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Title: Efficient Oxygen Electrocatalysis by Nanostructured Mixed-Metal Oxides

Abstract

Oxygen electrocatalysis plays a critical role in the efficiency of important energy conversion and storage systems. While many efforts have focused on designing efficient electrocatalysts for these processes, optimal catalysts that are inexpensive, active, selective, and stable are still being searched. Nonstoichiometric, mixed-metal oxides present a promising group of electrocatalysts for these processes due to the versatility of the surface composition and fast oxygen conducting properties. Herein, we demonstrate, using a combination of theoretical and experimental studies, the ability to develop design principles that can be used to engineer oxygen electrocatalysis activity of layered, mixed ionic-electronic conducting Ruddlesden– Popper (R–P) oxides. We show that a density function theory (DFT) derived descriptor, O2 binding energy on a surface oxygen vacancy, can be effective in identifying efficient R–P oxide structures for oxygen reduction reaction (ORR). Using a controlled synthesis method, well-defined nanostructures of R–P oxides are obtained, which along with thermochemical and electrochemical activity studies are used to validate the design principles. This has led to the identification of a highly active ORR electrocatalyst, nanostructured Co-doped lanthanum nickelate oxide, which when incorporated in solid oxide fuel cell cathodes significantly enhances the performance at intermediate temperatures (~550 °C), while maintaining long-term stability. Here,more » the reported findings demonstrate the effectiveness of the developed design principles to engineer mixed ionic-electronic conducting oxides for efficient oxygen electrocatalysis, and the potential of nanostructured Co-doped lanthanum nickelate oxides as promising catalysts for oxygen electrocatalysis.« less

Authors:
 [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. Wayne State Univ., Detroit, MI (United States)
Publication Date:
Research Org.:
Wayne State Univ., Detroit, MI (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1487017
Grant/Contract Number:  
SC0014347
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 26; 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

Citation Formats

Gu, Xiang -Kui, Carneiro, Juliana S. A., Samira, Samji, Das, Anirban, Ariyasingha, Nuwandi M., and Nikolla, Eranda. Efficient Oxygen Electrocatalysis by Nanostructured Mixed-Metal Oxides. United States: N. p., 2018. Web. doi:10.1021/jacs.7b11138.
Gu, Xiang -Kui, Carneiro, Juliana S. A., Samira, Samji, Das, Anirban, Ariyasingha, Nuwandi M., & Nikolla, Eranda. Efficient Oxygen Electrocatalysis by Nanostructured Mixed-Metal Oxides. United States. https://doi.org/10.1021/jacs.7b11138
Gu, Xiang -Kui, Carneiro, Juliana S. A., Samira, Samji, Das, Anirban, Ariyasingha, Nuwandi M., and Nikolla, Eranda. Wed . "Efficient Oxygen Electrocatalysis by Nanostructured Mixed-Metal Oxides". United States. https://doi.org/10.1021/jacs.7b11138. https://www.osti.gov/servlets/purl/1487017.
@article{osti_1487017,
title = {Efficient Oxygen Electrocatalysis by Nanostructured Mixed-Metal Oxides},
author = {Gu, Xiang -Kui and Carneiro, Juliana S. A. and Samira, Samji and Das, Anirban and Ariyasingha, Nuwandi M. and Nikolla, Eranda},
abstractNote = {Oxygen electrocatalysis plays a critical role in the efficiency of important energy conversion and storage systems. While many efforts have focused on designing efficient electrocatalysts for these processes, optimal catalysts that are inexpensive, active, selective, and stable are still being searched. Nonstoichiometric, mixed-metal oxides present a promising group of electrocatalysts for these processes due to the versatility of the surface composition and fast oxygen conducting properties. Herein, we demonstrate, using a combination of theoretical and experimental studies, the ability to develop design principles that can be used to engineer oxygen electrocatalysis activity of layered, mixed ionic-electronic conducting Ruddlesden– Popper (R–P) oxides. We show that a density function theory (DFT) derived descriptor, O2 binding energy on a surface oxygen vacancy, can be effective in identifying efficient R–P oxide structures for oxygen reduction reaction (ORR). Using a controlled synthesis method, well-defined nanostructures of R–P oxides are obtained, which along with thermochemical and electrochemical activity studies are used to validate the design principles. This has led to the identification of a highly active ORR electrocatalyst, nanostructured Co-doped lanthanum nickelate oxide, which when incorporated in solid oxide fuel cell cathodes significantly enhances the performance at intermediate temperatures (~550 °C), while maintaining long-term stability. Here, the reported findings demonstrate the effectiveness of the developed design principles to engineer mixed ionic-electronic conducting oxides for efficient oxygen electrocatalysis, and the potential of nanostructured Co-doped lanthanum nickelate oxides as promising catalysts for oxygen electrocatalysis.},
doi = {10.1021/jacs.7b11138},
journal = {Journal of the American Chemical Society},
number = 26,
volume = 140,
place = {United States},
year = {2018},
month = {5}
}

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Cited by: 11 works
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Figures / Tables:

Figure S1 Figure S1: The structures of B-site terminated (001) surfaces for first-series R-P oxides with mixed B-site transition metals. The cyan, green/blue, and red spheres represent La, transition metal, and O atoms, respectively.

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