Proton-filtering covalent organic frameworks with superior nitrogen penetration flux promote ambient ammonia synthesis

Liu, Sisi; Qian, Tao; Wang, Mengfan; Ji, Haoqing; Shen, Xiaowei; Wang, Chao; Yan, Chenglin

doi:10.1038/s41929-021-00599-w

Cited by 264 publications

(226 citation statements)

References 49 publications

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“…Commercial nitric acid is produced through a two-step procedure including artificial ammonia synthesis and the following catalytic oxidation. [5][6][7][8] NH 3 is usually produced from the Haber-Bosch process, which involves the reaction with H 2 and N 2 under high temperature (400-500 °C) and high pressure (200-300 atm) conditions. [9][10][11][12] HNO 3 is then obtained through NH 3 oxidation (Ostwald process) under harsh reaction conditions (400-600 °C, 150-250 atm).…”

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confidence: 99%

Catalytic Kinetics Regulation for Enhanced Electrochemical Nitrogen Oxidation by Ru‐Nanoclusters‐Coupled Mn₃O₄ Catalysts Decorated with Atomically Dispersed Ru Atoms

et al. 2022

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Electrochemical N2 oxidation reaction (NOR), using water and N2 in the atmosphere, represents a sustainable approach for nitric production to replace the conventional industrial synthesis with high energy consumption and greenhouse gas emission. Meanwhile, owing to chemical inertness of N2 and sluggish kinetics for 10‐electron transfer, emerging electrocatalysts remain largely underexplored. Herein, Ru‐nanoclusters‐coupled Mn3O4 catalysts decorated with atomically dispersed Ru atoms (Ru–Mn3O4) are designed and explored as an advanced electrocatalyst for ambient N2 oxidation, with an excellent Faraday efficiency (28.87%) and a remarkable NO3‐ yield (35.34 µg h‐1 mg‐1cat.), respectively. Experiments and density functional theory calculations reveal that the outstanding activity is ascribed to the coexistence of Ru clusters and single‐atom Ru. The synergistic effect between the Ru clusters and Mn3O4 can effectively activate the chemically inert N2, lowering the kinetic barrier for the vital breakage of N≡N. The intensive *OH supply and enhanced conductivity are used to regulate the catalytic kinetics for optimized performance. This work provides brand‐new ideas for the rational design of electrocatalysts in complicated electrocatalytic reactions with multiple dynamics‐different steps.

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confidence: 99%

Catalytic Kinetics Regulation for Enhanced Electrochemical Nitrogen Oxidation by Ru‐Nanoclusters‐Coupled Mn₃O₄ Catalysts Decorated with Atomically Dispersed Ru Atoms

et al. 2022

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“…Therefore, fewer active sites can be occupied by N 2 than protons due to the unfavorable supplies of nitrogen accompanied by the slow diffusion rate in aqueous electrolyte, resulting in poor NRR activity and selectivity. [10][11][12] Instead, most electrons and protons tend to go toward hydrogen evolution, and the enrichment and overflow of H 2 can further limit the N 2 available in aqueous solutions for catalysts, which would severely lower the efficiency of NRR. [13][14][15][16] Hence, the extremely low solubility of N 2 in aqueous electrolytes, especially under ambient conditions, is an essential bottleneck to further enhance the ammonia production rate and NRR selectivity.…”

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confidence: 99%

Interfacial Microextraction Boosting Nitrogen Feed for Efficient Ambient Ammonia Synthesis in Aqueous Electrolyte

Shen

Liu

Xia

et al. 2022

Adv Funct Materials

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The extremely low nitrogen (N 2 ) solubility in aqueous solution greatly limits the gas reactant supply to catalysts resulting in a bottleneck in establishing efficient electrocatalytic N 2 reduction reaction (NRR). Here, aiming at fairly few N 2 dissolving in aqueous electrolyte, an N 2 -microextractor (NME) that can extract the N 2 from water, then feed it to catalysts on electrodes, is reported. The NME consists of polymer framework and extractant that possess high solubility for N 2 , which serves as an ultra-thin interfacial system wrapping around electrodes. As expected, the enhancement of N 2 supply in NRR leads to a record-high Faradaic efficiency (80.1%) with an ammonia yield rate of 58.3 µg h −1 mg −1 under ambient conditions. This is of great significance to a sustainable "Ammonia Economy.

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“…[1][2][3] However, presently, the Haber-Bosch (HB) process, which is mainly employed to produce NH 3 by reducing N 2 with hydrogen (H 2 ), produces a large amount of greenhouse gas emissions with intensive energy consumption. [4][5][6][7][8] Therefore, there is an urgent need to introduce alternative technologies and explore affordable N 2 fixation methods to replace the traditional HB process. At present, the nitrogen reduction reaction (NRR) is used to produce NH 3 from N 2 via biochemistry, photocatalysis, and electrocatalysis.…”

Section: Introductionmentioning

confidence: 99%

Recent advances in material design and reactor engineering for electrocatalytic ambient nitrogen fixation

Ali

Muhammad

Qian

et al. 2022

Mater. Chem. Front.

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Proton-filtering covalent organic frameworks with superior nitrogen penetration flux promote ambient ammonia synthesis

Cited by 264 publications

References 49 publications

Catalytic Kinetics Regulation for Enhanced Electrochemical Nitrogen Oxidation by Ru‐Nanoclusters‐Coupled Mn₃O₄ Catalysts Decorated with Atomically Dispersed Ru Atoms

Catalytic Kinetics Regulation for Enhanced Electrochemical Nitrogen Oxidation by Ru‐Nanoclusters‐Coupled Mn₃O₄ Catalysts Decorated with Atomically Dispersed Ru Atoms

Interfacial Microextraction Boosting Nitrogen Feed for Efficient Ambient Ammonia Synthesis in Aqueous Electrolyte

Recent advances in material design and reactor engineering for electrocatalytic ambient nitrogen fixation

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Proton-filtering covalent organic frameworks with superior nitrogen penetration flux promote ambient ammonia synthesis

Cited by 264 publications

References 49 publications

Catalytic Kinetics Regulation for Enhanced Electrochemical Nitrogen Oxidation by Ru‐Nanoclusters‐Coupled Mn3O4 Catalysts Decorated with Atomically Dispersed Ru Atoms

Catalytic Kinetics Regulation for Enhanced Electrochemical Nitrogen Oxidation by Ru‐Nanoclusters‐Coupled Mn3O4 Catalysts Decorated with Atomically Dispersed Ru Atoms

Interfacial Microextraction Boosting Nitrogen Feed for Efficient Ambient Ammonia Synthesis in Aqueous Electrolyte

Recent advances in material design and reactor engineering for electrocatalytic ambient nitrogen fixation

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Catalytic Kinetics Regulation for Enhanced Electrochemical Nitrogen Oxidation by Ru‐Nanoclusters‐Coupled Mn₃O₄ Catalysts Decorated with Atomically Dispersed Ru Atoms

Catalytic Kinetics Regulation for Enhanced Electrochemical Nitrogen Oxidation by Ru‐Nanoclusters‐Coupled Mn₃O₄ Catalysts Decorated with Atomically Dispersed Ru Atoms