Noncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation

Geer, Ana M.; Liu, Chang; Musgrave, III, Charles B.; Webber, Christopher; Johnson, Grayson; Zhou, Hua; Sun, Cheng-Jun; Dickie, Diane A.; Goddard, III, William A.; Zhang, Sen; Gunnoe, T. Brent

doi:10.1002/smsc.202100037

Noncovalent Immobilization of Pentamethylcyclopentadienyl Iridium Complexes on Ordered Mesoporous Carbon for Electrocatalytic Water Oxidation

Journal Article · Fri Aug 06 00:00:00 EDT 2021 · Small Science

DOI:https://doi.org/10.1002/smsc.202100037· OSTI ID:1840931

Geer, Ana M. ^[1]; Liu, Chang ^[1]; Musgrave, III, Charles B. ^[2]; Webber, Christopher ^[1]; Johnson, Grayson ^[1]; Zhou, Hua ^[3]; Sun, Cheng-Jun ^[3]; Dickie, Diane A. ^[1]; Goddard, III, William A. ^[2]; ^[1]; Gunnoe, T. Brent ^[1]

Univ. of Virginia, Charlottesville, VA (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

The attachment of molecular catalysts to conductive supports for the preparation of solid-state anodes is important for the development of devices for electrocatalytic water oxidation. The preparation and characterization of three molecular cyclopentadienyl iridium(III) complexes, Cp*Ir(1-pyrenyl(2-pyridyl)ethanolate-κO,κN)Cl (1) (Cp* = pentamethylcyclopentadienyl), Cp*Ir(diphenyl(2-pyridyl)methanolate-κO,κN)Cl (2), and [Cp*Ir(4-(1-pyrenyl)-2,2'-bipyridine)Cl]Cl (3), as precursors for electrochemical water oxidation catalysts, are reported. These complexes contain aromatic groups that can be attached via noncovalent π-stacking to ordered mesoporous carbon (OMC). The resulting iridium-based OMC materials (Ir-1, Ir-2, and Ir-3) were tested for electrocatalytic water oxidation leading to turnover frequencies (TOFs) of 0.9–1.6 s^-1 at an overpotential of 300 mV under acidic conditions. The stability of the materials is demonstrated by electrochemical cycling and X-ray absorption spectroscopy analysis before and after catalysis. Theoretical studies on the interactions between the molecular complexes and the OMC support provide insight onto the noncovalent binding and are in agreement with the experimental loadings.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1840931

Journal Information:: Small Science, Journal Name: Small Science Journal Issue: 11 Vol. 1; ISSN 2688-4046

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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