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

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

doi:10.1021/acsami.2c20809

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

Journal Article · Tue Feb 21 23:00:00 EST 2023 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.2c20809· OSTI ID:1987780

^[1]; Ding, Lei ^[1]; Xie, Zhiqiang ^[1]; Yang, Gaoqiang ^[1]; Yu, Shule ^[1]; Wang, Weitian ^[1]; ^[2]; ^[3]; ^[2]; ^[2]; ^[4]; ^[1]

Univ. of Tennessee Space Inst. (UTSI), Tullahoma, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division

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). In this work, 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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC); USDOE Office of Nuclear Energy (NE)

Grant/Contract Number:: AC05-00OR22725; EE0008426; EE0008423; FE0011585

OSTI ID:: 1987780

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 9 Vol. 15; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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

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