Robust Copper-Based Nanosponge Architecture Decorated by Ruthenium with Enhanced Electrocatalytic Performance for Ambient Nitrogen Reduction to Ammonia

Kui Li; Lei Ding; Zhiqiang Xie; Gaoqiang Yang; Shule Yu; Weitian Wang; David A. Cullen; Harry M. Meyer; Guoxiang Hu; Panchapakesan Ganesh; Thomas R. Watkins; Feng Yuan Zhang

doi:10.1021/acsami.2c20809

Robust Copper-Based Nanosponge Architecture Decorated by Ruthenium with Enhanced Electrocatalytic Performance for Ambient Nitrogen Reduction to Ammonia

Kui Li, Lei Ding, Zhiqiang Xie, Gaoqiang Yang, Shule Yu, Weitian Wang, David A. Cullen, Harry M. Meyer, Guoxiang Hu, Panchapakesan Ganesh, Thomas R. Watkins, Feng Yuan Zhang

Research output: Contribution to journal › Article › peer-review

8 Scopus citations

Abstract

Electrochemical conversion of nitrogen to green ammonia is an attractive alternative to the Haber-Bosch process. However, it is currently bottlenecked by the lack of highly efficient electrocatalysts to drive the sluggish nitrogen reduction reaction (N₂RR). Herein, we strategically design a cost-effective bimetallic Ru-Cu mixture catalyst in a nanosponge (NS) architecture via a rapid and facile method. The porous NS mixture catalysts exhibit a large electrochemical active surface area and enhanced specific activity arising from the charge redistribution for improved activation and adsorption of the activated nitrogen species. Benefiting from the synergistic effect of the Cu constituent on morphology decoration and thermodynamic suppression of the competing hydrogen evolution reaction, the optimized Ru_0.15Cu_0.85 NS catalyst presents an impressive N₂RR performance with an ammonia yield rate of 26.25 μg h^-1 mg_cat.^-1 (corresponding to 10.5 μg h^-1 cm^-2) and Faradic efficiency of 4.39% as well as superior stability in alkaline medium, which was superior to that of monometallic Ru and Cu nanostructures. Additionally, this work develops a new bimetallic combination of Ru and Cu, which promotes the strategy to design efficient electrocatalysts for electrochemical ammonia production under ambient conditions.

Original language	English
Pages (from-to)	11703-11712
Number of pages	10
Journal	ACS Applied Materials and Interfaces
Volume	15
Issue number	9
DOIs	https://doi.org/10.1021/acsami.2c20809
State	Published - Mar 8 2023

Funding

The authors greatly appreciate the support from the U.S. Department of Energy Office of Energy Efficiency and Renewable Energy (EERE) under the Fuel Cell Technologies Office Award Number DE-EE0008426 and DE-EE0008423 and the National Energy Technology Laboratory under Award DE-FE0011585. A portion of the research was performed as part of a user project through Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences, which is a U.S. DOE Office of Science User Facility and by instrumentation provided by the U.S. DOE Office of Nuclear Energy, Fuel Cycle R&D Program, and the Nuclear Science User Facilities. The authors also wish to express their appreciation to Dr. Meiling Xiao, Alexander Terekhov, Douglas Warnberg, and Dr. Brian Canfield for their help.

Keywords

bimetallic catalysts
electrocatalysis
electrocatalytic reduction of nitrogen
green ammonia synthesis
nanosponge architecture

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1021/acsami.2c20809

Cite this

Li, K., Ding, L., Xie, Z., Yang, G., Yu, S., Wang, W., Cullen, D. A., Meyer, H. M., Hu, G., Ganesh, P., Watkins, T. R., & Zhang, F. Y. (2023). Robust Copper-Based Nanosponge Architecture Decorated by Ruthenium with Enhanced Electrocatalytic Performance for Ambient Nitrogen Reduction to Ammonia. ACS Applied Materials and Interfaces, 15(9), 11703-11712. https://doi.org/10.1021/acsami.2c20809

@article{9a46a9e60ec54b5fa98d6a45a395fa35,

title = "Robust Copper-Based Nanosponge Architecture Decorated by Ruthenium with Enhanced Electrocatalytic Performance for Ambient Nitrogen Reduction to Ammonia",

abstract = "Electrochemical conversion of nitrogen to green ammonia is an attractive alternative to the Haber-Bosch process. However, it is currently bottlenecked by the lack of highly efficient electrocatalysts to drive the sluggish nitrogen reduction reaction (N2RR). Herein, we strategically design a cost-effective bimetallic Ru-Cu mixture catalyst in a nanosponge (NS) architecture via a rapid and facile method. The porous NS mixture catalysts exhibit a large electrochemical active surface area and enhanced specific activity arising from the charge redistribution for improved activation and adsorption of the activated nitrogen species. Benefiting from the synergistic effect of the Cu constituent on morphology decoration and thermodynamic suppression of the competing hydrogen evolution reaction, the optimized Ru0.15Cu0.85 NS catalyst presents an impressive N2RR performance with an ammonia yield rate of 26.25 μg h-1 mgcat.-1 (corresponding to 10.5 μg h-1 cm-2) and Faradic efficiency of 4.39% as well as superior stability in alkaline medium, which was superior to that of monometallic Ru and Cu nanostructures. Additionally, this work develops a new bimetallic combination of Ru and Cu, which promotes the strategy to design efficient electrocatalysts for electrochemical ammonia production under ambient conditions.",

