Insights into electrochemical nitrogen reduction reaction mechanisms: Combined effect of single transition-metal and boron atom

Chen, Xingzhu; Ong, Wee‐Jun; Zhao, Xiujian; Zhang, Peng; Li, Neng

doi:10.1016/j.jechem.2020.10.043

Cited by 76 publications

(39 citation statements)

References 63 publications

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“…The adsorption of N 2 only on Mo 3 Au(111) and Ru 3 Au(111) is thermodynamically spontaneous, while it is non‐spontaneous adsorption on the other six catalysts. It is worth noting that the free energy required for adsorption of N 2 on Mo 3 Au(111) is more negative than the free energy of adsorbed H atom (Δ G *N2 <Δ G *H ), indicating that HER can be significantly inhibited [67–69] . Du and co‐workers proposed that Mo‐Ru, Mo‐Co, Mo‐W, Mo‐Fe, and Fe‐Ru dimers possess high catalytic selectivity toward NRR because of lower free energies of *N 2 than *H [13]…”

Section: Resultsmentioning

confidence: 99%

Theoretical Insights on Au‐based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity

Shi

Xiang

et al. 2021

ChemSusChem

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Electrochemical reduction of nitrogen to produce ammonia at moderate conditions in aqueous solutions holds great prospect but also faces huge challenges. Considering the high selectivity of Au‐based materials to inhibit competitive hydrogen evolution reaction (HER) and high activity of transition metals such as Fe and Mo toward the nitrogen reduction reaction (NRR), it was proposed that Au‐based alloy materials could act as efficient catalysts for N2 fixation based on density functional theory simulations. Only on Mo3Au(111) surface the adsorption of N2 is stronger than H atom. Thermodynamics combined with kinetics studies were performed to investigate the influence of composition and ratio of Au‐based alloys on NRR and HER. The binding energy and reorganization energy affected performance for the initial N2 activation and hydrogenation process. By considering the free‐energy diagram, the computed potential‐determining step was either the first or the fifth hydrogenation step on metal catalysts. The optimum catalytic activity could be achieved by adjusting atomic proportion in alloys to make all intermediate species exhibit moderate adsorption. Free‐energy diagrams of N2 hydrogenation via Langmuir‐Hinshelwood mechanism and hydrogen evolution via Tafel mechanism were compared to reveal that the Mo3Au surface showed satisfactory catalytic performance by simultaneously promoting NRR and suppressing HER. Theoretical simulations demonstrated that Au‐Mo alloy materials could be applied as high‐performance electrocatalysts for NRR.

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Section: Resultsmentioning

confidence: 99%

Theoretical Insights on Au‐based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity

Shi

Xiang

et al. 2021

ChemSusChem

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“…It is the combination of electrochemical and catalyst and has been widely used in oxygen reduction reaction, carbon dioxide reduction reaction, nitrogen reduction reaction (NRR), and so on. [3][4][5][6][7][8][9][10][11][12][13][14][15][16][17][18][19][20] The advantages of electrocatalytic NH 3 synthesis are that water can be used as hydrogen source directly under ambient conditions, the working potential is low, and electric energy can be provided by clean energy to avoid pollution caused by fossil fuel combustion, which is one of the ideal solutions to environmental and energy problems. It has not only important scientific significance but also potential application value and good development prospects.…”

Section: Doi: 101002/adts202100353mentioning

confidence: 99%

First‐Principles Study of 3d Transition Metal Atoms Doped Ni₁₃ Cluster as Efficient Electrocatalyst for Nitrogen Reduction Reaction

Song

Guo

et al. 2021

Advcd Theory and Sims

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Ammonia (NH 3 ), the source compound of all nitrogen-containing chemicals, is not only an important energy storage intermediate and potential energy carrier, but also an essential nitrogen source in fertilizer production. Therefore, it is very essential for agriculture and food production. In recent years, electrocatalytic NH 3 synthesis can be carried out under ambient condition, and clean electric energy can be used to activate nitrogen molecule, which is a technical route with great potential, so it is considered as a promising method. The key problem of electrocatalytic NH 3 synthesis is to design electrocatalysts with high catalytic activity and selectivity. Herein, a series of 3d transition metal (TM = Sc−Zn) atoms doped Ni 13 cluster as electrocatalysts for NH 3 synthesis using density functional theory are designed, and the effects of different TM atoms and active centers on the catalytic performance and reaction mechanism of electrocatalytic NH 3 are explored. The results screen out that Ni 12 V cluster has the best catalytic effect, and the introduction of charges can further reduce the free energy barrier of the nitrogen reduction reaction and effectively inhibit the hydrogen evolution reaction.

