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Synthesis and characterization of a photosensitive interface for hydrogen generation: chemically modified p-type semiconducting silicon photocathodes

Journal Article · · Proc. Natl. Acad. Sci. U.S.A.; (United States)
; ; ; ;

p-Si photocathodes functionalized first with an N,N'-dialkyl-4,4'-bipyridinium redox reagent, (PQ/sup 2+/+./)/sub surf/, and then with a Pt precursor, PtCl/sub 6//sup 2 -/, give significant efficiency (up to 5%) for photoelectrochemical H/sub 2/ generation with 632.8-nm light. Naked p-Si photocathodes give nearly zero efficiency, owing to poor H/sub 2/ evolution kinetics that are improved by the (PQ/sup 2+/+.//sub surf)/Pt modification. The mechanism of H/sub 2/ evolution from p-Si/(PQ/sup 2+/+./)/sub surf/Pt is first photoexcitation of electrons to the conduction band of Si followed by (PQ/sup 2 +/)/sub surf/ ..-->.. (PQ/sup +.//sub surf/ reduction. The dispersion of Pt then catalyzes H/sub 2/O reduction to give H/sub 2/ and regeneration of (PQ/sup 2/)/sub surf/. The overall energy conversion efficiency rivals the best direct optical to chemical conversion systems reported to date.

Research Organization:
Massachusetts Inst. of Technology, Cambridge
OSTI ID:
7017702
Journal Information:
Proc. Natl. Acad. Sci. U.S.A.; (United States), Journal Name: Proc. Natl. Acad. Sci. U.S.A.; (United States) Vol. 77:11; ISSN PNASA
Country of Publication:
United States
Language:
English

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Related Subjects

08 HYDROGEN
080101 -- Hydrogen-- Production-- Electrolysis
080106* -- Hydrogen-- Production-- Biosynthesis & Photochemical Processes
14 SOLAR ENERGY
140505 -- Solar Energy Conversion-- Photochemical
Photobiological
& Thermochemical Conversion-- (1980-)
AZINES
BIPYRIDINES
CATHODES
ELECTROCHEMICAL CELLS
ELECTRODES
ELECTROLYSIS
ELECTROLYTIC CELLS
ELEMENTS
EQUIPMENT
HETEROCYCLIC COMPOUNDS
HYDROGEN PRODUCTION
INTERFACES
LYSIS
MATERIALS
ORGANIC COMPOUNDS
ORGANIC NITROGEN COMPOUNDS
P-TYPE CONDUCTORS
PHOTOCATHODES
PHOTOELECTROCHEMICAL CELLS
PHOTOELECTROLYSIS
PHOTOELECTROLYTIC CELLS
PYRIDINES
SEMICONDUCTOR MATERIALS
SEMIMETALS
SILICON
SOLAR EQUIPMENT