Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 6, Issue 21, Pages 18475-18479Publisher
AMER CHEMICAL SOC
DOI: 10.1021/am506435u
Keywords
water oxidation catalyst; 1st row transition metal; electrochemistry; graphene
Funding
- National Science Foundation [DMR-1308229]
- Overseas Study Program of Guangzhou Elite Project [JY201326]
- Division Of Materials Research
- Direct For Mathematical & Physical Scien [1308229] Funding Source: National Science Foundation
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Covalent anchoring of 2,2'-bipyridine (L) to a graphene (Gr) modified electrode followed by treatment with an Mx+(NO3)(x) solution (M = Fe3+, Co2+, Ni2+, or Cu2+) results in surface-bound catalysts with high redox activity in neutral water at ambient temperature. Raman and IR spectroscopies indicate the successful L grafting and Gr deposition onto the electrodes, whereas metal concentration was determined by inductively coupled plasma mass spectrometry (ICP-MS). Cyclic voltammetry measurements were used to investigate catalytic performances, whereas a rotating ring-disk electrode was used to measure the faraday efficiencies of oxygen evolution reaction and determine experimental turnover frequencies (TOFs). Of the four metal-L complexes investigated, Co-L on a Gr-modified indium tin oxide (ITO) electrode exhibits the best catalytic activity. Washing with a solution containing catalytically inert Zn2+ removes Co weakly bound by surface carboxylate functionalities, and ensures the presence of only covalently attached active catalytic species. This process results in an experimental TOF of 14 s(-1) at an overpotential of 834 mV. Functionalization of Gr-modified electrodes with appropriate metal-binding moieties thus provides a feasible strategy for loading first row transition metals onto conductive surfaces for the generation of highly active water oxidation catalysts.
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