Chasing the Achilles’ Heel in Hybrid Systems of Diruthenium Water Oxidation Catalysts Anchored on Indium Tin Oxide: The Stability of the Anchor

Odrobina, Jann; Scholz, Julius; Risch, Marcel; Dechert, Sebastian; Jooss, Christian; Meyer, Franc

doi:10.1021/acscatal.7b01883

Title: Chasing the Achilles’ Heel in Hybrid Systems of Diruthenium Water Oxidation Catalysts Anchored on Indium Tin Oxide: The Stability of the Anchor

Journal Article · 17 August 2017 · ACS Catalysis

DOI: https://doi.org/10.1021/acscatal.7b01883 · OSTI ID:1393664

Odrobina, Jann ^[1]; Scholz, Julius ^[1];

^[1]; Dechert, Sebastian ^[1];

^[1];

^[1]

Univ. of Goettingen (Germany)

The development of hybrid devices for photo-driven water oxidation with dinuclear molecular ruthenium catalysts on solid supports aims both at high efficiencies of the catalyst and at high stability of the linking to the surface. We herein report a systematic study regarding the stability of catalysts anchored on an indium tin oxide (ITO) support via different acid functional groups at the ligand backbone: viz., a single carboxylate anchor, two carboxylate anchors, and a phosphonate anchor. The integrity of the hybrid electrodes ITO|mesoITO|catalyst was evaluated under acidic aqueous conditions as a function of the applied electric potential below and above the onset of the oxygen evolution reaction (OER). Rotating ring disk electrode (RRDE) experiments allowed us to distinguish between the water oxidation and the desorption processes. X-ray photoemission (XPS) and X-ray absorption spectroscopy (XAS) after electrochemical treatment showed high chemical stability of the catalyst core structure but pronounced dependence of the hybrid stability on the oxidation state of the ruthenium center. A combination of these different spectroscopic techniques shed light on the mechanisms underlying catalyst desorption. Specifically, catalysts equipped with carboxylate anchors are found to continuously desorb already at low applied potentials below the OER onset, while for the more rugged phosphonate-based hybrid oxidative P–C(aryl) bond cleavage is proposed to occur, but only after reaching the high-valent Ru^VRu^IV state. These findings reveal specific challenges for anchoring strategies in molecular water oxidation catalysis.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (US)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

OSTI ID:: 1393664

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 9 Vol. 7; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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