Electrochemical characterization of surface-bound redox polymers derived from 1,1'-bis(((3-(triethoxysilyl)propyl)amino)carbonyl)cobaltocenium: charge transport, anion binding, and use in photoelectrochemical hydrogen generation
This paper describes the behavior of electrode-bound redox material derived from the hydrolysis of the -Si(OEt)/sub 3/ groups of 1,1'-bis(((3-(triethoxysilyl)propyl)amino)carbonyl)cobaltocenium (I). Surfaces of the conventional electrodes SnO/sub 2/ and Pt derivatized with I have a reversible electrochemical response in H/sub 2/O/electrolyte; the E/sup 0/' is pH independent at -0.62 V vs. SCE. The photoelectrochemical behavior of p-type Si photocathodes derivatized with I reveals that the photoreduction of the cobaltocenium derivative can be effected at an electrode potential approx. 500 mV more positive than on metallic electrodes, consistent with the known behavior of p-type Si photocathodes. When polymer from I is deposited on p-type Si and subsequently coated with a small amount of Rh or Pd (approx. 10/sup -7/ mol/cm/sup 2/), the photoelectrochemical generation of H/sub 2/ is possible with 632.8-nm (approx. 15 mW/cm/sup 2/) radiation and efficiencies in the vicinity of 2%. The polymer derived from I is more optically transparent and more durable at negative potentials than redox polymers derived from vilogen monomers. Potential-step measurements and steady-state-current measurements for mediated redox processes show that the charge-transport rate for the polymer derived from I is about the same as for polymers from viologen monomers. 32 references, 8 figures.
- Research Organization:
- Massachusetts Institute of Technology, Cambridge
- OSTI ID:
- 6007400
- Journal Information:
- Inorg. Chem.; (United States), Journal Name: Inorg. Chem.; (United States) Vol. 24:20; ISSN INOCA
- Country of Publication:
- United States
- Language:
- English
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Related Subjects
080102* -- Hydrogen-- Production-- Thermochemical Processes
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
400500 -- Photochemistry
ANIONS
CHARGE TRANSPORT
CHARGED PARTICLES
CHEMICAL REACTIONS
CHEMISTRY
COBALT COMPOUNDS
DATA
DECOMPOSITION
DERIVATIZATION
EFFICIENCY
ELECTROCHEMICAL CELLS
ELECTROCHEMISTRY
ELECTRODES
EQUIPMENT
EXPERIMENTAL DATA
HYDROGEN PRODUCTION
HYDROLYSIS
INFORMATION
IONS
LYSIS
NUMERICAL DATA
PH VALUE
PHOTOCHEMICAL REACTIONS
PHOTOELECTROCHEMICAL CELLS
POLYMERS
REDOX REACTIONS
SOLAR EQUIPMENT
SOLVOLYSIS
SURFACES
TRANSITION ELEMENT COMPOUNDS