期刊
ACS APPLIED MATERIALS & INTERFACES
卷 8, 期 15, 页码 10038-10047出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.6b01557
关键词
photoelectrochemistry; hydrogen production; cobaloxime; gallium phosphide; polyvinylimidazole; solar fuels
资金
- College of Liberal Arts and Sciences at Arizona State University
- Biodesign Institute Center for Applied Structural Discovery (CASD)
- IGERT-SUN fellowship - National Science Foundation [1144616]
- Arizona State University College of Liberal Arts and Sciences (CLAS) Undergraduate Summer Enrichment program
We report the immobilization of hydrogen-producing cobaloxime catalysts onto p-type gallium phosphide (111)A and (111)B substrates via coordination to a surface-grafted polyvinylimidazole brush. Successful grafting of the polymeric interface and subsequent assembly of cobalt-containing catalysts are confirmed using grazing angle attenuated total reflection Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. Photoelectrochemical testing in aqueous conditions at neutral pH shows that cobaloxime modification of either crystal face yields a similar enhancement of photoperformance, achieving a greater than 4-fold increase in current density and associated rates of hydrogen production as compared to results obtained using unfunctionalized electrodes tested under otherwise identical conditions. Under simulated solar illumination (100 mW cm(-2)), the catalyst-modified photocathodes achieve a current density approximate to 1 mA cm(-2) when polarized at 0 V vs the reversible hydrogen electrode reference and show near-unity Faradaic efficiency for hydrogen production as determined by gas chromatography analysis of the headspace. This work illustrates the modularity and versatility of the catalyst-polymer-semiconductor approach for directly coupling light harvesting to fuel production and the ability to export this chemistry across distinct crystal face orientations.
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