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Adsorption/Deposition of the Ligands 9,10-Phenanthroline-5,6-dione and 9,10-Phenanthroline-5,6-diol and Their Metal Complexes on Pyrolytic Graphite Electrodes

Shi, Minglian and Anson, Fred C. (1998) Adsorption/Deposition of the Ligands 9,10-Phenanthroline-5,6-dione and 9,10-Phenanthroline-5,6-diol and Their Metal Complexes on Pyrolytic Graphite Electrodes. Analytical Chemistry, 70 (8). pp. 1489-1495. ISSN 0003-2700. https://resolver.caltech.edu/CaltechAUTHORS:20170913-084950345

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Abstract

Metal complexes of the electroactive ligand 9,10-phenanthroline-5,6-dione (pdon) are receiving extensive study because of their demonstrated potential as electrocatalysts for the oxidation of NADH and other substrates. In aqueous media, the reduced ligand, 9,10-phenanthroline-5,6-diol (pdol), and its complexes with transition metals are only slightly soluble and tend to accumulate on the surfaces of electrodes, where they are generated by reduction of pdon. The adsorbed (or precipitated) molecular layers can interfere with the continued electroreduction of the more soluble, oxidized precursors from which they are generated. The use of freshly cleaved basal plane pyrolytic graphite electrodes allowed the surface coordination chemistry and electrochemistry of pdon, pdol, and their complexes to be inspected in more detail than in previous studies. The results revealed several general trends:  (i) Coordination of pdon to transition metals shifts its reduction potential to more positive values. (ii) The affinity of the dipositive form of transition metal redox couples for pdon is greater than that of the tripositive form by a factor that exceeds the corresponding affinities for 9,10-phenanthroline. (iii) Pdol and its complexes are much less soluble in aqueous media than are pdon and its complexes. (iv) Complexes of pdon are much less strongly adsorbed on graphite than is the free ligand in both its protonated and unprotonated forms.


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https://doi.org/10.1021/ac971234cDOIArticle
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Additional Information:© 1998 American Chemical Society. Received for review November 12, 1997. Accepted January 28, 1998. Publication Date (Web): March 13, 1998. This work was supported by the National Science Foundation. We appreciated receiving a copy of ref 12 prior to publication and helpful discussions with Prof. E. Steckhan and Dr. G. Hilt.
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Issue or Number:8
Record Number:CaltechAUTHORS:20170913-084950345
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170913-084950345
Official Citation:Adsorption/Deposition of the Ligands 9,10-Phenanthroline-5,6-dione and 9,10-Phenanthroline-5,6-diol and Their Metal Complexes on Pyrolytic Graphite Electrodes. Minglian Shi and and Fred C. Anson. Analytical Chemistry 1998 70 (8), 1489-1495 DOI: 10.1021/ac971234c
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:81400
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:14 Sep 2017 22:22
Last Modified:03 Oct 2019 18:42

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