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	pH-dependent electron transfer from re-bipyridyl complexes to metal oxide nanocrystalline thin films
	Chunxing She ; Neil A. Anderson ; Jianchang Guo ; Fang Liu ; Wan-Hee Goh ; Dai-Tao Chen ; Debra L. Mohler ; Zhong-Qun Tian ; Tian ZQ(田中群) ; Joseph T. Hupp ; Tianquan Lian
	2005-09
英文摘要	Photoinduced interfacial electron transfer (ET) from molecular adsorbates to semiconductor nanoparticles has been a subject of intense recent interest. Unlike intramolecular ET, the existence of a quasicontinuum of electronic states in the solid leads to a dependence of ET rate on the density of accepting states in the semiconductor, which varies with the position of the adsorbate excited-state oxidation potential relative to the conduction band edge. For metal oxide semiconductors, their conduction band edge position varies with the pH of the solution, leading to pH-dependent interfacial ET rates in these materials. In this work we examine this dependence in Re(L-P)(CO)(3)Cl (or ReC1P) [L-P = 2,2'-bipyridine-4.4'-bis-CH2PO(OH)(2)] and Re(L-A)(CO)(3)Cl (or ReC1A) [L-A = 2,2'-bipyridine-4,4'-bis-CH2COOH] sensitized TiO2 and ReC1P sensitized SnO2 nanocrystalline thin films using femtosecond transient IR spectroscopy. ET rates are measured as a function of pH by monitoring the CO stretching modes of the adsorbates and mid-IR absorption of the injected electrons. The injection rate to TiO2 was found to decrease by 1000-fold from pH 0-9, while it reduced by only a factor of a few to SnO2 over a similar pH range. Comparison with the theoretical predictions based on Marcus' theory of nonadiabatic interfacial ET suggests that the observed pH-dependent ET rate can be qualitatively accounted for by considering the chance of density of electron-accepting states caused by the pH-dependent conduction band edge position.
语种	英语
出版者	AMER CHEMICAL SOC
内容类型	期刊论文
源URL	[http://dx.doi.org/doi: 10.1021/jp053948u]
专题	化学化工－已发表论文
推荐引用方式 GB/T 7714	Chunxing She,Neil A. Anderson,Jianchang Guo,et al. pH-dependent electron transfer from re-bipyridyl complexes to metal oxide nanocrystalline thin films[J],2005.
APA	Chunxing She.,Neil A. Anderson.,Jianchang Guo.,Fang Liu.,Wan-Hee Goh.,...&Tianquan Lian.(2005).pH-dependent electron transfer from re-bipyridyl complexes to metal oxide nanocrystalline thin films..
MLA	Chunxing She,et al."pH-dependent electron transfer from re-bipyridyl complexes to metal oxide nanocrystalline thin films".(2005).

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