Lattice‐Confined Single‐Atom Fe1Sx on Mesoporous TiO2 for Boosting Ambient Electrocatalytic N2 Reduction Reaction

Chen, Jiayin; Kang, Yikun; Zhang, Wei; Zhang, Zhenghao; Chen, Yan; Yang, Yi; Duan, Linlin; Li, Yefei; Li, Wei

doi:10.1002/ange.202203022

Cited by 15 publications

(1 citation statement)

References 63 publications

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“…25,26 Although the NRR process has the advantages of zero carbon emission and low energy consumption, it suffers from insufficient Faraday efficiency and low NH 3 yield in practical applications. 27−29 Moreover, the high dissociation energy of the extremely inert N−N bond, the difficulty of N 2 adsorption, 30,31 the limited number of active sites of the catalysts, 32 and the presence of competing hydrogenolysis reaction (HER), 33 result in low electrocatalytic activity of electrocatalytic nitrogen reduction to ammonia. 34−36 Therefore, it is important to design NRR catalysts with high activity, durability, and effectiveness.…”

Section: Introductionmentioning

confidence: 99%

Recent Progress and Outlook on Metal Phosphides for Nitrogen Gas Electrocatalytic Ammonia Synthesis

Sun,

Xing,

Song

et al. 2024

Energy Fuels

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Ammonia (NH 3 ) is a significant chemical and carbon-free energy carrier with important applications in industry and agriculture. Ammonia is primarily produced through the Haber−Bosch process (HB), which necessitates high temperatures and pressures, consumes a significant amount of energy, and produces a substantial amount of CO 2 . Electrocatalytic nitrogen reduction (NRR) for ammonia synthesis is a promising alternative to the HB process due to its mild reaction conditions and low energy consumption. However, the low ammonia yields reported for nonmetallic or metallic NRR catalysts are still far from the industrialization needs. In recent years, researchers have discovered that metal phosphides possess easy-to-regulate morphology, good stability, and synergistic properties that enable them to exhibit good electrocatalytic activity for the nitrogen reduction reaction. This emerging research direction has been identified as a promising approach for the development of high-performance NRR electrocatalysts. This article provides an overview of the advancements in the use of metal phosphides for electrocatalytic nitrogen reduction and ammonia synthesis in recent years. It briefly discusses their synthesis methods, structural modulation, and morphology modifications as well as the reaction mechanism and performance in nitrogen reduction reactions. Additionally, it addresses the potential challenges that metal phosphides may encounter in NRR applications and offers insights into future development prospects. This paper aims to propose innovative ideas for designing metal phosphide electrocatalysts to enhance the efficiency of electrocatalytic nitrogen reduction to produce ammonia.

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Section: Introductionmentioning

confidence: 99%

Recent Progress and Outlook on Metal Phosphides for Nitrogen Gas Electrocatalytic Ammonia Synthesis

Sun,

Xing,

Song

et al. 2024

Energy Fuels

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Advancing the Electrochemistry of Gas‐Involved Reactions through Theoretical Calculations and Simulations from Microscopic to Macroscopic

Liu

Wang

et al. 2022

Adv Funct Materials

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Nowadays, gas‐involved electrochemical reactions, such as carbon dioxide reduction reaction (CO2RR), nitrogen reduction reaction (NRR), and hydrogen evolution reaction (HER), have gradually become viable solutions to the global environmental pollution and energy crisis. However, their further development is inseparable from the in‐depth understanding of reaction mechanisms, which are incredibly complicated and cannot be satisfied by experiments alone. In this context, theoretical calculations and simulations are of great significance in establishing composition–structure–activity relationships, providing priceless mechanistic discernment and predicting prospective electrocatalysts and systems. Among them, density functional theory (DFT), molecular dynamics (MD) simulations, and finite element simulation (FES) are emerging as three mature theoretical tools. This paper presents a review of the basic principles and research progress of DFT, MD, and FES to deepen the understanding of CO2RR, NRR, and HER. Some remarkable work around theoretical calculations and simulations are highlighted, including the utilization of DFT to investigate the intrinsic properties of catalysts and MD or FES to restore the whole reaction systems from different temporal and spatial scales. Eventually, to sum up, forward‐looking insights and perspectives on the future optimizations and application modes of the three computational techniques to compensate for their shortcomings and limitations are presented.

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Rigorous Assessment of Cl⁻‐Based Anolytes on Electrochemical Ammonia Synthesis

Hao

Yao

et al. 2022

Advanced Science

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Many challenges in the electrochemical synthesis of ammonia have been recognized with most effort focused on delineating false positives resulting from unidentified sources of nitrogen. However, the influence of oxidizing anolytes on the crossover and oxidization of ammonium during the electrolysis reaction remains unexplored. Here it is reported that the use of analytes containing halide ions (Cl − and Br − ) can rapidly convert the ammonium into N 2 , which further intensifies the crossover of ammonium. Moreover, the extent of migration and oxidation of ammonium is found to be closely associated with external factors, such as applied potentials and the concentration of Cl − . These findings demonstrate the profound impact of oxidizing anolytes on the electrochemical synthesis of ammonia. Based on these results, many prior reported ammonia yield rates are calibrated. This work emphasizes the significance of avoiding selection of anolytes that can oxidize ammonium, which is believed to promote further progress in electrochemical nitrogen fixation.

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Lattice‐Confined Single‐Atom Fe₁S_x on Mesoporous TiO₂ for Boosting Ambient Electrocatalytic N₂ Reduction Reaction

Cited by 15 publications

References 63 publications

Recent Progress and Outlook on Metal Phosphides for Nitrogen Gas Electrocatalytic Ammonia Synthesis

Recent Progress and Outlook on Metal Phosphides for Nitrogen Gas Electrocatalytic Ammonia Synthesis

Advancing the Electrochemistry of Gas‐Involved Reactions through Theoretical Calculations and Simulations from Microscopic to Macroscopic

Rigorous Assessment of Cl⁻‐Based Anolytes on Electrochemical Ammonia Synthesis

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Lattice‐Confined Single‐Atom Fe1Sx on Mesoporous TiO2 for Boosting Ambient Electrocatalytic N2 Reduction Reaction

Cited by 15 publications

References 63 publications

Recent Progress and Outlook on Metal Phosphides for Nitrogen Gas Electrocatalytic Ammonia Synthesis

Recent Progress and Outlook on Metal Phosphides for Nitrogen Gas Electrocatalytic Ammonia Synthesis

Advancing the Electrochemistry of Gas‐Involved Reactions through Theoretical Calculations and Simulations from Microscopic to Macroscopic

Rigorous Assessment of Cl−‐Based Anolytes on Electrochemical Ammonia Synthesis

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Product

Resources

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Lattice‐Confined Single‐Atom Fe₁S_x on Mesoporous TiO₂ for Boosting Ambient Electrocatalytic N₂ Reduction Reaction

Rigorous Assessment of Cl⁻‐Based Anolytes on Electrochemical Ammonia Synthesis