Unravelling the effect of charge dynamics at the plasmonic metal/semiconductor interface for CO2 photoreduction

被引:218
作者
Collado, Laura [1 ,2 ]
Reynal, Anna [3 ,4 ,5 ]
Fresno, Fernando [1 ]
Barawi, Mariam [1 ]
Escudero, Carlos [6 ]
Perez-Dieste, Virginia [6 ]
Coronado, Juan M. [2 ]
Serrano, David P. [2 ,7 ]
Durrant, James R. [3 ,4 ]
de la Pena O'Shea, Victor A. [1 ]
机构
[1] Inst IMDEA Energy, Photoactivated Proc Unit, Avda Ramon Sagra 3, Madrid 28935, Spain
[2] Inst IMDEA Energy, Thermochem Proc Unit, Avda Ramon Sagra 3, Madrid 28935, Spain
[3] Imperial Coll London, Dept Chem, Exhibit Rd, London SW7 2AZ, England
[4] Imperial Coll London, Ctr Plast Elect, Exhibit Rd, London SW7 2AZ, England
[5] Teesside Univ, Sch Sci Engn & Design, Borough Rd, Middlesbrough TS1 3BA, Cleveland, England
[6] ALBA Synchrotron Light Source, Carretera BP 1413,Km 3-3, Cerdanyola Del Valles, Spain
[7] Rey Juan Carlos Univ, Dept Chem & Energy Technol, C Tulipan S-N, Madrid 28935, Spain
基金
欧洲研究理事会;
关键词
IN-SITU; PHOTOCATALYTIC CONVERSION; HYDROCARBON FUELS; OXIDE INTERFACES; HOLY-GRAIL; TIO2; SURFACE; WATER; SEMICONDUCTOR; NANOPARTICLES;
D O I
10.1038/s41467-018-07397-2
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
070301 [无机化学]; 070403 [天体物理学]; 070507 [自然资源与国土空间规划学]; 090105 [作物生产系统与生态工程];
摘要
Sunlight plays a critical role in the development of emerging sustainable energy conversion and storage technologies. Light-induced CO2 reduction by artificial photosynthesis is one of the cornerstones to produce renewable fuels and environmentally friendly chemicals. Interface interactions between plasmonic metal nanoparticles and semiconductors exhibit improved photoactivities under a wide range of the solar spectrum. However, the photoinduced charge transfer processes and their influence on photocatalysis with these materials are still under debate, mainly due to the complexity of the involved routes occurring at different timescales. Here, we use a combination of advanced in situ and time-resolved spectroscopies covering different timescales, combined with theoretical calculations, to unravel the overall mechanism of photocatalytic CO2 reduction by Ag/TiO2 catalysts. Our findings provide evidence of the key factors determining the enhancement of photoactivity under ultraviolet and visible irradiation, which have important implications for the design of solar energy conversion materials.
引用
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页数:10
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