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“…[32][33][34][35] To date, a variety of transition metal SACs prepared on carbonaceous substrates have demonstrated outstanding catalytic activities in many reactions, such as hydrogenation, oxygen reduction, nitrogen reduction, and carbon dioxide conversion. [36][37][38][39] Moreover, it has been reported that doping heteroatoms (N, P, or S) into the carbonaceous material can modulate the electronic structure of adjoining sp 2 carbon and boost catalytic performance consequently, and carbon-based materials have been widely employed as supports for SACs to enhance the catalytic performance due to the strong electronic coupling between single atom active sites and carbon substrate, which enables efficient charge transfer between them. [31,40] Our previous study has demonstrated that a catalyst with isolated single Fe atoms of Fe-N 4 coordination anchored on N-doped porous carbon (Fe SA/NPCs) possesses superior catalytic activity on oxygen reduction reaction (ORR).…”

Section: Introductionmentioning

confidence: 99%

Fe Single‐Atom Catalyst for Efficient and Rapid Fenton‐Like Degradation of Organics and Disinfection against Bacteria

Yang

Yang²,

Yin

et al. 2022

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The Fenton‐like reaction has great potential in water treatment. Herein, an efficient and reusable catalytic system is developed based on atomically dispersed Fe catalyst by anchoring Fe atoms on nitrogen‐doped porous carbon (Fe SA/NPCs). The catalyst of Fe SA/NPCs exhibits enhanced performance in activating peroxymonosulfate (PMS) for organic pollutant degradation and bacterial inactivation. The Fe SA/NPCs + PMS system demonstrates a high turnover frequency of 39.31 min−1 in Rhodamine B (RhB) degradation as well as a strong bactericidal activity that can completely sterilize an Escherichia coli culture within 5 min. Meanwhile, the degradation activity of RhB by Fe SA/NPCs is improved up to 28 to 371‐fold in comparison with the controls. Complete degradation of RhB can be achieved in 30 s by the Fe SA/NPCs + PMS system, demonstrating an efficiency much higher than most traditional Fenton‐like processes. Experiments with different radical scavengers and density functional theory calculations have revealed that singlet oxygen (1O2) generated on the N‐coordinated single Fe atom (Fe‐N4) sites is the key reactive species for the effective and rapid pollutant degradation and bacterial inactivation. This work innovatively affords a promising single‐Fe‐atom catalyst/PMS system for applying Fenton‐like reactions in water treatment.

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Insights into electrochemical nitrogen reduction reaction mechanisms: Combined effect of single transition-metal and boron atom

Cited by 76 publications

References 63 publications

Theoretical Insights on Au‐based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity

Theoretical Insights on Au‐based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity

First‐Principles Study of 3d Transition Metal Atoms Doped Ni₁₃ Cluster as Efficient Electrocatalyst for Nitrogen Reduction Reaction

Fe Single‐Atom Catalyst for Efficient and Rapid Fenton‐Like Degradation of Organics and Disinfection against Bacteria

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Insights into electrochemical nitrogen reduction reaction mechanisms: Combined effect of single transition-metal and boron atom

Cited by 76 publications

References 63 publications

Theoretical Insights on Au‐based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity

Theoretical Insights on Au‐based Bimetallic Alloy Electrocatalysts for Nitrogen Reduction Reaction with High Selectivity and Activity

First‐Principles Study of 3d Transition Metal Atoms Doped Ni13 Cluster as Efficient Electrocatalyst for Nitrogen Reduction Reaction

Fe Single‐Atom Catalyst for Efficient and Rapid Fenton‐Like Degradation of Organics and Disinfection against Bacteria

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First‐Principles Study of 3d Transition Metal Atoms Doped Ni₁₃ Cluster as Efficient Electrocatalyst for Nitrogen Reduction Reaction