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dc.contributor.authorChunxing She
dc.contributor.authorNeil A. Anderson
dc.contributor.authorJianchang Guo
dc.contributor.authorFang Liu
dc.contributor.authorWan-Hee Goh
dc.contributor.authorDai-Tao Chen
dc.contributor.authorDebra L. Mohler
dc.contributor.authorZhong-Qun Tian
dc.contributor.author田中群
dc.contributor.authorJoseph T. Hupp
dc.contributor.authorTianquan Lian
dc.date.accessioned2011-10-25T05:46:11Z
dc.date.available2011-10-25T05:46:11Z
dc.date.issued2005-09
dc.identifier.citationJ. Phys. Chem. B, 2005, 109 (41): 19345–19355zh_CN
dc.identifier.issn1520-6106
dc.identifier.urihttp://dx.doi.org/doi: 10.1021/jp053948u
dc.identifier.urihttps://dspace.xmu.edu.cn/handle/2288/10999
dc.description.abstractPhotoinduced 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.zh_CN
dc.language.isoenzh_CN
dc.publisherAMER CHEMICAL SOCzh_CN
dc.titlepH-dependent electron transfer from re-bipyridyl complexes to metal oxide nanocrystalline thin filmszh_CN
dc.typeArticlezh_CN


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