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High-rate solar-light photoconversion of CO2 to fuel: controllable transformation from C1 to C2 products

Title
High-rate solar-light photoconversion of CO2 to fuel: controllable transformation from C1 to C2 products
Author(s)
Sorcar, SauravThompson, JamieHwang, Yun JuPark, YoungHoMajima, TetsuroGrimes, Craig A.Durrant, James R.In, Su-Il
Issued Date
2018-11
Citation
Energy & Environmental Science, v.11, no.11, pp.3183 - 3193
Type
Article
Keywords
REDUCED GRAPHENE OXIDEEXPOSED 001 FACETSPHOTOCATALYTIC CONVERSIONHIGH-PERFORMANCECARBON-DIOXIDEREDUCTIONNANOPARTICLESWATERANATASEWRAPPED TIO2
ISSN
1754-5692
Abstract
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.
URI
http://hdl.handle.net/20.500.11750/9472
DOI
10.1039/c8ee00983j
Publisher
Royal Society of Chemistry
Related Researcher
  • 인수일 In, Su-Il 에너지공학과
  • Research Interests CO2 conversion to hydrocarbon fuels; Water splitting for hydrogen generation; Quantum dot devices; Dye sensitized solar cells; Environmental remediation; Synthesis of functional nanomaterials; CO2 연료전환; 수소생산을 위한 광전기화학적 물분해; 양자점 태양전지; 염료감응 태양전지; 공해물질 저감연구; 기능성 나노소재 개발
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Department of Energy Science and Engineering Green and Renewable Energy for Endless Nature(GREEN) Lab 1. Journal Articles

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