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

Matheu, Roc; Francàs, Laia; Chernev, Petko; Ertem, Mehmed Z.; Batista, Victor; Haumann, Michael; Sala, Xavier; Llobet, Antoni

doi:10.1021/acscatal.5b00132

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

Journal Article · Thu May 07 00:00:00 EDT 2015 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5b00132· OSTI ID:1221759

Matheu, Roc ^[1]; Francàs, Laia ^[1]; Chernev, Petko ^[2]; Ertem, Mehmed Z. ^[3]; Batista, Victor ^[4]; Haumann, Michael ^[2]; Sala, Xavier ^[5]; Llobet, Antoni ^[6]

Institute of Chemical Research of Catalonia (ICIQ), Tarragona (Spain)
Freie Univ., Berlin (Germany)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Yale Univ., New Haven, CT (United States)
Univ. Autonoma de Barcelona, Barcelona (Spain)
Institute of Chemical Research of Catalonia (ICIQ), Tarragona (Spain); Univ. Autonoma de Barcelona, Barcelona (Spain)

Electrochemical reduction of the dizaonium complex, [Ru^II(bda)(NO)(N–N₂)₂]³⁺, 2³⁺ (N–N₂²⁺ is 4-(pyridin-4-yl) benzenediazonium and bda^2– 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 TOF_is of 300 s^–1 and TONs >45000. The observed performance is comparable to the best electrocatalysts reported so far, at neutral pH.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Argonne-Northwestern Solar Energy Research Center (ANSER)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: 05K14KE1; Ha3265/6-1; CTQ-2013-49075-R; CTQ2011-26440; SEV-2013-0319; AC02-98CH10886; SC0001059

OSTI ID:: 1221759

Report Number(s):: BNL-108389-2015-JA; R&D Project: CO045; KC0301020

Journal Information:: ACS Catalysis, Vol. 5, Issue 6; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 68 works

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

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