Electrochemical Reduction of Nitrates on CoO Nanoclusters‐Functionalized Graphene with Highest Mass Activity and Nearly 100% Selectivity to Ammonia (Adv. Energy Mater. 17/2023)

Kani, Nishithan C.; Nguyen, Ngoc Hoang Lan; Markel, Kyle; Bhawnani, Rajan; Shindel, Benjamin; Sharma, Kartikey; Kim, Sung-Joon; Dravid, Vinayak P.; Berry, Vikas; Gauthier, Joseph A.; Singh, Meenesh R.

doi:10.1002/aenm.202370069

Cited by 8 publications

(8 citation statements)

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“…[ 9–15 ] More importantly, NO 3 − has become one of the most widely existing water contaminations, arising from the cumulation of agricultural runoffs and the discharging of industrial sewage. [ 16–19 ] Therefore, electrochemical NO 3 RR is a versatile strategy for NH 3 synthesis along with pollutant removal from water bodies.…”

Section: Introductionmentioning

confidence: 99%

Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia

Wang,

Hao,

Sun

et al. 2024

Advanced Materials

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Electrocatalytic nitrate reduction reaction (NO3RR) toward ammonia synthesis is recognized as a sustainable strategy to balance the global nitrogen cycle. However, it still remains a great challenge to achieve highly efficient ammonia production due to the complex proton‐coupled electron transfer process in NO3RR. Here, the controlled synthesis of RuMo alloy nanoflowers (NFs) with unconventional face‐centered cubic (fcc) phase and hexagonal close‐packed/fcc heterophase for highly efficient NO3RR is reported. Significantly, fcc RuMo NFs demonstrate high Faradaic efficiency of 95.2% and a large yield rate of 32.7 mg h−1 mgcat−1 toward ammonia production at 0 and −0.1 V (vs reversible hydrogen electrode), respectively. In situ characterizations and theoretical calculations have unraveled that fcc RuMo NFs possess the highest d‐band center with superior electroactivity, which originates from the strong Ru─Mo interactions and the high intrinsic activity of the unconventional fcc phase. The optimal electronic structures of fcc RuMo NFs supply strong adsorption of key intermediates with suppression of the competitive hydrogen evolution, which further determines the remarkable NO3RR performance. The successful demonstration of high‐performance zinc‐nitrate batteries with fcc RuMo NFs suggests their substantial application potential in electrochemical energy supply systems.

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Section: Introductionmentioning

confidence: 99%

Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia

Wang,

Hao,

Sun

et al. 2024

Advanced Materials

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“…[2] Currently, the mature industrial NH 3 synthesis depends on the energyintensive Haber-Bosch (H-B) process alongside massive CO 2 emission. [3] Electrochemical N 2 /NO 3 À reduction reaction (NRR/ NO 3 RR) to ammonia under mild conditions using renewable electricity is increasingly being investigated as an attractive alternative. [4] Nevertheless, on account of the chemical inertness of N 2 , poor NH 3 yield and Faradaic efficiency (FE) have been achieved via NRR.…”

Section: Introductionmentioning

confidence: 99%

Highly efficient electrochemical ammonia synthesis via nitrate reduction over metallic Cu phase coupling sulfion oxidation

Wang,

Zhou,

Wang

et al. 2024

ChemSusChem

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Electrochemical nitrate reduction reaction (NO3RR) is a promising technology for ammonia production and denitrification of wastewater. Its application is seriously restricted by the development of the highly active and selective electrocatalyst and a rational electrolysis system. Here, we constructed an efficient electrochemical ammonia production process via nitrate reduction on the metallic Cu electrocatalyst when coupled with anodic sulfion oxidation reaction (SOR). The synthesized Cu catalyst delivers an excellent NH3 Faradaic efficiency of 95.6% and a NH3 yield of 0.313 mmol h‐1 cm‐2 at −0.2 V vs. reversible hydrogen electrode, which mainly stem from the more favorable conversion of NO2‐ to NH3 on Cu0. Importantly, the well‐designed electrolysis system with cathodic NO3RR and anodic SOR achieves a dramatically reduced cell voltage of 0.8 V at 50 mA cm‐2 in comparison with the one with anodic oxygen evolution reaction (OER) of 1.9 V. This work presents an effective strategy for the energy‐saving ammonia production via constructing effective nitrate reduction catalyst and replacing the OER with SOR while removing the pollutants including nitrate and sulfion.

