Electrochemistry at a Metal Nanoparticle on a Tunneling Film: A Steady-State Model of Current Densities at a Tunneling Ultramicroelectrode
Here, a new methodology is proposed for treating electrochemical current densities in metal-insulator-metal nanoparticle (M-I-MNP) systems. The described model provides broad, practical insights about MNP-mediated electron transfer to redox species in solution, where electron transfer from the under...
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| Published in: | Journal of the American Chemical Society Vol. 137; no. 35; pp. 11321 - 11326 |
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| Main Authors: | , , |
| Format: | Journal Article |
| Language: | English |
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United States
American Chemical Society
09-09-2015
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| Abstract | Here, a new methodology is proposed for treating electrochemical current densities in metal-insulator-metal nanoparticle (M-I-MNP) systems. The described model provides broad, practical insights about MNP-mediated electron transfer to redox species in solution, where electron transfer from the underlying electrode to a MNP via tunneling and heterogeneous electron transfer from the MNP to redox species in solution are treated as sequential steps. Tunneling is treated through an adaptation of the Simmons model of tunneling in metal–insulator–metal structures, and explicit equations are provided for tunneling currents, which demonstrate the effect of various experimental parameters, such as insulator thickness and MNP size. Overall, a general approach is demonstrated for determining experimental conditions where tunneling will have a measurable impact on the electrochemistry of M-I-MNP systems. |
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| AbstractList | Here, a new methodology is proposed for treating electrochemical current densities in metal-insulator-metal nanoparticle (M-I-MNP) systems. The described model provides broad, practical insights about MNP-mediated electron transfer to redox species in solution, where electron transfer from the underlying electrode to a MNP via tunneling and heterogeneous electron transfer from the MNP to redox species in solution are treated as sequential steps. Tunneling is treated through an adaptation of the Simmons model of tunneling in metal-insulator-metal structures, and explicit equations are provided for tunneling currents, which demonstrate the effect of various experimental parameters, such as insulator thickness and MNP size. Overall, a general approach is demonstrated for determining experimental conditions where tunneling will have a measurable impact on the electrochemistry of M-I-MNP systems. |
| Author | Hill, Caleb M Kim, Jiyeon Bard, Allen J |
| AuthorAffiliation | The University of Texas at Austin Center for Electrochemistry, Department of Chemistry |
| AuthorAffiliation_xml | – name: Center for Electrochemistry, Department of Chemistry – name: The University of Texas at Austin |
| Author_xml | – sequence: 1 givenname: Caleb M surname: Hill fullname: Hill, Caleb M – sequence: 2 givenname: Jiyeon surname: Kim fullname: Kim, Jiyeon – sequence: 3 givenname: Allen J surname: Bard fullname: Bard, Allen J email: ajbard@mail.utexas.edu |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/26280667$$D View this record in MEDLINE/PubMed |
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| References | ref9/cit9 ref6/cit6 ref3/cit3 ref27/cit27 Khairutdinov R. F. (ref14/cit14) 1989; 30 ref18/cit18 ref11/cit11 ref25/cit25 ref16/cit16 ref23/cit23 ref8/cit8 ref5/cit5 ref2/cit2 ref20/cit20 ref17/cit17 ref10/cit10 ref26/cit26 ref19/cit19 ref21/cit21 ref12/cit12 ref15/cit15 Bard A. J. (ref22/cit22) 2001 ref13/cit13 ref4/cit4 ref1/cit1 ref24/cit24 ref7/cit7 |
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| Title | Electrochemistry at a Metal Nanoparticle on a Tunneling Film: A Steady-State Model of Current Densities at a Tunneling Ultramicroelectrode |
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