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Enhanced Photochemical Hydrogen Production by a Molecular Diiron Catalyst Incorporated into a Metal–Organic Framework
Open accessAbstract
A molecular proton reduction catalyst [FeFe](dcbdt)(CO)6 (1, dcbdt = 1,4-dicarboxylbenzene-2,3-dithiolate) with structural similarities to [FeFe]-hydrogenase active sites has been incorporated into a highly robust Zr(IV)-based metal-organic framework (MOF) by postsynthetic exchange (PSE). The PSE protocol is crucial as direct solvothermal synthesis fails to produce the functionalized MOF. The molecular integrity of the organometallic site within the MOF is demonstrated by a variety of techniques, including X-ray absorption spectroscopy. In conjunction with [Ru(bpy)3](2+) as a photosensitizer and ascorbate as an electron donor, MOF-[FeFe](dcbdt)(CO)6 catalyzes photochemical hydrogen evolution in water at pH 5. The immobilized catalyst shows substantially improved initial rates and overall hydrogen production when compared to a reference system of complex 1 in solution. Improved catalytic performance is ascribed to structural stabilization of the complex when incorporated in the MOF as well as the protection of reduced catalysts 1(-) and 1(2-) from undesirable charge recombination with oxidized ascorbate.
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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
Metal-organic framework materials as catalysts
Lee, J., Farha, O. K., Roberts, J., Scheidt, K. A., Nguyen, S. T., & Hupp, J. T. (2009) · Chemical Society Reviews · doi:10.1039/b807080f · Cited by 7,969
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Xu, H.-Q., Hu, J., Wang, D., Li, Z., Zhang, Q., Luo, Y., Yu, S.-H., & Jiang, H.-L. (2015) · Journal of the American Chemical Society · doi:10.1021/jacs.5b08773 · Cited by 1,166
Single Pt Atoms Confined into a Metal–Organic Framework for Efficient Photocatalysis
Fang, X., Shang, Q., Wang, Y., Jiao, L., Yao, T., Li, Y., Zhang, Q., Luo, Y., & Jiang, H. (2018) · Advanced Materials · doi:10.1002/adma.201705112 · Cited by 837
When defects turn into virtues: The curious case of zirconium-based metal-organic frameworks
Taddei, M. (2017) · Coordination Chemistry Reviews · doi:10.1016/j.ccr.2017.04.010 · Cited by 341
Shi, D., Zheng, R., Sun, M., Cao, X., Sun, C., Cui, C., Liu, C., Zhao, J., & Du, M. (2017) · Angewandte Chemie International Edition · doi:10.1002/anie.201709869 · Cited by 308
Metadata
- Authors
- Pullen, S., Fei, H., Orthaber, A., Cohen, S. M., & Ott, S.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2013-10-31
- Volume
- 135
- Issue
- 45
- Pages
- 16997-17003
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2024564951
- Cited by
- 535
- References
- 2
- FWCI
- 19.84
- Type
- journal article
- Language
- en
- Open access
- hybrid
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- Pullen, S., Fei, H., Orthaber, A., Cohen, S. M., & Ott, S. (2013). Enhanced Photochemical Hydrogen Production by a Molecular Diiron Catalyst Incorporated into a Metal–Organic Framework. Journal of the American Chemical Society. https://doi.org/10.1021/ja407176p
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