keywords = "bimetallic catalysts, electrocatalysis, electrocatalytic reduction of nitrogen, green ammonia synthesis, nanosponge architecture",

author = "Kui Li and Lei Ding and Zhiqiang Xie and Gaoqiang Yang and Shule Yu and Weitian Wang and Cullen, {David A.} and Meyer, {Harry M.} and Guoxiang Hu and Panchapakesan Ganesh and Watkins, {Thomas R.} and Zhang, {Feng Yuan}",

note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

year = "2023",

month = mar,

day = "8",

doi = "10.1021/acsami.2c20809",

language = "English",

volume = "15",

pages = "11703--11712",

journal = "ACS Applied Materials and Interfaces",

issn = "1944-8244",

publisher = "American Chemical Society",

number = "9",

}

Li, K, Ding, L, Xie, Z, Yang, G, Yu, S, Wang, W, Cullen, DA , Meyer, HM, Hu, G, Ganesh, P , Watkins, TR & Zhang, FY 2023, 'Robust Copper-Based Nanosponge Architecture Decorated by Ruthenium with Enhanced Electrocatalytic Performance for Ambient Nitrogen Reduction to Ammonia', ACS Applied Materials and Interfaces, vol. 15, no. 9, pp. 11703-11712. https://doi.org/10.1021/acsami.2c20809

TY - JOUR

T1 - Robust Copper-Based Nanosponge Architecture Decorated by Ruthenium with Enhanced Electrocatalytic Performance for Ambient Nitrogen Reduction to Ammonia

AU - Li, Kui

AU - Ding, Lei

AU - Xie, Zhiqiang

AU - Yang, Gaoqiang

AU - Yu, Shule

AU - Wang, Weitian

AU - Cullen, David A.

AU - Meyer, Harry M.

AU - Hu, Guoxiang

AU - Ganesh, Panchapakesan

AU - Watkins, Thomas R.

AU - Zhang, Feng Yuan

PY - 2023/3/8

Y1 - 2023/3/8

N2 - Electrochemical conversion of nitrogen to green ammonia is an attractive alternative to the Haber-Bosch process. However, it is currently bottlenecked by the lack of highly efficient electrocatalysts to drive the sluggish nitrogen reduction reaction (N2RR). Herein, we strategically design a cost-effective bimetallic Ru-Cu mixture catalyst in a nanosponge (NS) architecture via a rapid and facile method. The porous NS mixture catalysts exhibit a large electrochemical active surface area and enhanced specific activity arising from the charge redistribution for improved activation and adsorption of the activated nitrogen species. Benefiting from the synergistic effect of the Cu constituent on morphology decoration and thermodynamic suppression of the competing hydrogen evolution reaction, the optimized Ru0.15Cu0.85 NS catalyst presents an impressive N2RR performance with an ammonia yield rate of 26.25 μg h-1 mgcat.-1 (corresponding to 10.5 μg h-1 cm-2) and Faradic efficiency of 4.39% as well as superior stability in alkaline medium, which was superior to that of monometallic Ru and Cu nanostructures. Additionally, this work develops a new bimetallic combination of Ru and Cu, which promotes the strategy to design efficient electrocatalysts for electrochemical ammonia production under ambient conditions.

AB - Electrochemical conversion of nitrogen to green ammonia is an attractive alternative to the Haber-Bosch process. However, it is currently bottlenecked by the lack of highly efficient electrocatalysts to drive the sluggish nitrogen reduction reaction (N2RR). Herein, we strategically design a cost-effective bimetallic Ru-Cu mixture catalyst in a nanosponge (NS) architecture via a rapid and facile method. The porous NS mixture catalysts exhibit a large electrochemical active surface area and enhanced specific activity arising from the charge redistribution for improved activation and adsorption of the activated nitrogen species. Benefiting from the synergistic effect of the Cu constituent on morphology decoration and thermodynamic suppression of the competing hydrogen evolution reaction, the optimized Ru0.15Cu0.85 NS catalyst presents an impressive N2RR performance with an ammonia yield rate of 26.25 μg h-1 mgcat.-1 (corresponding to 10.5 μg h-1 cm-2) and Faradic efficiency of 4.39% as well as superior stability in alkaline medium, which was superior to that of monometallic Ru and Cu nanostructures. Additionally, this work develops a new bimetallic combination of Ru and Cu, which promotes the strategy to design efficient electrocatalysts for electrochemical ammonia production under ambient conditions.

KW - bimetallic catalysts

KW - electrocatalysis

KW - electrocatalytic reduction of nitrogen

KW - green ammonia synthesis

KW - nanosponge architecture

UR - http://www.scopus.com/inward/record.url?scp=85148873531&partnerID=8YFLogxK

U2 - 10.1021/acsami.2c20809

DO - 10.1021/acsami.2c20809

M3 - Article

C2 - 36812428

AN - SCOPUS:85148873531

SN - 1944-8244

VL - 15

SP - 11703

EP - 11712

JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

IS - 9

ER -

Robust Copper-Based Nanosponge Architecture Decorated by Ruthenium with Enhanced Electrocatalytic Performance for Ambient Nitrogen Reduction to Ammonia

Abstract

Funding

Keywords

UN SDGs

Access to Document

Other files and links

Fingerprint

Cite this