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Adaptive semiconductor/electrocatalyst junctions in water-splitting photoanodes
Open accessAbstract
High-efficiency photoelectrochemical water-splitting devices require the integration of electrocatalysts (ECs) with light-absorbing semiconductors (SCs), but the energetics and charge-transfer processes at SC/EC interfaces are poorly understood. We fabricate model EC-coated single-crystal TiO2 electrodes and directly probe SC/EC interfaces in situ using two working electrodes to independently monitor and control the potential and current at both the SC and the EC. We discover that redox-active ion-permeable ECs such as Ni(OH)2 or NiOOH yield 'adaptive' SC/EC junctions where the effective Schottky barrier height changes in situ with the oxidation level of the EC. In contrast, dense, ion-impermeable IrOx ECs yield constant-barrier-height 'buried' junctions. Conversion of dense, thermally deposited NiOx on TiO2 into ion-permeable Ni(OH)2 or NiOOH correlated with increased apparent photovoltage and fill factor. These results provide new insight into the dynamic behaviour of SC/EC interfaces to guide the design of efficient SC/EC devices. They also illustrate a new class of adaptive semiconductor junctions.
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Cites
Electrochemical Photolysis of Water at a Semiconductor Electrode
FUJISHIMA, A., & HONDA, K. (1972) · Nature · doi:10.1038/238037a0 · Cited by 34,169
A realizable renewable energy future
Turner, J. A. (1999) · Science · doi:10.1126/science.285.5428.687 · Cited by 1,642
Cited by
Water photolysis at 12.3% efficiency via perovskite photovoltaics and Earth-abundant catalysts
Luo, J., Im, J.-H., Mayer, M. T., Schreier, M., Nazeeruddin, M. K., Park, N.-G., Tilley, S. D., Fan, H. J., & Grätzel, M. (2014) · Science · doi:10.1126/science.1258307 · Cited by 2,509
Transition‐Metal (Co, Ni, and Fe)‐Based Electrocatalysts for the Water Oxidation Reaction
Han, L., Dong, S., & Wang, E. (2016) · Advanced Materials · doi:10.1002/adma.201602270 · Cited by 1,769
Single atom tungsten doped ultrathin α-Ni(OH)2 for enhanced electrocatalytic water oxidation
Yan, J., Kong, L., Ji, Y., White, J., Li, Y., Zhang, J., An, P., Liu, S., Lee, S.-T., & Ma, T. (2019) · Nature Communications · doi:10.1038/s41467-019-09845-z · Cited by 561
Metadata
- Authors
- Lin, F., & Boettcher, S. W.
- Venue
- Nature Materials
- Published
- 2013-12-01
- Volume
- 13
- Issue
- 1
- Pages
- 81-86
- ISSN
- 1476-1122 (ISSN-L)
- 1476-4660
- OpenAlex
- W2165332053
- Cited by
- 490
- References
- 2
- FWCI
- 13.59
- Type
- journal article
- Language
- en
- Open access
- green
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