(英文版)
基 金:supported by the National Natural Science Foundation of China(No.22172068);the Natural Science Foundation of Jiangsu Province(No.BK20221485);the Liaoning Revitalization Talents Program(No.XLYC1902065);the Scientific Research Fund of Liaoning Provincial Department of Education(No.LJKMZ20220747);the Talent Scientific Research Fund of LSHU(No.2016XJJ-012).
摘 要:Photogenerated charge separation and transfer is one of the bottleneck steps in photocatalysis,and efficient charge separation strategies are strongly desired.Here,mimicking the electron transport chain in natural photosynthesis,we report the design and fabrication of a charge transfer chain using bismuth-based semiconductor as a proof-of-concept.In view of the thermodynamic energy band positions and structural similarity based on the density functional theory(DFT)analysis,heterostructured combination ofα-Bi_(2)O_(3),perovskite-like Bi_(4)Ti_(3)O_(12),and sillenite Bi12TiO20 was designed for fabrication of charge transfer chain.By tuning the molar ratio of Bi and Ti precursors,the Bi_(4)Ti_(3)O_(12)and Bi12TiO20 particles were formed on the surface ofα-Bi_(2)O_(3)by an insitu transformation process,giving rise to Bi_(12)TiO_(20)-Bi_(4)Ti_(3)O_(12)/α-Bi_(2)O_(3)composites with charge transfer chain.We propose that the effective charge transfer is accomplished amongα-Bi_(2)O_(3),Bi12TiO20,and Bi_(4)Ti_(3)O_(12),which significantly improves the photogenerated charge separation and transfer,as indicated by photoluminescene,time-resolved photoluminescene,and electrochemical impedance spectra results.As expected,the Bi_(12)TiO_(20)-Bi_(4)Ti_(3)O_(12)/α-Bi_(2)O_(3)shows the superior photocatalytic activity for the degradation of environmental pollutants with high concentration.Even for the refractory pollutants like 4-chlorophenol,the optimal Bi_(12)TiO_(20)-Bi_(4)Ti_(3)O_(12)/α-Bi_(2)O_(3)composite shows 28 times higher than that ofα-Bi_(2)O_(3)for photocatalytic degradation,verifying the superiority of photogenerated charge transfer chain in photocatalysis.This work demonstrates the feasibility of the charge transfer chain strategy to boost the photogenerated charge separation,which is of great significance for designing energy and environmental-related materials in heterogonous photocatalysis.
关 键 词:photogenerated charge separation charge transfer chain bismuth titanates bismuth oxides
分 类 号:TB33[一般工业技术—材料科学与工程]
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