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Title: Behavior of the Ru-bda water oxidation catalyst covalently anchored on glassy carbon electrodes

Electrochemical reduction of the dizaonium complex, [RuII(bda)(NO)(N–N2)2]3+, 23+ (N–N22+ is 4-(pyridin-4-yl) benzenediazonium and bda2– is [2,2'-bipyridine]-6,6'-dicarboxylate), in acetone produces the covalent grafting of this molecular complex onto glassy carbon (GC) electrodes. Multiple cycling voltammetric experiments on the GC electrode generates hybrid materials labeled as GC-4, with the corresponding Ru-aqua complex anchored on the graphite surface. GC-4 has been characterized at pH = 7.0 by electrochemical techniques and X-ray absorption spectroscopy (XAS) and has been shown to act as an active catalyst for the oxidation of water to dioxygen. This new hybrid material has a lower catalytic performance than its counterpart in homogeneous phase and progressively decomposes to form RuO2 at the electrode surface. The resulting metal oxide attached at the GC electrode surface, GC-RuO2, is a very fast and rugged heterogeneous water oxidation catalyst with TOFis of 300 s–1 and TONs >45000. The observed performance is comparable to the best electrocatalysts reported so far, at neutral pH.
 [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [2] ;  [5] ;  [6]
  1. Institute of Chemical Research of Catalonia (ICIQ), Tarragona (Spain)
  2. Freie Univ., Berlin (Germany)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Yale Univ., New Haven, CT (United States)
  5. Univ. Autonoma de Barcelona, Barcelona (Spain)
  6. Institute of Chemical Research of Catalonia (ICIQ), Tarragona (Spain); Univ. Autonoma de Barcelona, Barcelona (Spain)
Publication Date:
OSTI Identifier:
Report Number(s):
Journal ID: ISSN 2155-5435; R&D Project: CO045; KC0301020
Grant/Contract Number:
05K14KE1; Ha3265/6-1; CTQ-2013-49075-R; CTQ2011-26440; SEV-2013-0319; AC02-98CH10886
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 5; Journal Issue: 6; Journal ID: ISSN 2155-5435
American Chemical Society
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY water oxidation catalysis; electrocatalysis; water splitting; Ru complexes; modified graphite electrodes; heterogeneous water oxidation catalysis; RuO2