Highly Selective Electrochemical Nitrate to Ammonia Conversion by Dispersed Ru in a Multielement Alloy Catalyst

Meiqi Yang; Boyang Li; Shuke Li; Qi Dong; Zhennan Huang; Sunxiang Zheng; Ying Fang; Guangye Zhou; Xi Chen; Xiaobo Zhu; Tangyuan Li; Miaofang Chi; Guofeng Wang; Liangbing Hu; Zhiyong Jason Ren

doi:10.1021/acs.nanolett.3c01978

Highly Selective Electrochemical Nitrate to Ammonia Conversion by Dispersed Ru in a Multielement Alloy Catalyst

Meiqi Yang, Boyang Li, Shuke Li, Qi Dong, Zhennan Huang, Sunxiang Zheng, Ying Fang, Guangye Zhou, Xi Chen, Xiaobo Zhu, Tangyuan Li, Miaofang Chi, Guofeng Wang, Liangbing Hu, Zhiyong Jason Ren

electron Microscopy and Microanalysis

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

30 Scopus citations

Abstract

Electrochemical reduction of nitrate to ammonia (NH₃) converts an environmental pollutant to a critical nutrient. However, current electrochemical nitrate reduction operations based on monometallic and bimetallic catalysts are limited in NH₃ selectivity and catalyst stability, especially in acidic environments. Meanwhile, catalysts with dispersed active sites generally exhibit a higher atomic utilization and distinct activity. Herein, we report a multielement alloy nanoparticle catalyst with dispersed Ru (Ru-MEA) with other synergistic components (Cu, Pd, Pt). Density functional theory elucidated the synergy effect of Ru-MEA than Ru, where a better reactivity (NH₃ partial current density of −50.8 mA cm^-2) and high NH₃ faradaic efficiency (93.5%) is achieved in industrially relevant acidic wastewater. In addition, the Ru-MEA catalyst showed good stability (e.g., 19.0% decay in FE_NH3 in three hours). This work provides a potential systematic and efficient catalyst discovery process that integrates a data-guided catalyst design and novel catalyst synthesis for a range of applications.

Original language	English
Pages (from-to)	7733-7742
Number of pages	10
Journal	Nano Letters
Volume	23
Issue number	16
DOIs	https://doi.org/10.1021/acs.nanolett.3c01978
State	Published - Aug 23 2023

Funding

This work was supported by Princeton Catalysis Initiative (PCI). We acknowledge the use of the PRISM Image and Analysis Center (IAC) at Princeton University. B.L. and G.W. acknowledge the support from U.S. National Science Foundation (NSF DMR #1905572). Z.H. and M.C. were supported by the U.S. DOE, Office of BES, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science program. Microscopy work was performed at the Center for Nanophase Materials Sciences, which is a U.S. DOE Office of Science User Facility at Oak Ridge National Laboratory.

Funders	Funder number
Center for Nanophase Materials Sciences
Office of BES
Princeton Catalysis Initiative
National Science Foundation	NSF DMR #1905572
U.S. Department of Energy
Oak Ridge National Laboratory
Princeton University

Keywords

acidic
ammonia
electrochemical nitrate reduction
industrial wastewater
multielement alloy catalyst

UN SDGs

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

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10.1021/acs.nanolett.3c01978

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title = "Highly Selective Electrochemical Nitrate to Ammonia Conversion by Dispersed Ru in a Multielement Alloy Catalyst",

abstract = "Electrochemical reduction of nitrate to ammonia (NH3) converts an environmental pollutant to a critical nutrient. However, current electrochemical nitrate reduction operations based on monometallic and bimetallic catalysts are limited in NH3 selectivity and catalyst stability, especially in acidic environments. Meanwhile, catalysts with dispersed active sites generally exhibit a higher atomic utilization and distinct activity. Herein, we report a multielement alloy nanoparticle catalyst with dispersed Ru (Ru-MEA) with other synergistic components (Cu, Pd, Pt). Density functional theory elucidated the synergy effect of Ru-MEA than Ru, where a better reactivity (NH3 partial current density of −50.8 mA cm-2) and high NH3 faradaic efficiency (93.5%) is achieved in industrially relevant acidic wastewater. In addition, the Ru-MEA catalyst showed good stability (e.g., 19.0% decay in FENH3 in three hours). This work provides a potential systematic and efficient catalyst discovery process that integrates a data-guided catalyst design and novel catalyst synthesis for a range of applications.",

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author = "Meiqi Yang and Boyang Li and Shuke Li and Qi Dong and Zhennan Huang and Sunxiang Zheng and Ying Fang and Guangye Zhou and Xi Chen and Xiaobo Zhu and Tangyuan Li and Miaofang Chi and Guofeng Wang and Liangbing Hu and Ren, {Zhiyong Jason}",

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AU - Yang, Meiqi

AU - Li, Boyang

AU - Li, Shuke

AU - Dong, Qi

AU - Huang, Zhennan

AU - Zheng, Sunxiang

AU - Fang, Ying

AU - Zhou, Guangye

AU - Chen, Xi

AU - Zhu, Xiaobo

AU - Li, Tangyuan

AU - Chi, Miaofang

AU - Wang, Guofeng

AU - Hu, Liangbing

AU - Ren, Zhiyong Jason

PY - 2023/8/23

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N2 - Electrochemical reduction of nitrate to ammonia (NH3) converts an environmental pollutant to a critical nutrient. However, current electrochemical nitrate reduction operations based on monometallic and bimetallic catalysts are limited in NH3 selectivity and catalyst stability, especially in acidic environments. Meanwhile, catalysts with dispersed active sites generally exhibit a higher atomic utilization and distinct activity. Herein, we report a multielement alloy nanoparticle catalyst with dispersed Ru (Ru-MEA) with other synergistic components (Cu, Pd, Pt). Density functional theory elucidated the synergy effect of Ru-MEA than Ru, where a better reactivity (NH3 partial current density of −50.8 mA cm-2) and high NH3 faradaic efficiency (93.5%) is achieved in industrially relevant acidic wastewater. In addition, the Ru-MEA catalyst showed good stability (e.g., 19.0% decay in FENH3 in three hours). This work provides a potential systematic and efficient catalyst discovery process that integrates a data-guided catalyst design and novel catalyst synthesis for a range of applications.

AB - Electrochemical reduction of nitrate to ammonia (NH3) converts an environmental pollutant to a critical nutrient. However, current electrochemical nitrate reduction operations based on monometallic and bimetallic catalysts are limited in NH3 selectivity and catalyst stability, especially in acidic environments. Meanwhile, catalysts with dispersed active sites generally exhibit a higher atomic utilization and distinct activity. Herein, we report a multielement alloy nanoparticle catalyst with dispersed Ru (Ru-MEA) with other synergistic components (Cu, Pd, Pt). Density functional theory elucidated the synergy effect of Ru-MEA than Ru, where a better reactivity (NH3 partial current density of −50.8 mA cm-2) and high NH3 faradaic efficiency (93.5%) is achieved in industrially relevant acidic wastewater. In addition, the Ru-MEA catalyst showed good stability (e.g., 19.0% decay in FENH3 in three hours). This work provides a potential systematic and efficient catalyst discovery process that integrates a data-guided catalyst design and novel catalyst synthesis for a range of applications.

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KW - electrochemical nitrate reduction

KW - industrial wastewater

KW - multielement alloy catalyst

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Highly Selective Electrochemical Nitrate to Ammonia Conversion by Dispersed Ru in a Multielement Alloy Catalyst

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Keywords

UN SDGs

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