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Title: Molecular Mixed-Metal Manganese Oxido Cubanes as Precursors to Heterogeneous Oxygen Evolution Catalysts

Abstract

Well-defined mixed-metal [CoMn3O4] and [NiMn3O4] cubane complexes were synthesized and used as precursors for heterogeneous oxygen evolution reaction (OER) electrocatalysts. The discrete clusters were dropcasted onto glassy carbon (GC) and indium tin oxide (ITO) electrodes, and the OER activities of the resulting films were evaluated. The catalytic surfaces were analyzed by various techniques to gain insight into the structure-function relationships of the electrocatalysts' heterometallic composition. Depending on preparation conditions, the Co-Mn oxide was found to change metal composition during catalysis, while the Ni-Mn oxides maintained the NiMn3 ratio. XAS studies provided structural insights indicating that the electrocatalysts are different from the molecular precursors, but that the original NiMn3O4 cubane-like geometry was maintained in the absence of thermal treatment (2-Ni). In contrast, the thermally generated 3-Ni develops an oxide-like extended structure. Both 2-Ni and 3-Ni undergo structural changes upon electrolysis, but they do not convert into the same material. The observed structural motifs in these heterogeneous electrocatalysts are reminiscent of the biological oxygen-evolving complex in PhotosystemII, including the MMn3O4 cubane moiety. The reported studies demonstrate the use of discrete heterometallic oxide clusters as precursors for heterogeneous water oxidation catalysts of novel composition and the distinct behavior of two sets of mixedmore » metal oxides.« less

Authors:
 [1];  [2];  [3];  [3];  [3];  [1]
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  1. California Inst. of Technology (CalTech), Pasadena, CA (United States). Division of Chemistry and Chemical Engineering
  2. Joint Center for Artificial Photosynthesis, Pasadena, CA (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Physical Biosciences Division
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1512240
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Chemistry - A European Journal
Additional Journal Information:
Journal Volume: 21; Journal Issue: 38; Journal ID: ISSN 0947-6539
Publisher:
ChemPubSoc Europe
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Suseno, Sandy, McCrory, Charles C. L., Tran, Rosalie, Gul, Sheraz, Yano, Junko, and Agapie, Theodor. Molecular Mixed-Metal Manganese Oxido Cubanes as Precursors to Heterogeneous Oxygen Evolution Catalysts. United States: N. p., 2015. Web. doi:10.1002/chem.201501104.
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Suseno, Sandy, McCrory, Charles C. L., Tran, Rosalie, Gul, Sheraz, Yano, Junko, & Agapie, Theodor. Molecular Mixed-Metal Manganese Oxido Cubanes as Precursors to Heterogeneous Oxygen Evolution Catalysts. United States. https://doi.org/10.1002/chem.201501104
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Suseno, Sandy, McCrory, Charles C. L., Tran, Rosalie, Gul, Sheraz, Yano, Junko, and Agapie, Theodor. Tue . "Molecular Mixed-Metal Manganese Oxido Cubanes as Precursors to Heterogeneous Oxygen Evolution Catalysts". United States. https://doi.org/10.1002/chem.201501104. https://www.osti.gov/servlets/purl/1512240.
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@article{osti_1512240,
title = {Molecular Mixed-Metal Manganese Oxido Cubanes as Precursors to Heterogeneous Oxygen Evolution Catalysts},
author = {Suseno, Sandy and McCrory, Charles C. L. and Tran, Rosalie and Gul, Sheraz and Yano, Junko and Agapie, Theodor},
abstractNote = {Well-defined mixed-metal [CoMn3O4] and [NiMn3O4] cubane complexes were synthesized and used as precursors for heterogeneous oxygen evolution reaction (OER) electrocatalysts. The discrete clusters were dropcasted onto glassy carbon (GC) and indium tin oxide (ITO) electrodes, and the OER activities of the resulting films were evaluated. The catalytic surfaces were analyzed by various techniques to gain insight into the structure-function relationships of the electrocatalysts' heterometallic composition. Depending on preparation conditions, the Co-Mn oxide was found to change metal composition during catalysis, while the Ni-Mn oxides maintained the NiMn3 ratio. XAS studies provided structural insights indicating that the electrocatalysts are different from the molecular precursors, but that the original NiMn3O4 cubane-like geometry was maintained in the absence of thermal treatment (2-Ni). In contrast, the thermally generated 3-Ni develops an oxide-like extended structure. Both 2-Ni and 3-Ni undergo structural changes upon electrolysis, but they do not convert into the same material. The observed structural motifs in these heterogeneous electrocatalysts are reminiscent of the biological oxygen-evolving complex in PhotosystemII, including the MMn3O4 cubane moiety. The reported studies demonstrate the use of discrete heterometallic oxide clusters as precursors for heterogeneous water oxidation catalysts of novel composition and the distinct behavior of two sets of mixed metal oxides.},
doi = {10.1002/chem.201501104},
journal = {Chemistry - A European Journal},
number = 38,
volume = 21,
place = {United States},
year = {Tue Aug 04 00:00:00 EDT 2015},
month = {Tue Aug 04 00:00:00 EDT 2015}
}
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https://doi.org/10.1002/chem.201501104
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Figures / Tables:

Figure 1 Figure 1: RDV of 2-Co (A) and 2-Ni (B) on glassy carbon disks before and after 2 h CP in 1 M NaOH solution; (C) stability test of 2 over 2 h of CP held at 10 mA cm–2 at 1600 rpm rotation rate.
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