The Nature of Photocatalytic “Water Splitting” on Silicon Nanowires†
Dong Liu
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
These authors contributed equally to this work.
Search for more papers by this authorLeilei Li
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
These authors contributed equally to this work.
Search for more papers by this authorYang Gao
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
Search for more papers by this authorDr. Chengming Wang
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
Search for more papers by this authorProf. Jun Jiang
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
Search for more papers by this authorCorresponding Author
Prof. Yujie Xiong
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/Search for more papers by this authorDong Liu
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
These authors contributed equally to this work.
Search for more papers by this authorLeilei Li
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
These authors contributed equally to this work.
Search for more papers by this authorYang Gao
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
Search for more papers by this authorDr. Chengming Wang
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
Search for more papers by this authorProf. Jun Jiang
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
Search for more papers by this authorCorresponding Author
Prof. Yujie Xiong
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/
Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials, and School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026 (P. R. China) http://staff.ustc.edu.cn/∼yjxiong/Search for more papers by this authorThis work was financially supported by the 973 Program (No. 2014CB848900), NSFC (No. 91123010, 21471141, 21101145, 21473166), Recruitment Program of Global Experts, CAS Hundred Talent Program, Specialized Research Fund for the Doctoral Program of Higher Education (No. 20123402110050), Fundamental Research Funds for the Central Universities (No. WK2060190025, WK2310000035), and Beijing National Laboratory for Molecular Sciences (2013002).
Abstract
Silicon should be an ideal semiconductor material if it can be proven usable for photocatalytic water splitting, given its high natural abundance. Thus it is imperative to explore the possibility of water splitting by running photocatalysis on a silicon surface and to decode the mechanism behind it. It is reported that hydrogen gas can indeed be produced from Si nanowires when illuminated in water, but the reactions are not a real water-splitting process. Instead, the production of hydrogen gas on the Si nanowires occurs through the cleavage of SiH bonds and the formation of SiOH bonds, resulting in the low probability of generating oxygen. On the other hand, these two types of surface dangling bonds both extract photoexcited electrons, whose competition greatly impacts on carrier lifetime and reaction efficiency. Thus surface chemistry holds the key to achieving high efficiency in such a photocatalytic system.
Supporting Information
As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors.
| Filename | Description |
|---|---|
| ange_201411200_sm_miscellaneous_information.pdf3.3 MB | miscellaneous_information |
Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.
References
- 1I. Oh, J. Kye, S. Hwang, Nano Lett. 2012, 12, 298.
- 2C. Liu, J. Tang, H. M. Chen, B. Liu, P. Yang, Nano Lett. 2013, 13, 2989.
- 3A. L. Linsebigler, G. Lu, J. T. Yates, Jr., Chem. Rev. 1995, 95, 735.
- 4M. Shao, L. Cheng, X. Zhang, D. D. D. Ma, S. T. Lee, J. Am. Chem. Soc. 2009, 131, 17738.
- 5Z. H. Chen, Y. B. Tang, Y. Liu, Z. H. Kang, X. J. Zhang, X. Fan, C. S. Lee, I. Bello, W. J. Zhang, S. T. Lee, J. Appl. Phys. 2009, 105, 034307.
- 6F. Y. Wang, Q. D. Yang, G. Xu, N. Y. Lei, Y. K. Tsang, N. B. Wong, J. C. Ho, Nanoscale 2011, 3, 3269.
- 7N. Megouda, Y. Cofininier, S. Szunerits, T. Hadjersi, O. Elkechai, R. Boukherroub, Chem. Commun. 2011, 47, 991.
- 8S. Lian, C. H. A. Tsang, Z. Kang, Y. Liu, N. Wong, S. T. Lee, Mater. Res. Bull. 2011, 46, 2441.
- 9Y. M. A. Yamada, Y. Yuyama, T. Sato, S. Fujikawa, Y. Uozumi, Angew. Chem. Int. Ed. 2014, 53, 127; Angew. Chem. 2014, 126, 131.
- 10R. Q. Zhang, X. M. Liu, Z. Wen, Q. Jiang, J. Phys. Chem. C 2011, 115, 3425.
