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Constructing Supramolecular System For Photo-driven Water Oxidation

Posted on:2015-09-07Degree:MasterType:Thesis
Country:ChinaCandidate:L N DuanFull Text:PDF
GTID:2181330467984572Subject:Applied Chemistry
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Utilizing solar energy to split water into molecular oxygen and hydrogen is an attractive way to product clean and sustainable fuels for meeting environmentally problems and the future energy demands. Recently, a great number of researches have been made in constructing a Photoelectrochemical Cell (PEC), in order to realize effectively photo-driven water splitting. However, the main problem of the PEC performance is poor electron transfer and charge separation. To resolve this problem, two types of assembly supramoleculars (ASMs) have been synthesized in this paper.Firstly, ASM1and ASM2have been assembled as catalyst-catalyst supramoleculars. They are separately synthesized with Ru1and Ru2, which are both developed with low over potentials in our group. And the chemical catalytic activities of ASM1and ASM2are investgated in pure water, with [Ce(NH4)2(NO3)6](CeⅣ) as an oxidant. In this study, it is interesting to find that the catalytic activity of ASM2is three times higher than the precursor Ru2, and much higher than ASM1. So it suggests that electron transfer can be improved by changing the molecular links of the precursor.In addition, another type of supramolecules, ASM3-ASM5, has been assembled by phtosensitizer and catalyst together. The photocatalytic activity of ASM3-ASM5are measured in pH=6.8phosphate buffer solution (10%acetonitrile), Na2S2O8as an electron acceptor, and visible light (λ>400nm). ASM4has obtained the best photocatalytic performance with a TON of34. It can be demonstrated that photocatalytic performance can be benefited by adjusting the distance of photosensitizer and catalyst. Besides, ASM6has obtained a higher TON, compared with the complex31, which reported by Sun Licheng research group,.These two kinds of supramolecules, connected with flexible linkages, could be used as suitable candidates for assembly photoanodes for water oxidation in PECs. Such works are undergoing in our lab.
Keywords/Search Tags:Supramolecular, chemical catalytic water oxidation, photocatalytic wateroxidation
PDF Full Text Request
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