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Synthesis of Chemicals Using Solar Energy with Stable Photoelectrochemically Active Heterostructures
Journal article   Peer reviewed

Synthesis of Chemicals Using Solar Energy with Stable Photoelectrochemically Active Heterostructures

Syed Mubeen, Nirala Singh, Joun Lee, Galen D Stucky, Martin Moskovits and Eric W Mcfarland
Nano letters, Vol.13(5), pp.2110-2115
2013
DOI: 10.1021/nl400502u
PMID: 23586680
url
https://escholarship.org/uc/item/73w777jmView
Open Access

Abstract

Efficient and cost-effective conversion of solar energy to useful chemicals and fuels could lead to a significant reduction in fossil hydrocarbon use. Artificial systems that use solar energy to produce chemicals have been reported for more than a century. However the most efficient devices demonstrated, based on traditionally fabricated compound semiconductors, have extremely short working lifetimes due to photocorrosion by the electrolyte. Here we report a stable, scalable design and molecular level fabrication strategy to create photoelectrochemically active heterostructure (PAH) units consisting of an efficient semiconductor light absorber in contact with oxidation and reduction electrocatalysts and otherwise protected by alumina. The functional heterostructures are fabricated by layer-by-layer, template-directed, electrochemical synthesis in porous anodic aluminum oxide membranes to produce high density arrays of electronically autonomous, nanostructured, corrosion resistant, photoactive units (~10(9)-10(10) PAHs per cm(2)). Each PAH unit is isolated from its neighbor by the transparent electrically insulating oxide cellular enclosure that makes the overall assembly fault tolerant. When illuminated with visible light, the free floating devices have been demonstrated to produce hydrogen at a stable rate for over 24 h in corrosive hydroiodic acid electrolyte with light as the only input. The quantum efficiency (averaged over the solar spectrum) for absorbed photons-to-hydrogen conversion was 7.4% and solar-to-hydrogen energy efficiency of incident light was 0.9%. The fabrication approach is scalable for commercial manufacturing and readily adaptable to a variety of earth abundant semiconductors which might otherwise be unstable as photoelectrocatalysts.
Materials Science Physics Chemical synthesis methods Condensed matter: structure, mechanical and thermal properties Cross-disciplinary physics: materials science; rheology Exact sciences and technology Low-dimensional structures (superlattices, quantum well structures, multilayers): structure, and nonelectronic properties Methods of nanofabrication Surfaces and interfaces; thin films and whiskers (structure and nonelectronic properties)

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