- 11K. Onda, B. Li, J. Zhao, K. D. Jordan, J. L. Yang, H. Petek, Science 2005, 308, 1154.
- 12Y. Wang, H. J. Sun, S. J. Tan, H. Feng, Z. W. Cheng, J. Zhao, A. D. Zhao, B. Wang, Y. Luo, J. L. Yang, J. G. Hou, Nat. Commun. 2013, 4, 2214.
- 13C. Xu, W. Yang, Q. Guo, D. Dai, M. Chen, X. Yang, J. Am. Chem. Soc. 2014, 136, 602.
- 14M. L. Zhang, K. Q. Peng, X. Fan, J. S. Jie, R. Q. Zhang, S. T. Lee, N. B. Wong, J. Phys. Chem. C 2008, 112, 4444.
- 15K. Q. Peng, Y. Wu, H. Fang, X. Y. Zhong, Y. Xu, J. Zhu, Angew. Chem. Int. Ed. 2005, 44, 2737; Angew. Chem. 2005, 117, 2797.
- 16Z. Huang, X. Zhang, M. Reiche, L. Liu, W. Lee, T. Shimizu, S. Senz, U. Gosele, Nano Lett. 2008, 8, 3046.
- 17C. Peng, J. Gao, S. Wang, X. Zhang, X. Zhang, X. Sun, J. Phys. Chem. C 2011, 115, 3866.
- 18J. S. DuChene, B. C. Sweeny, A. C. Johnston-Peck, D. Su, E. A. Stach, W. D. Wei, Angew. Chem. Int. Ed. 2014, 53, 7887; Angew. Chem. 2014, 126, 8021.
- 19Y. C. Pu, G. Wang, K. D. Chang, Y. Ling, Y. K. Lin, B. C. Fitzmorris, C. M. Liu, X. Lu, Y. Tong, J. Z. Zhang, Y. J. Tsu, Y. Li, Nano Lett. 2013, 13, 3817.
- 20J. Bisquert, A. Zaban, M. Greenshtein, I. Mora-Seró, J. Am. Chem. Soc. 2004, 126, 13550.
- 21X. H. Sun, S. D. Wang, N. B. Wong, D. D. D. Ma, S. T. Lee, B. K. Teo, Inorg. Chem. 2003, 42, 2398.
- 22W. Theiß, Surf. Sci. Rep. 1997, 29, 91.
- 23D. J. Michalak, S. R. Amy, A. Estève, Y. J. Chabal, J. Phys. Chem. C 2008, 112, 11907.
- 24D. J. Michalak, S. R. Amy, D. Aureau, M. Dai, A. Estève, Y. J. Chabal, Nat. Mater. 2010, 9, 266.
- 25K. A. Perrine, A. V. Teplyakov, Chem. Soc. Rev. 2010, 39, 3256.
- 26M. Marini, S. De Niederhausern, R. Iseppi, M. Bondi, C. Sabia, M. Toselli, F. Pilati, Biomacromolecules 2007, 8, 1246.
- 27M. V. Wolkin, J. Jorne, P. M. Fauchet, G. Allan, C. Delerue, Phys. Rev. Lett. 1999, 82, 197.
- 28G. Kresse, J. Furthmüller, Phys. Rev. B 1996, 54, 11169.
- 29H. Raza, Phys. Rev. B 2007, 76, 045308.
- 30F. Bianco, D. R. Bowler, J. H. G. Owen, S. A. Köster, M. Longobardi, C. Renner, ACS Nano 2013, 7, 4422.
- 31H. Dau, C. Limber, T. Reier, M. Risch, S. Roggan, P. Strasser, ChemCatChem 2010, 2, 724.
- 32Y. Xia, J. A. Rogers, K. E. Paul, G. M. Whitesides, Chem. Rev. 1999, 99, 1823.
- 33C. Hu, T. Peng, X. Hu, Y. Nie, X. Zhou, J. Qu, H. He, J. Am. Chem. Soc. 2010, 132, 857.
Citing Literature
This is the
German version
of Angewandte Chemie.
Note for articles published since 1962:
Do not cite this version alone.
Take me to the International Edition version with citable page numbers, DOI, and citation export.
We apologize for the inconvenience.
