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Photochemical energy storage: studies of inorganic photoassistance agents. Progress report, December 17, 1979-March 31, 1981

Technical Report ·
DOI:https://doi.org/10.2172/6727863· OSTI ID:6727863

Research progress has been made in the study of p-type semiconductor (photocathode) electrode materials. A number of small band gap (E/sub g/ approximately equal to 1.1 to 1.4 eV) p-type semiconductors have been demonstrated to have poor H/sub 2/ evolution kinetics despite the fact that a reasonable output photovoltage (E/sub V/) compared to E/sub g/ could be expected. Special emphasis has been on p-type Si (E/sub g/ = 1.1 eV) and p-type InP (E/sub g/ = 1.35 eV). Both of these materials give poor kinetics for H/sub 2/ evolution from H/sub 2/O, while the kinetics for N,N'-dimethyl-4,4'-bipyridinium, MV/sup 2 +/, reduction to MV/sup +/ are good at a pH where E/sup 0/(H/sub 2/O/H/sub 2/) is the same as E/sup 0/(MV/sup 2+/+/). A surface derivatizing reagent from diquarternizing 4,4'-bipyridine with 1-bromo-3-trimethyloxysilylpropane can be used to functionalize p-type Si with polymeric quantities of redox reagent. The surface-confined bipyridinium reagent, (PQ/sup 2 +/)/sub surf./, can be photoreduced to (PQ/sup +/)/sub surf./ and this reduced species can be used to effect H/sub 2/ evolution if a Pt catalyst is incorporated into the polymer. Efficiency for conversion of monochromatic 632.8 nm light to H/sub 2/ exceeds 6%, compared to much less than 1% for the naked p-type Si without the surface catalyst system. Studies of n-type semiconductor (photoanode) electrode materials modified with biferrocene-based redox mediators for I/sup -/ ..-->.. I/sub 3//sup -/ oxidation have been undertaken for comparison to ferrocene-based reagents for the same reaction; a five- to ten-fold overall improvement in heterogeneous I/sup -/ ..-->.. I/sub 3//sup -/ rate can be achieved using the two-electron mediator compared to the one-electron transfer system.

Research Organization:
Massachusetts Inst. of Tech., Cambridge (USA)
Sponsoring Organization:
USDOE
OSTI ID:
6727863
Report Number(s):
DOE/ER/04178-4
Country of Publication:
United States
Language:
English

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