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Immobilization-Enabled Proton Reduction Catalysis by a Di-iron Hydrogenase Mimic

Sanabria-Chinchilla, Jean and Javier, Alnald and Crouthers, Danielle and Baricuatro, Jack H. and Darensbourg, Marcetta Y. and Soriaga, Manuel P. (2014) Immobilization-Enabled Proton Reduction Catalysis by a Di-iron Hydrogenase Mimic. Electrocatalysis, 5 (1). pp. 5-7. ISSN 1868-2529. https://resolver.caltech.edu/CaltechAUTHORS:20140211-073815565

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Abstract

We have long been interested in the influence of surface immobilization on the electrochemical integrity of redox-active moieties [1–5]. Our studies have shown that, if the electroactive group itself is directly chemisorbed on (coordinated to) the electrode surface, profound alterations result in both the thermodynamics and kinetics of the electron transfer processes; the oxidative chemisorption of the iodide anion (to zerovalent iodine atoms) or the hydroquinone molecule (to benzoquinone) are prototypical examples. The changes are more subtle and less dramatic if the electroactive site is only a pendant moiety tethered to the surface via an anchor group; mercapto hydroquinone bound exclusively via the –SH group is a well-known specimen. We recently extended our investigations to include enzyme-inspired molecular electrocatalysts in which the multinuclear reactive site may require a certain entatic state to carry out its catalytic function; the anticipation is that the motion-restricted surface-tethered species would suffer diminished catalytic activity. The results are described in this brief communication.


Item Type:Article
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http://link.springer.com/article/10.1007/s12678-013-0157-yPublisherArticle
http://dx.doi.org/10.1007/s12678-013-0157-yDOIArticle
http://dx.doi.org/10.1007/s12678-014-0188-zDOIAddendum
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ORCID:
AuthorORCID
Javier, Alnald0000-0002-0306-5462
Soriaga, Manuel P.0000-0002-0077-6226
Additional Information:© 2013 Springer Science+Business Media New York. Published online: 17 September 2013. This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, as follows: The electrocatalysis work was supported through the Office of Science of the U.S. Department of Energy under Award No. DE-SC0004993; the synthesis and characterization of the di-iron complexes were supported by the National Science Foundation (CHE-0616695) (MYD) and the Texas A&M University-CONACYT program (MPS).
Group:JCAP
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
NSFCHE-0616695
Texas A&M University-CONACYT ProgramUNSPECIFIED
Issue or Number:1
Record Number:CaltechAUTHORS:20140211-073815565
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20140211-073815565
Official Citation:Sanabria-Chinchilla, J., Javier, A., Crouthers, D. et al. Electrocatalysis (2014) 5: 5. doi:10.1007/s12678-013-0157-y
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:43761
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:11 Feb 2014 15:58
Last Modified:09 Mar 2020 13:18

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