Dynamics of photogenerated holes in surface modified α-Fe 2 O 3 photoanodes for solar water splitting | Zendy

Mónica Barroso | Zendy; Camilo A. Mesa | Zendy; Stephanie R. Pendlebury | Zendy; Alexander J. Cowan | Zendy; Takashi Hisatomi | Zendy; Kevin Sivula | Zendy; Michaël Grätzel | Zendy; David R. Klug | Zendy; James R. Durrant | Zendy

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Dynamics of photogenerated holes in surface modified α-Fe ₂ O ₃ photoanodes for solar water splitting

Author(s) -

Mónica Barroso,

Camilo A. Mesa,

Stephanie R. Pendlebury,

Alexander J. Cowan,

Takashi Hisatomi,

Kevin Sivula,

Michaël Grätzel,

David R. Klug,

James R. Durrant

Publication year - 2012

Publication title -

proceedings of the national academy of sciences

Language(s) - English

Resource type - Journals

SCImago Journal Rank - 5.011

H-Index - 771

eISSN - 1091-6490

pISSN - 0027-8424

DOI - 10.1073/pnas.1118326109

Subject(s) - overlayer , hematite , photocurrent , water splitting , electrocatalyst , surface states , passivation , materials science , electrode , photoelectrolysis , chemistry , chemical physics , inorganic chemistry , analytical chemistry (journal) , nanotechnology , electrochemistry , mineralogy , optoelectronics , photocatalysis , electrolysis , surface (topology) , electrolyte , catalysis , biochemistry , geometry , mathematics , layer (electronics) , chromatography

This paper addresses the origin of the decrease in the external electrical bias required for water photoelectrolysis with hematite photoanodes, observed following surface treatments of such electrodes. We consider two alternative surface modifications: a cobalt oxo/hydroxo-based (CoO(x)) overlayer, reported previously to function as an efficient water oxidation electrocatalyst, and a Ga(2)O(3) overlayer, reported to passivate hematite surface states. Transient absorption studies of these composite electrodes under applied bias showed that the cathodic shift of the photocurrent onset observed after each of the surface modifications is accompanied by a similar cathodic shift of the appearance of long-lived hematite photoholes, due to a retardation of electron/hole recombination. The origin of the slower electron/hole recombination is assigned primarily to enhanced electron depletion in the Fe(2)O(3) for a given applied bias.

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