期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 116, 期 32, 页码 16870-16875出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp304254k
关键词
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资金
- European Community's Sixth Framework Marie Curie International Reintegration Program [042095]
- Seventh Framework Program Novel Materials for Energy Applications [227179]
- Swiss NSF [206021-121306, IZK0Z2-133944, 200021-132126]
- European Research Council [ERC-2010-MG 267816 Li-Lo]
- Swiss Federal Office of Energy [152316-101883, 153613-102809]
- Office of Science/BES, of the U.S. DoE [DE-AC02-05CH11231]
- Natural Science Foundation of China [20873128]
- National Basic Research Program of China [2010CB923302]
- Hundred Talents Program of the Chinese Academy of Sciences
- Swiss National Science Foundation (SNF) [IZK0Z2_133944] Funding Source: Swiss National Science Foundation (SNF)
Visible light active photoelectrodes for hydrogen generation by solar photoelectrochemical water splitting have been under scrutiny for many decades. In particular, the role of electron holes and charge transfer remains controversial. We have investigated the oxygen evolution of hematite in alkaline aqueous electrolyte under a bias potential during visible light illumination in a photoelectrochemical cell operando with soft X-ray (O 1s) spectroscopy. Only under these conditions, two new spectral signatures evolve in the valence band, which we identify as an O 2p hole transition into the charge transfer band and an Fe 3d type hole into the upper Hubbard band. Quantitative analysis of their spectral weight and comparison with the photocurrent reveals that both types of holes, contrary to earlier speculations and common perception, contribute to the photocurrent.
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