NDLI: Synthesis, photoelectrochemical properties, and first principles study of n-type CuW1−xMoxO4 electrodes showing enhanced visible light absorption

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Energy & Environmental Science Vol - 6 Issue - 7

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Synthesis, photoelectrochemical properties, and first principles study of n-type CuW_1−xMo_xO₄ electrodes showing enhanced visible light absorption

Content Provider	Royal Society of Chemistry (RSC)
Author	Galli, Giulia A. Ping, Yuan Hill, James C. Choi, Kyoung-Shin
Copyright Year	2013
Abstract	Molybdenum-rich solid solutions of CuWO4 and CuMoO4 (i.e., CuW1−xMoxO4, x > 0.4) having a wolframite structure were prepared as thin-film type electrodes using a new electrochemical route. The synthesis of Mo-rich CuW1−xMoxO4 was not previously achieved because the CuMoO4 phase that is isostructural to CuWO4 is not thermodynamically stable. The resulting solid solution, CuW0.35Mo0.65O4, exhibited a significantly reduced optical bandgap (Eg = 2.0 eV), compared to CuWO4 (Eg = 2.3 eV). Since both CuW0.35Mo0.65O4 and CuWO4 are n-type semiconductors, their photoelectrochemical properties were compared for possible use as photoanodes in water splitting photoelectrochemical cells. CuW1−xMoxO4 showed enhanced photon absorption not only in the 2.0 eV ≤ E ≤ 2.3 eV region but also above 2.3 eV, compared to CuWO4, which directly resulted in enhanced photocurrent generation. Ab initio calculations were performed to understand the origin of the bandgap reduction by Mo incorporation. The calculations showed that the conduction band edge of CuWO4 is mainly composed of W 5d and O 2p hybrid orbitals. Therefore, when Mo atoms with 4d orbitals, which are lower in energy than W 5d orbitals, occupy W sites, the conduction band edge is shifted to lower energy. These results suggest that there may be many unexplored new compositions in ternary oxide systems that possess ideal bandgap energies for solar energy conversion.
Starting Page	2440
Ending Page	2446
Page Count	7
File Format	HTM / HTML PDF
ISSN	17545692
Volume Number	6
Issue Number	8
Journal	Energy & Environmental Science
DOI	10.1039/c3ee40827b
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Mo Wolframite Electrochemistry Solid solution Band gap Electronvolt Extrinsic semiconductor Photoelectrochemical cell Water splitting Photon Photocurrent Ab initio Valence and conduction bands Solar energy
Content Type	Text
Resource Type	Article
Subject	Environmental Chemistry Pollution Renewable Energy, Sustainability and the Environment Nuclear Energy and Engineering

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