Design of template-stabilized active and earth-abundant oxygen evolution catalysts in acid
Abstract
Oxygen evolution reaction (OER) catalysts that are earth-abundant and are active and stable in acid are unknown. Active catalysts derived from Co and Ni oxides dissolve at low pH, whereas acid stable systems such as Mn oxides (MnOx) display poor OER activity. We now demonstrate a rational approach for the design of earth-abundant catalysts that are stable and active in acid by treating activity and stability as decoupled elements of mixed metal oxides. Manganese serves as a stabilizing structural element for catalytically active Co centers in CoMnOx films. In acidic solutions (pH 2.5), CoMnOx exhibits the OER activity of electrodeposited Co oxide (CoOx) with a Tafel slope of 70–80 mV per decade while also retaining the long-term acid stability of MnOx films for OER at 0.1 mA cm-2. Driving OER at greater current densities in this system is not viable because at high anodic potentials, Mn oxides convert to and dissolve as permanganate. However, by exploiting the decoupled design of the catalyst, the stabilizing structural element may be optimized independently of the Co active sites. By screening potential–pH diagrams, we replaced Mn with Pb to prepare CoFePbOx films that maintained the high OER activity of CoOx at pH 2.5 whilemore »
- Authors:
-
- Harvard Univ., Cambridge, MA (United States)
- Publication Date:
- Research Org.:
- Harvard Univ., Cambridge, MA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Science Foundation (NSF)
- OSTI Identifier:
- 1599222
- Grant/Contract Number:
- SC0017619; ECS-0335765
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemical Science
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 7; Journal ID: ISSN 2041-6520
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Huynh, Michael, Ozel, Tuncay, Liu, Chong, Lau, Eric C., and Nocera, Daniel G. Design of template-stabilized active and earth-abundant oxygen evolution catalysts in acid. United States: N. p., 2017.
Web. doi:10.1039/C7SC01239J.
Huynh, Michael, Ozel, Tuncay, Liu, Chong, Lau, Eric C., & Nocera, Daniel G. Design of template-stabilized active and earth-abundant oxygen evolution catalysts in acid. United States. https://doi.org/10.1039/C7SC01239J
Huynh, Michael, Ozel, Tuncay, Liu, Chong, Lau, Eric C., and Nocera, Daniel G. Fri .
"Design of template-stabilized active and earth-abundant oxygen evolution catalysts in acid". United States. https://doi.org/10.1039/C7SC01239J. https://www.osti.gov/servlets/purl/1599222.
@article{osti_1599222,
title = {Design of template-stabilized active and earth-abundant oxygen evolution catalysts in acid},
author = {Huynh, Michael and Ozel, Tuncay and Liu, Chong and Lau, Eric C. and Nocera, Daniel G.},
abstractNote = {Oxygen evolution reaction (OER) catalysts that are earth-abundant and are active and stable in acid are unknown. Active catalysts derived from Co and Ni oxides dissolve at low pH, whereas acid stable systems such as Mn oxides (MnOx) display poor OER activity. We now demonstrate a rational approach for the design of earth-abundant catalysts that are stable and active in acid by treating activity and stability as decoupled elements of mixed metal oxides. Manganese serves as a stabilizing structural element for catalytically active Co centers in CoMnOx films. In acidic solutions (pH 2.5), CoMnOx exhibits the OER activity of electrodeposited Co oxide (CoOx) with a Tafel slope of 70–80 mV per decade while also retaining the long-term acid stability of MnOx films for OER at 0.1 mA cm-2. Driving OER at greater current densities in this system is not viable because at high anodic potentials, Mn oxides convert to and dissolve as permanganate. However, by exploiting the decoupled design of the catalyst, the stabilizing structural element may be optimized independently of the Co active sites. By screening potential–pH diagrams, we replaced Mn with Pb to prepare CoFePbOx films that maintained the high OER activity of CoOx at pH 2.5 while exhibiting long-term acid stability at higher current densities (at 1 mA cm-2 for over 50 h at pH 2.0). Under these acidic conditions, CoFePbOx exhibits OER activity that approaches noble metal oxides, thus establishing the viability of decoupling functionality in mixed metal catalysts for designing active, acid-stable, and earth-abundant OER catalysts.},
doi = {10.1039/C7SC01239J},
journal = {Chemical Science},
number = 7,
volume = 8,
place = {United States},
year = {Fri May 05 00:00:00 EDT 2017},
month = {Fri May 05 00:00:00 EDT 2017}
}
Web of Science
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Quasi-single-crystalline CoO hexagrams with abundant defects for highly efficient electrocatalytic water oxidation
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- Liang, Zuozhong; Huang, Zhehao; Yuan, Haitao
- Chemical Science, Vol. 9, Issue 34
Cobalt-doped hematite thin films for electrocatalytic water oxidation in highly acidic media
journal, January 2019
- Kwong, Wai Ling; Lee, Cheng Choo; Shchukarev, Andrey
- Chemical Communications, Vol. 55, Issue 34
Photoelectrochemical cell for P–H/C–H cross-coupling with hydrogen evolution
journal, January 2019
- Wang, Jing-Hao; Li, Xu-Bing; Li, Jian
- Chemical Communications, Vol. 55, Issue 70
Fabricating Cu, Cu 2 O and hybrid Cu-Cu 2 O nanoparticles in carbon matrix and exploring catalytic activity of oxygen and hydrogen evolution and green A 3 -coupling reaction
journal, November 2018
- Muthukumar, Pandi; Kumar, P. Suresh; Anthony, Savarimuthu Philip
- Materials Research Express, Vol. 6, Issue 2
Electrochemical characterization of manganese oxides as a water oxidation catalyst in proton exchange membrane electrolysers
journal, May 2019
- Hayashi, Toru; Bonnet-Mercier, Nadège; Yamaguchi, Akira
- Royal Society Open Science, Vol. 6, Issue 5
FeNxC Based Catalysts Prepared by the Calcination of Iron-Ethylenediamine@Polyaniline as the Cathode-Catalyst of Proton Exchange Membrane Fuel Cell
journal, August 2019
- Wang, Yen-Zen; Huang, Wen-Yao; Hsieh, Tar-Hwa
- Polymers, Vol. 11, Issue 8
Design of Multi‐Metallic‐Based Electrocatalysts for Enhanced Water Oxidation
journal, May 2019
- Bo, Xin; Dastafkan, Kamran; Zhao, Chuan
- ChemPhysChem, Vol. 20, Issue 22
Efficient oxygen evolution electrocatalysis in acid by a perovskite with face-sharing IrO6 octahedral dimers
journal, December 2018
- Yang, Lan; Yu, Guangtao; Ai, Xuan
- Nature Communications, Vol. 9, Issue 1
Stable Potential Windows for Long‐Term Electrocatalysis by Manganese Oxides Under Acidic Conditions
journal, March 2019
- Li, Ailong; Ooka, Hideshi; Bonnet, Nadège
- Angewandte Chemie, Vol. 131, Issue 15
Noble-Metal-Free Electrocatalysts for Oxygen Evolution
journal, November 2018
- Lyu, Fenglei; Wang, Qingfa; Choi, Sung Mook
- Small, Vol. 15, Issue 1