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Strengthening reactive metal-support interaction to stabilize high-density Pt single atoms on electron-deficient g-C3N4 for boosting photocatalytic H2 production
Open accessAbstract
Abstract Tuning reactive metal-support interaction (RMSI) is a promising approach to optimizing catalytic active sites via the electronic, geometric and compositional effects. In general, the RMSI is conducted on the reducible oxides via a high-temperature reaction (>550 °C). Herein we report a strong RMSI between Pt single atom (PtSA) and non-oxide-based g-C3N4 built by an in-situ photocatalytic reduction method at a sub-zero temperature. The experimental observation confirms that the rich N vacancies in g-C3N4 produce an obvious electron-deficient effect, which greatly enhances the RMSI. This strong RMSI contributes to the highest PtSA coverage density of 0.35 mg m−2 reported to date in carbon-based materials and outstanding H2-evolution activity of 174.5 mmol g−1 h−1 per PtSA relative to those on the electron-rich g-C3N4. The structure simulation reveals that the RMSI can not only stabilize the PtSA on the electron-deficient g-C3N4 via the strong chemical bond between PtSA and the two-coordinated C (C2C) sites caused by the N vacancies, but also promises the PtSA with an optimized electronic and geometric structures for capturing photogenerated electrons and producing H2. This finding opens a new channel for designing and manipulating single atom-loaded photocatalyst via the RMSI at a sub-zero low temperature.
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Noble-metal single-atoms in thermocatalysis, electrocatalysis, and photocatalysis
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Metadata
- Authors
- Zhou, P., Lv, F., Li, N., Zhang, Y., Mu, Z., Tang, Y., Lai, J., Chao, Y., Luo, M., Lin, F., Zhou, J., Su, D., & Guo, S.
- Venue
- Nano Energy
- Publisher
- Elsevier BV
- Published
- 2019-02
- Volume
- 56
- Pages
- 127-137
- ISSN
- 2211-2855 (ISSN-L)
- OpenAlex
- W2900857781
- Cited by
- 344
- References
- 35
- FWCI
- 7.41
- Type
- journal article
- Language
- en
- Open access
- green
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- Zhou, P., Lv, F., Li, N., Zhang, Y., Mu, Z., Tang, Y., Lai, J., Chao, Y., Luo, M., Lin, F., Zhou, J., Su, D., & Guo, S. (2019). Strengthening reactive metal-support interaction to stabilize high-density Pt single atoms on electron-deficient g-C3N4 for boosting photocatalytic H2 production. Nano Energy. https://doi.org/10.1016/j.nanoen.2018.11.033
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