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Title: Nature of Activated Manganese Oxide for Oxygen Evolution

Abstract

Electrodeposited manganese oxide films (MnOx) are promising stable oxygen evolution catalysts. They are able to catalyze the oxygen evolution reaction in acidic solutions but with only modest activity when prepared by constant anodic potential deposition. We show herein that the performance of these catalysts is improved when they are “activated” by potential cycling protocols, as measured by Tafel analysis (where lower slope is better): upon activation the Tafel slope decreases from ~120 to ~70 mV/decade in neutral conditions and from ~650 to ~90 mV/decade in acidic solutions. Electrochemical, spectroscopic, and structural methods were employed to study the activation process and support a mechanism where the original birnessite-like MnOx (δ-MnO2) undergoes a phase change, induced by comproportionation with cathodically generated Mn(OH)2, to a hausmannite-like intermediate (α-Mn3O4). Subsequent anodic conditioning from voltage cycling or water oxidation produces a disordered birnessite-like phase, which is highly active for oxygen evolution. At pH 2.5, the current density of activated MnOx (at an overpotential of 600 mV) is 2 orders of magnitude higher than that of the original MnOx and begins to approach that of Ru and Ir oxides in acid.

Authors:
 [1];  [2];  [3];  [1]
+ Show Author Affiliations
  1. Harvard Univ., Cambridge, MA (United States)
  2. Columbia Univ., New York, NY (United States)
  3. Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Next Generation of Materials Design (CNGMD); Energy Frontier Research Centers (EFRC) (United States). Programmable Quantum Materials (Pro-QM); Columbia Univ., New York, NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1387229
Grant/Contract Number:  
AC36-99GO10337; SC0009565; SC0001085; AC36-08GO28308; AC02-98CH10886
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 47; Related Information: CNGMD partners with National Renewable Energy Laboratory (lead); Colorado School of Mines; Harvard University; Lawrence Berkeley National Laboratory; Massachusetts Institute of Technology; Oregon State University; SLAC National Accelerator Laboratory; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; solar (photovoltaic); solar (fuels); solid state lighting; phonons; thermoelectric; hydrogen and fuel cells; defects; charge transport; optics; materials and chemistry by design; synthesis (novel materials); thin films; radiology; oxides; deposition; transition metals

Citation Formats

Huynh, Michael, Shi, Chenyang, Billinge, Simon J. L., and Nocera, Daniel G. Nature of Activated Manganese Oxide for Oxygen Evolution. United States: N. p., 2015. Web. doi:10.1021/jacs.5b06382.
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Huynh, Michael, Shi, Chenyang, Billinge, Simon J. L., & Nocera, Daniel G. Nature of Activated Manganese Oxide for Oxygen Evolution. United States. https://doi.org/10.1021/jacs.5b06382
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Huynh, Michael, Shi, Chenyang, Billinge, Simon J. L., and Nocera, Daniel G. Tue . "Nature of Activated Manganese Oxide for Oxygen Evolution". United States. https://doi.org/10.1021/jacs.5b06382. https://www.osti.gov/servlets/purl/1387229.
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@article{osti_1387229,
title = {Nature of Activated Manganese Oxide for Oxygen Evolution},
author = {Huynh, Michael and Shi, Chenyang and Billinge, Simon J. L. and Nocera, Daniel G.},
abstractNote = {Electrodeposited manganese oxide films (MnOx) are promising stable oxygen evolution catalysts. They are able to catalyze the oxygen evolution reaction in acidic solutions but with only modest activity when prepared by constant anodic potential deposition. We show herein that the performance of these catalysts is improved when they are “activated” by potential cycling protocols, as measured by Tafel analysis (where lower slope is better): upon activation the Tafel slope decreases from ~120 to ~70 mV/decade in neutral conditions and from ~650 to ~90 mV/decade in acidic solutions. Electrochemical, spectroscopic, and structural methods were employed to study the activation process and support a mechanism where the original birnessite-like MnOx (δ-MnO2) undergoes a phase change, induced by comproportionation with cathodically generated Mn(OH)2, to a hausmannite-like intermediate (α-Mn3O4). Subsequent anodic conditioning from voltage cycling or water oxidation produces a disordered birnessite-like phase, which is highly active for oxygen evolution. At pH 2.5, the current density of activated MnOx (at an overpotential of 600 mV) is 2 orders of magnitude higher than that of the original MnOx and begins to approach that of Ru and Ir oxides in acid.},
doi = {10.1021/jacs.5b06382},
journal = {Journal of the American Chemical Society},
number = 47,
volume = 137,
place = {United States},
year = {Tue Nov 17 00:00:00 EST 2015},
month = {Tue Nov 17 00:00:00 EST 2015}
}
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Figures / Tables:

Figure 1 Figure 1: Cyclic voltammogram of a 1 cm2 FTO electrode in 0.5 mM Mn2+ and 0.9 M KNO3 solution at 100 mV/s scan rate showing the first (blue line ) and second (red line ) cycles.
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