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“…Thereinto, electrocatalytic NO 3 À reduction reaction (NO 3 À RR) and NO 2 À reduction reaction (NO 2 À RR) to NH 3 have been extensively studied to improve the reaction activity and NH 3 selectivity. [11][12][13][14][15] Various electrocatalysts have been investigated for electrocatalytic NO 3 À RR and NO 2 À RR, such as some single transition metal catalysts, [16][17][18][19][20][21] or the complexes of noble or non-noble metals with Cu, [22][23][24][25][26][27][28] Co, [4,29] or Ni, [30][31][32] etc. Particularly, Co centers are reported as the active sites to promote H 2 O decomposition to supply sufficient H adsorption (H ads ) for the rapid hydrogenation process of the NH 3 synthesis.…”

Section: Introductionmentioning

confidence: 99%

Gram‐level NH₃ Electrosynthesis via NO_x reduction on a Cu Activated Co Electrode

Liu,

Meng,

Zhu

et al. 2023

Angew Chem Int Ed

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Ambient electrochemical ammonia (NH3) synthesis is one promising alternative to the energy‐intensive Haber‐Bosch route. However, the industrial requirement for the electrochemical NH3 production with amperes current densities or gram‐level NH3 yield remains a grand challenge. Herein, we report the high‐rate NH3 production via NO3‐ and NO2‐ reduction using the Cu activated Co electrode in a bipolar membrane (BPM) assemble electrolyser, wherein BPM maintains the ion balance and the liquid level of electrolyte. Benefited from the abundant activated Co sites and optimal structure, the target CuCo electrode delivers a current density of 2.64 A cm‐2 with the Faradaic efficiency of 96.45% and the high NH3 yield rate of 279.44 mg h‐1 cm‐2 in H‐type cell using alkaline electrolyte. Combined with in‐situ experiments and theoretical calculations, we found that Cu optimizes the adsorption behavior of NO2‐ and facilitates the hydrogenation steps on Co sites toward a rapid NO2‐ reduction process. Importantly, this activated Co electrode affords a large NH3 production up to 4.11 g h‐1 in a homemade reactor, highlighting its large‐scale practical feasibility.

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Electrochemical Reduction of Nitrates on CoO Nanoclusters‐Functionalized Graphene with Highest Mass Activity and Nearly 100% Selectivity to Ammonia (Adv. Energy Mater. 17/2023)

Cited by 8 publications

References 0 publications

Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia

Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia

Highly efficient electrochemical ammonia synthesis via nitrate reduction over metallic Cu phase coupling sulfion oxidation

Gram‐level NH₃ Electrosynthesis via NO_x reduction on a Cu Activated Co Electrode

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Electrochemical Reduction of Nitrates on CoO Nanoclusters‐Functionalized Graphene with Highest Mass Activity and Nearly 100% Selectivity to Ammonia (Adv. Energy Mater. 17/2023)

Cited by 8 publications

References 0 publications

Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia

Crystal Phase Engineering of Ultrathin Alloy Nanostructures for Highly Efficient Electroreduction of Nitrate to Ammonia

Highly efficient electrochemical ammonia synthesis via nitrate reduction over metallic Cu phase coupling sulfion oxidation

Gram‐level NH3 Electrosynthesis via NOx reduction on a Cu Activated Co Electrode

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Gram‐level NH₃ Electrosynthesis via NO_x reduction on a Cu Activated Co Electrode