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Noncovalent Immobilization of Electrocatalysts on Carbon Electrodes for Fuel Production

Blakemore, James D. and Gupta, Ayush and Warren, Jeffrey J. and Brunschwig, Bruce S. and Gray, Harry B. (2013) Noncovalent Immobilization of Electrocatalysts on Carbon Electrodes for Fuel Production. Journal of the American Chemical Society, 135 (49). pp. 18288-18291. ISSN 0002-7863. http://resolver.caltech.edu/CaltechAUTHORS:20131203-150617731

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Abstract

We show that molecular catalysts for fuel-forming reactions can be immobilized on graphitic carbon electrode surfaces via noncovalent interactions. A pyrene-appended bipyridine ligand (P) serves as the linker between each complex and the surface. Immobilization of a rhodium proton-reduction catalyst, [Cp*Rh(P)Cl]Cl (1), and a rhenium CO_2-reduction catalyst, Re(P)(CO)_3Cl (2), afford electrocatalytically active assemblies. X-ray photoelectron spectroscopy and electrochemistry confirm catalyst immobilization. Reduction of 1 in the presence of p-toluenesulfonic acid results in catalytic H_2 production, while reduction of 2 in the presence of CO_2 results in catalytic CO production.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/ja4099609DOIArticle
http://pubs.acs.org/doi/abs/10.1021/ja4099609PublisherArticle
ORCID:
AuthorORCID
Blakemore, James D.0000-0003-4172-7460
Brunschwig, Bruce S.0000-0002-6135-6727
Additional Information:© 2013 American Chemical Society. Received: September 26, 2013. Publication Date (Web): November 18, 2013. The authors thank Peter Agbo for helpful discussions regarding surface preparation and David Lacy for assistance with the GC product analysis. Research was carried out in part at the Molecular Materials Research Center of the Beckman Institute at Caltech. This work was supported by the NSF CCI Solar Fuels Program (CHE-1305124) and a CCI Postdoctoral Fellowship to J.D.B.
Group:CCI Solar Fuels
Funders:
Funding AgencyGrant Number
NSFCHE-1305124
NSF Postdoctoral FellowshipUNSPECIFIED
Record Number:CaltechAUTHORS:20131203-150617731
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20131203-150617731
Official Citation:Noncovalent Immobilization of Electrocatalysts on Carbon Electrodes for Fuel Production James D. Blakemore, Ayush Gupta, Jeffrey J. Warren, Bruce S. Brunschwig, and Harry B. Gray Journal of the American Chemical Society 2013 135 (49), 18288-18291
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:42806
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:03 Dec 2013 23:42
Last Modified:05 Sep 2017 22:29

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