Near-Unity Nitrate to Ammonia conversion via reactant enrichment at the solid-liquid interface

Electroreduction of nitrate (NO 3 ‒ ) to ammonia (NH 3 ) is a promising approach for addressing energy challenges. However, the activity is limited by NO 3 ‒ mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO 3 ‒ from the inner Helmho...

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Published in	Nature communications Vol. 16; no. 1; pp. 5715 - 12
Main Authors	Liao, Wanru, Wang, Jun, Tan, Yao, Zi, Xin, Liu, Changxu, Wang, Qiyou, Zhu, Li, Kao, Cheng-Wei, Chan, Ting-Shan, Li, Hongmei, Zhang, Yali, Liu, Kang, Cai, Chao, Fu, Junwei, Xi, Beidou, Cortés, Emiliano, Chai, Liyuan, Liu, Min
Format	Journal Article
Language	English
Published	London Nature Publishing Group UK 01.07.2025 Nature Publishing Group Nature Portfolio
Subjects	119/118 147/135 147/143 639/301/299/886 639/638/169/896 639/638/675 639/638/77/887 Agricultural production Ammonia Carbon Efficiency Electrolytes Electrowinning Energy Enrichment Groundwater Humanities and Social Sciences Liquid-solid interfaces Mass transfer Molybdenum disulfide Morphology multidisciplinary Nitrates Scanning electron microscopy Science Science (multidisciplinary) Silver
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Abstract	Electroreduction of nitrate (NO 3 ‒ ) to ammonia (NH 3 ) is a promising approach for addressing energy challenges. However, the activity is limited by NO 3 ‒ mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO 3 ‒ from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO 3 ‒ concentration decreases, impeding practical applications in the conversion of NO 3 ‒ -to-NH 3 . Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO 3 ‒ reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS 2 (Ag-MoS 2 ) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO 3 ‒ . Thus, Ag-MoS 2 exhibits a ~ 28.6-fold NO 3 ‒ concentration in the IHP than the counterpart without junction, and achieves near-100% NH 3 Faradaic efficiency with an NH 3 yield rate of ~20 mg h ‒1 cm ‒2 under ultralow NO 3 ‒ concentrations. Electroreduction of low-concentration NO 3 − to NH 3 is limited by NO 3 − mass transfer. Here, the authors propose a strategy for NO 3 − enrichment through charge rearrangement within the inner Helmholtz plane, achieving near-unity conversion of NO 3 − to NH 3 .
AbstractList	Electroreduction of nitrate (NO 3 ‒ ) to ammonia (NH 3 ) is a promising approach for addressing energy challenges. However, the activity is limited by NO 3 ‒ mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO 3 ‒ from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO 3 ‒ concentration decreases, impeding practical applications in the conversion of NO 3 ‒ -to-NH 3 . Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO 3 ‒ reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS 2 (Ag-MoS 2 ) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO 3 ‒ . Thus, Ag-MoS 2 exhibits a ~ 28.6-fold NO 3 ‒ concentration in the IHP than the counterpart without junction, and achieves near-100% NH 3 Faradaic efficiency with an NH 3 yield rate of ~20 mg h ‒1 cm ‒2 under ultralow NO 3 ‒ concentrations. Electroreduction of low-concentration NO 3 − to NH 3 is limited by NO 3 − mass transfer. Here, the authors propose a strategy for NO 3 − enrichment through charge rearrangement within the inner Helmholtz plane, achieving near-unity conversion of NO 3 − to NH 3 . Abstract Electroreduction of nitrate (NO3 ‒) to ammonia (NH3) is a promising approach for addressing energy challenges. However, the activity is limited by NO3 ‒ mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO3 ‒ from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO3 ‒ concentration decreases, impeding practical applications in the conversion of NO3 ‒-to-NH3. Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO3 ‒ reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS2 (Ag-MoS2) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO3 ‒. Thus, Ag-MoS2 exhibits a ~ 28.6-fold NO3 ‒ concentration in the IHP than the counterpart without junction, and achieves near-100% NH3 Faradaic efficiency with an NH3 yield rate of ~20 mg h‒1 cm‒2 under ultralow NO3 ‒ concentrations. Electroreduction of nitrate (NO3‒) to ammonia (NH3) is a promising approach for addressing energy challenges. However, the activity is limited by NO3‒ mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO3‒ from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO3‒ concentration decreases, impeding practical applications in the conversion of NO3‒-to-NH3. Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO3‒ reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS2 (Ag-MoS2) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO3‒. Thus, Ag-MoS2 exhibits a ~ 28.6-fold NO3‒ concentration in the IHP than the counterpart without junction, and achieves near-100% NH3 Faradaic efficiency with an NH3 yield rate of ~20 mg h‒1 cm‒2 under ultralow NO3‒ concentrations.Electroreduction of nitrate (NO3‒) to ammonia (NH3) is a promising approach for addressing energy challenges. However, the activity is limited by NO3‒ mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO3‒ from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO3‒ concentration decreases, impeding practical applications in the conversion of NO3‒-to-NH3. Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO3‒ reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS2 (Ag-MoS2) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO3‒. Thus, Ag-MoS2 exhibits a ~ 28.6-fold NO3‒ concentration in the IHP than the counterpart without junction, and achieves near-100% NH3 Faradaic efficiency with an NH3 yield rate of ~20 mg h‒1 cm‒2 under ultralow NO3‒ concentrations. Electroreduction of nitrate (NO ) to ammonia (NH ) is a promising approach for addressing energy challenges. However, the activity is limited by NO mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO concentration decreases, impeding practical applications in the conversion of NO -to-NH . Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS (Ag-MoS ) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO . Thus, Ag-MoS exhibits a ~ 28.6-fold NO concentration in the IHP than the counterpart without junction, and achieves near-100% NH Faradaic efficiency with an NH yield rate of ~20 mg h cm under ultralow NO concentrations. Electroreduction of nitrate (NO3‒) to ammonia (NH3) is a promising approach for addressing energy challenges. However, the activity is limited by NO3‒ mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO3‒ from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO3‒ concentration decreases, impeding practical applications in the conversion of NO3‒-to-NH3. Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO3‒ reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS2 (Ag-MoS2) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO3‒. Thus, Ag-MoS2 exhibits a ~ 28.6-fold NO3‒ concentration in the IHP than the counterpart without junction, and achieves near-100% NH3 Faradaic efficiency with an NH3 yield rate of ~20 mg h‒1 cm‒2 under ultralow NO3‒ concentrations.Electroreduction of low-concentration NO3− to NH3 is limited by NO3− mass transfer. Here, the authors propose a strategy for NO3− enrichment through charge rearrangement within the inner Helmholtz plane, achieving near-unity conversion of NO3− to NH3. Electroreduction of nitrate (NO 3 ‒ ) to ammonia (NH 3 ) is a promising approach for addressing energy challenges. However, the activity is limited by NO 3 ‒ mass transfer, particularly at reduction potential, where an abundance of electrons on the cathode surface repels NO 3 ‒ from the inner Helmholtz plane (IHP). This constraint becomes pronounced as NO 3 ‒ concentration decreases, impeding practical applications in the conversion of NO 3 ‒ -to-NH 3 . Herein, we propose a generic strategy of catalyst bandstructure engineering for the enrichment of negatively charged ions through solid-liquid (S-L) junction-mediated charge rearrangement within IHP. Specifically, during NO 3 ‒ reduction, the formation of S-L junction induces hole transfer from Ag-doped MoS 2 (Ag-MoS 2 ) to electrode/electrolyte interface, triggering abundant positive charges on the IHP to attract NO 3 ‒ . Thus, Ag-MoS 2 exhibits a ~ 28.6-fold NO 3 ‒ concentration in the IHP than the counterpart without junction, and achieves near-100% NH 3 Faradaic efficiency with an NH 3 yield rate of ~20 mg h ‒1 cm ‒2 under ultralow NO 3 ‒ concentrations.
ArticleNumber	5715
Author	Liu, Changxu Tan, Yao Xi, Beidou Zi, Xin Chan, Ting-Shan Cortés, Emiliano Kao, Cheng-Wei Wang, Jun Liu, Min Liao, Wanru Wang, Qiyou Cai, Chao Zhang, Yali Zhu, Li Li, Hongmei Liu, Kang Fu, Junwei Chai, Liyuan
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Snippet	Electroreduction of nitrate (NO 3 ‒ ) to ammonia (NH 3 ) is a promising approach for addressing energy challenges. However, the activity is limited by NO 3 ‒... Electroreduction of nitrate (NO 3 ‒ ) to ammonia (NH 3 ) is a promising approach for addressing energy challenges. However, the activity is limited by NO 3 ‒... Electroreduction of nitrate (NO ) to ammonia (NH ) is a promising approach for addressing energy challenges. However, the activity is limited by NO mass... Electroreduction of nitrate (NO3‒) to ammonia (NH3) is a promising approach for addressing energy challenges. However, the activity is limited by NO3‒ mass... Abstract Electroreduction of nitrate (NO3 ‒) to ammonia (NH3) is a promising approach for addressing energy challenges. However, the activity is limited by NO3...
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SubjectTerms	119/118 147/135 147/143 639/301/299/886 639/638/169/896 639/638/675 639/638/77/887 Agricultural production Ammonia Carbon Efficiency Electrolytes Electrowinning Energy Enrichment Groundwater Humanities and Social Sciences Liquid-solid interfaces Mass transfer Molybdenum disulfide Morphology multidisciplinary Nitrates Scanning electron microscopy Science Science (multidisciplinary) Silver
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Title	Near-Unity Nitrate to Ammonia conversion via reactant enrichment at the solid-liquid interface
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