气候变化领域集成服务门户(CCPortal): Direct photoactivation of a nickel-based, water-reduction photocathode by a highly conjugated supramolecular chromophore

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DOI	10.1039/c7ee03115g
	Direct photoactivation of a nickel-based, water-reduction photocathode by a highly conjugated supramolecular chromophore
	Shan B.; Nayak A.; Sampaio R.N.; Eberhart M.S.; Troian-Gautier L.; Brennaman M.K.; Meyer G.J.; Meyer T.J.
发表日期	2018
ISSN	17545692
起始页码	447
结束页码	455
卷号	11 期号:2
英文摘要	In dye-sensitized photoelectrosynthesis cells, multi-step photoinduced electron transfer takes place to generate redox-separated (RS) states that activate catalysts for water splitting or carbon dioxide reduction. From photoexcitation of the chromophores to formation of the RS states, the solar energy initially stored at the chromophore excited states is reduced stepwise in a sequence of photoinduced electron transfer steps. We report here a water-reduction photocathode based on a supramolecular chromophore, an ethyne-bridged (porphyrinato)zincII and bis(terpyridyl)rutheniumII complex, which is surface-bound to a mesoporous nickel oxide electrode, with an over-layer of nickel sulfide derivative as a water reduction catalyst. Visible light excitation of the chromophore generates a long-lived RS state that forms directly at its excited state with the electron delocalized at the terpyridyl ligands for transferring to the nickel sulfide catalyst, and the hole at the zinc porphyrin moiety for injecting into the nickel oxide electrode. The resulting photocathode shows enhanced photoelectrocatalytic performances relative to the previously reported NiO-based photocathodes. A key element lies in the efficient, direct activation of the catalyst by the long-lived, RS excited state that minimizes the energy loss along the photoinduced electron transfer steps towards water reduction. © 2018 The Royal Society of Chemistry.
英文关键词	Carbon; Carbon dioxide; Catalysts; Chromophores; Dye-sensitized solar cells; Electrodes; Electron transitions; Electrons; Energy dissipation; Field emission cathodes; Nickel; Nickel oxide; Photocathodes; Pollution control; Ruthenium compounds; Solar energy; Sulfur compounds; Supramolecular chemistry; Zinc; Carbon dioxide reduction; Direct activation; Oxide electrodes; Photo activations; Photo-induced electron transfer; Photoelectrocatalytic; Visible light excitation; Zinc porphyrins; Excited states; carbon dioxide; catalyst; electrode; electron; inorganic compound; performance assessment; photovoltaic system; porphyrin; redox conditions; reduction
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/190329
作者单位	Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, NC 27599-3290, United States
推荐引用方式 GB/T 7714	Shan B.,Nayak A.,Sampaio R.N.,et al. Direct photoactivation of a nickel-based, water-reduction photocathode by a highly conjugated supramolecular chromophore[J],2018,11(2).
APA	Shan B..,Nayak A..,Sampaio R.N..,Eberhart M.S..,Troian-Gautier L..,...&Meyer T.J..(2018).Direct photoactivation of a nickel-based, water-reduction photocathode by a highly conjugated supramolecular chromophore.Energy & Environmental Science,11(2).
MLA	Shan B.,et al."Direct photoactivation of a nickel-based, water-reduction photocathode by a highly conjugated supramolecular chromophore".Energy & Environmental Science 11.2(2018).