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Where Do Photogenerated Holes Go in Anatase:Rutile TiO2? A Transient Absorption Spectroscopy Study of Charge Transfer and Lifetime

文献类型:期刊论文

作者Barnes, Piers2; Ling, Min1; Sotelo-Vazquez, Carlos1; Quesada-Cabrera, Raul1; Li, Can3; Kafizas, Andreas2; Wang, Xiuli2,3; Pendlebury, Stephanie R.2; Parkin, Ivan P.1; Durrantt, James R.2
刊名JOURNAL OF PHYSICAL CHEMISTRY A
出版日期2016-02-11
卷号120期号:5页码:715-723
ISSN号1089-5639
DOI10.1021/acs.jpca.5b11567
文献子类Article
英文摘要Anatase:rutile TiO2 junctions are often shown to be more photocatalytically active than anatase or rutile alone, but the underlying cause of this improvement is not fully understood. Herein, we employ transient absorption spectroscopy to study hole transfer across the anatase:rutile heterojunction in films as a function of phase composition. By exploiting the different signatures in the photoinduced absorption of trapped charges in anatase and rutile, we were able to separately track the yield and lifetime of holes in anatase and rutile sites within phase composites. Photogenerated holes transfer from rutile to anatase on submicrosecond time scales. This hole transfer can significantly increase the anatase hole yield, with a 20:80 anatase:rutile composite showing a 5-fold increase in anatase holes observed from the microsecond. Hole transfer does not result in an increase in charge-carrier lifetime, where an intermediate recombination dynamic between that of pure anatase (t(1/2) approximate to 0.5 ms) and rutile (t(1/2) approximate to 20 ms) is found in the anatase:rutile junction (412 approximate to 4 ms). Irrespective of what the formal band energy alignment may be, we demonstrate the importance of trap-state energetics for determining the direction of photogenerated charge separation across heterojunctions and how transient absorption spectroscopy, a method that can specifically track the migration of trapped charges, is a useful tool for understanding this behavior.
WOS关键词SENSITIZED NANOCRYSTALLINE TIO2 ; PHOTOCATALYTIC ACTIVITY ; SOLAR-CELLS ; TITANIUM-DIOXIDE ; BAND ALIGNMENT ; RUTILE TIO2 ; ELECTRONIC-STRUCTURE ; CARRIER DYNAMICS ; WATER ; PHASE
WOS研究方向Chemistry ; Physics
语种英语
WOS记录号WOS:000370210800007
出版者AMER CHEMICAL SOC
源URL[http://cas-ir.dicp.ac.cn/handle/321008/171174]  
专题大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者Kafizas, Andreas; Durrantt, James R.
作者单位1.UCL, Dept Chem, 20 Gordon St, London WC1H 0AJ, England
2.Univ London Imperial Coll Sci Technol & Med, Dept Chem, South Kensington Campus, London SW7 2AZ, England
3.Chinese Acad Sci, State Key Lab Catalysis, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, 457 Zhongshan Rd, Dalian 116023, Peoples R China
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Barnes, Piers,Ling, Min,Sotelo-Vazquez, Carlos,et al. Where Do Photogenerated Holes Go in Anatase:Rutile TiO2? A Transient Absorption Spectroscopy Study of Charge Transfer and Lifetime[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2016,120(5):715-723.
APA Barnes, Piers.,Ling, Min.,Sotelo-Vazquez, Carlos.,Quesada-Cabrera, Raul.,Li, Can.,...&Durrantt, James R..(2016).Where Do Photogenerated Holes Go in Anatase:Rutile TiO2? A Transient Absorption Spectroscopy Study of Charge Transfer and Lifetime.JOURNAL OF PHYSICAL CHEMISTRY A,120(5),715-723.
MLA Barnes, Piers,et al."Where Do Photogenerated Holes Go in Anatase:Rutile TiO2? A Transient Absorption Spectroscopy Study of Charge Transfer and Lifetime".JOURNAL OF PHYSICAL CHEMISTRY A 120.5(2016):715-723.

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来源:大连化学物理研究所

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