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Cobalt-dithiolene complexes for the photocatalytic and electrocatalytic reduction of protons in aqueous solutions
Open accessAbstract
Artificial photosynthesis (AP) is a promising method of converting solar energy into fuel (H 2 ). Harnessing solar energy to generate H 2 from H + is a crucial process in systems for artificial photosynthesis. Widespread application of a device for AP would rely on the use of platinum-free catalysts due to the scarcity of noble metals. Here we report a series of cobalt dithiolene complexes that are exceptionally active for the catalytic reduction of protons in aqueous solvent mixtures. All catalysts perform visible-light-driven reduction of protons from water when paired with as the photosensitizer and ascorbic acid as the sacrificial donor. Photocatalysts with electron withdrawing groups exhibit the highest activity with turnovers up to 9,000 with respect to catalyst. The same complexes are also active electrocatalysts in 1∶1 acetonitrile/water. The electrocatalytic mechanism is proposed to be ECEC, where the Co dithiolene catalysts undergo rapid protonation once they are reduced to . Subsequent reduction and reaction with H + lead to H 2 formation. Cobalt dithiolene complexes thus represent a new group of active catalysts for the reduction of protons.
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Citations
Cites
A Cobalt–Dithiolene Complex for the Photocatalytic and Electrocatalytic Reduction of Protons
McNamara, W. R., Han, Z., Alperin, P. J., Brennessel, W. W., Holland, P. L., & Eisenberg, R. (2011) · Journal of the American Chemical Society · doi:10.1021/ja207842r · Cited by 398
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Cited by
Robust Photogeneration of H 2 in Water Using Semiconductor Nanocrystals and a Nickel Catalyst
Han, Z., Qiu, F., Eisenberg, R., Holland, P. L., & Krauss, T. D. (2012) · Science · doi:10.1126/science.1227775 · Cited by 771
Self-citationEarth-abundant hydrogen evolution electrocatalysts
McKone, J. R., Marinescu, S. C., Brunschwig, B. S., Winkler, J. R., & Gray, H. B. (2014) · Chem. Sci. · doi:10.1039/c3sc51711j · Cited by 727
Thoi, V. S., Sun, Y., Long, J. R., & Chang, C. J. (2013) · Chem. Soc. Rev. · doi:10.1039/c2cs35272a · Cited by 668
Metal-complex chromophores for solar hydrogen generation
Yuan, Y.-J., Yu, Z.-T., Chen, D.-Q., & Zou, Z.-G. (2017) · Chemical Society Reviews · doi:10.1039/c6cs00436a · Cited by 423
Nickel Complexes for Robust Light-Driven and Electrocatalytic Hydrogen Production from Water
Das, A., Han, Z., Brennessel, W. W., Holland, P. L., & Eisenberg, R. (2015) · ACS Catalysis · doi:10.1021/acscatal.5b00045 · Cited by 258
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Metadata
- Authors
- McNamara, W. R., Han, Z., Yin, C.-J. (., Brennessel, W. W., Holland, P. L., & Eisenberg, R.
- Venue
- Proceedings of the National Academy of Sciences
- Published
- 2012-06-12
- Volume
- 109
- Issue
- 39
- Pages
- 15594-15599
- ISSN
- 0027-8424 (ISSN-L)
- 1091-6490
- OpenAlex
- W2162029871
- Cited by
- 296
- References
- 1
- FWCI
- 11.78
- Type
- journal article
- Language
- en
- Open access
- bronze
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- McNamara, W. R., Han, Z., Yin, C.-J. (., Brennessel, W. W., Holland, P. L., & Eisenberg, R. (2012). Cobalt-dithiolene complexes for the photocatalytic and electrocatalytic reduction of protons in aqueous solutions. Proceedings of the National Academy of Sciences. https://doi.org/10.1073/pnas.1120757109
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