气候变化领域集成服务门户(CCPortal): High-rate solar-light photoconversion of CO2 to fuel: Controllable transformation from C1 to C2 products

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DOI	10.1039/c8ee00983j
	High-rate solar-light photoconversion of CO2 to fuel: Controllable transformation from C1 to C2 products
	Sorcar S.; Thompson J.; Hwang Y.; Park Y.H.; Majima T.; Grimes C.A.; Durrant J.R.; In S.-I.
发表日期	2018
ISSN	17545692
起始页码	3183
结束页码	3193
卷号	11 期号:11
英文摘要	The production of solar fuels offers a viable pathway for reducing atmospheric CO2 concentrations and the storage and transport of solar energy. While photoconversion of CO2 into C1 hydrocarbon products, notably methane (CH4), is known, the ability to directly achieve significant quantities of higher-order hydrocarbons represents an important step towards practical implementation of solar fuel technologies. We describe an efficient, stable, and readily synthesized CO2-reduction photocatalyst, Pt-sensitized graphene-wrapped defect-induced blue-coloured titania, that produces a record high combined photocatalytic yield of ethane (C2H6) and methane. For the first time, a systematic ultraviolet photoelectron spectroscopy study on the mechanism underlying ethane formation indicates that the process is dependent upon upward band bending at the reduced blue-titania/graphene interface. Furthermore, transient absorption spectroscopy indicates photogenerated holes move into the graphene while electrons accumulate on the Ti3+ sites, a phenomenon contradicting prior assumptions that graphene acts as an electron extractor. We find that both mechanisms serve to enhance multielectron transfer processes that generate CH3. Utilizing a continuous flow-through (CO2, H2O) photoreactor, over the course of multiple 7 h runs approximate totals of 77 μmol g-1 C2H6 and 259 μmol g-1 CH4 are obtained under one sun AM 1.5G illumination. The photocatalyst exhibits an apparent quantum yield of 7.9%, 5.2% CH4 and 2.7% C2H6, and stable photocatalytic performance over the test duration of 42 h. The carbon source for both products is verified using 13CO2 isotopic experiments. © The Royal Society of Chemistry 2018.
英文关键词	Absorption spectroscopy; Atmospheric movements; Carbon dioxide; Ethane; Fuel storage; Fuels; Methane; Solar energy; Titanium dioxide; Ultraviolet photoelectron spectroscopy; CO2 concentration; Continuous flows; Higher order hydrocarbons; Hydrocarbon product; Multielectron transfer; Photocatalytic performance; Photogenerated holes; Transient absorption spectroscopies; Graphene; carbon dioxide; catalyst; concentration (composition); electron; energy storage; ethane; power generation; quantitative analysis; solar power; titanium; transformation
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190064
作者单位	Department of Energy Science and Engineering, DGIST, 333 Techno Jungang-daero, Hyeonpung-myeon, Dalseong-gun, Daegu, 42988, South Korea; Department of Chemistry and Centre for Plastic Electronics, Imperial College London, London, SW7 2AZ, United Kingdom; Institute of Scientific and Industrial Research (SANKEN), Osaka University, Mihogaoka 8-1, Ibaraki Osaka, 567-0047, Japan; Flux Photon Corporation, 6900 Darcy Lane, Raleigh, NC 27606, United States
推荐引用方式 GB/T 7714	Sorcar S.,Thompson J.,Hwang Y.,et al. High-rate solar-light photoconversion of CO2 to fuel: Controllable transformation from C1 to C2 products[J],2018,11(11).
APA	Sorcar S..,Thompson J..,Hwang Y..,Park Y.H..,Majima T..,...&In S.-I..(2018).High-rate solar-light photoconversion of CO2 to fuel: Controllable transformation from C1 to C2 products.Energy & Environmental Science,11(11).
MLA	Sorcar S.,et al."High-rate solar-light photoconversion of CO2 to fuel: Controllable transformation from C1 to C2 products".Energy & Environmental Science 11.11(2018).