Efficient direct solar-to-hydrogen conversion by in situ interface transformation of a tandem structure
Abstract
Photosynthesis is nature's route to convert intermittent solar irradiation into storable energy, while its use for an industrial energy supply is impaired by low efficiency. Artificial photosynthesis provides a promising alternative for efficient robust carbon-neutral renewable energy generation. The approach of direct hydrogen generation by photoelectrochemical water splitting utilizes customized tandem absorber structures to mimic the Z-scheme of natural photosynthesis. Here a combined chemical surface transformation of a tandem structure and catalyst deposition at ambient temperature yields photocurrents approaching the theoretical limit of the absorber and results in a solar-to-hydrogen efficiency of 14%. The potentiostatically assisted photoelectrode efficiency is 17%. Present benchmarks for integrated systems are clearly exceeded. Details of the in situ interface transformation, the electronic improvement and chemical passivation are presented. The surface functionalization procedure is widely applicable and can be precisely controlled, allowing further developments of high-efficiency robust hydrogen generators.
Additional Information
© 2015 Macmillan Publishers Limited. This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. Received 4 Feb 2015; Accepted 7 Aug 2015; Published 15 Sep 2015. We are grateful for support by R. van de Krol and for experimental support by M. Kernbach and H. Kriegel. M. Niemeyer, C. Karcher and J. Ohlmann supported the solar cell development. K. Harbauer and T. Münchenberg assisted with ohmic contact preparation. U. Bloeck performed the TEM measurements, S. Brunken provided the RuO2 counter electrode. We also thank P. Bogdanoff, K. Fountaine and C. McCrory for helpful discussions. M.M.M. acknowledges a scholarship by the Studienstiftung des deutschen Volkes and H.-J.L. acknowledges support by the DFG (project Nr. 1192-3/4). The discussion and interpretation of the data, feedback with experimentation as well as article layout and writing was also supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under Award Number DE-SC0004993. Contributions: T.H., H.-J.L. and M.M.M. designed the study. M.M.M. executed the experiments and did the data analysis. D.L. and F.D. prepared the tandem absorber. M.M.M. and H.J.L. wrote the paper and all authors commented on the manuscript. The authors declare no competing financial interests.Attached Files
Published - ncomms9286.pdf
Supplemental Material - ncomms9286-s1.pdf
Files
| Name | Size | Download all |
|---|---|---|
|
md5:38ec13ad4baa9440fd5a2f4ff1ea3167
|
414.1 kB | Preview Download |
|
md5:2cb2c01aebbc7cdde48cbd88604c75dd
|
1.5 MB | Preview Download |
Additional details
- PMCID
- PMC4579846
- Eprint ID
- 61885
- Resolver ID
- CaltechAUTHORS:20151105-084800992
- Studienstiftung des deutschen Volkes
- 1192-3/4
- Deutsche Forschungsgemeinschaft (DFG)
- DE-SC0004993
- Department of Energy (DOE)
- Created
-
2015-11-05Created from EPrint's datestamp field
- Updated
-
2022-05-23Created from EPrint's last_modified field
- Caltech groups
- JCAP