Insights into the role of cation vacancy for significantly enhanced electrochemical nitrogen reduction

Yang, Xiaohui; Ling, Faling; Su, Jinfeng; Zi, Xiangrong; Zhang, Han; Zhang, Huijuan; Li, Jian; Zhou, Miao; Wang, Yu

doi:10.1016/j.apcatb.2019.118477

Cited by 81 publications

(42 citation statements)

References 48 publications

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“…Compared with the creation of anion defects in transition metal‐based composites, the higher formation energy makes it more challenging to controllably produce cation vacancies in metal compounds. The methods used to create cation defects in metal complexes include in situ formation, [ 93–96 ] thermal calcination, [ 19,97 ] chemical/electrochemical etching, [ 98–100 ] and plasma treatment. [ 75,101,102 ] In this section, the influence of single type of cation defects such as Co, Fe, and Ni vacancies and multivacancies such as oxygen, Fe, and Co vacancies on the electrochemical reactions will be discussed.…”

Section: Cation Defects In Transition Metal Composites For Electrocatmentioning

confidence: 99%

Defective Structures in Metal Compounds for Energy‐Related Electrocatalysis

2020

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Catalysts play a critical role in accelerating the electrochemical reactions. Engineering the electronic structures and surface properties of electrocatalysts is a feasible approach to improve their catalytic performance. Introducing defects such as anion and cation vacancies into transition metal‐based materials to enhance their activity for various energy‐related electrocatalytic reactions has been receiving increasingly attention in recent years. In this review, a systematic summary of the anion and cation defects on different electrochemical reactions will be presented. In particular, the commonly used methods to produce anion vacancies (such as oxygen, sulfur, and phosphorus defects) and cation vacancies (such as Fe, Co, and Ni defects) will be discussed. The control of the defect density and refilling heteroatoms to stabilize the anion defects and simultaneously to further enhance their catalytic performance are also summarized. In addition, recent work on creating multivacancies in transition metal‐based electrocatalysts for maximizing their catalytic activities is reviewed as well. Finally, future research on defect engineering in metal compounds for electrocatalysis is proposed. This review will guide the further development of various energy‐related electrocatalytic reactions promoted by defective structures in metal composites.

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Section: Cation Defects In Transition Metal Composites For Electrocatmentioning

confidence: 99%

Defective Structures in Metal Compounds for Energy‐Related Electrocatalysis

2020

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“…By embedding MoN nanoparticles (NPs) into N-doped hierarchical porous carbon framework, an excellent Mo vacancy electrocatalyst can be obtained. [47] Compared with the previously reported anion-vacancy catalysts, it has a significant increase in electrical activity (NH 3 yield: 76.9 µg h −1 mg cat.…”

Section: Wwwadvmatinterfacesdementioning

confidence: 80%

“…[43] Copyright 2019, Elsevier B.V. d) Reproduced with permission. [47] Copyright 2020, Elsevier B.V. e) Reproduced with permission. [50] Copyright 2020, Elsevier B.V. f) Reproduced with permission.…”

Section: Wwwadvmatinterfacesdementioning

confidence: 99%

Recent Advances in the Application of Structural‐Phase Engineering Strategies in Electrochemical Nitrogen Reduction Reaction

Huang

2020

Adv Materials Inter

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“…In nature, there are three distinguished nitrogenase enzymes with metal‐centered catalytic cofactors of FeMo‐co, FeFe‐co, and VFe‐co, respectively . To mimic the catalytic role of nitrogenase enzymes to achieve the synthesis of NH 3 , a series of potential catalysts containing Fe, Mo, and V elements, including Mo nanofilm, MoS 2 , Mo 2 C, MoO 2 , MoP, MoN, Fe 2 O 3 , FeS x , Fe 3 C, and VN, etc., have been tested for electrochemical NRR under ambient conditions. Recently, both experimental and computational studies showed that a combination of ligand, geometric and synergistic effect of bimetal atoms may facilitate electrochemical NRR .…”

Section: Introductionmentioning

confidence: 99%

Ammonia Synthesis via Electrochemical Nitrogen Reduction Reaction on Iron Molybdate under Ambient Conditions

2020

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The electrochemical nitrogen reduction reaction (NRR) is an environmentally friendly and sustainable strategy for ammonia synthesis under ambient conditions, in comparison with the traditional Haber‐Bosch process. However, the N≡N triple bond has a high bond energy, which causes the electrochemical NRR to suffer from sluggish kinetics. Inevitable ammonia contamination also disturbs the quantification of ammonia produced from the electrochemical NRR. To construct a bimetal‐atom active center to mimic nitrogenase in nature, we herein prepared iron molybdate, Fe2(MoO4)3, using it as catalyst for electrochemical NRR. It is active and stable with an NH3 yield rate of ca. 7.5 µg h–1 mgcat–1 and a Faradaic efficiency of ca. 1.0 % in 0.1 m Na2SO4 at –0.7 V for 2 h, due to synergistic effect of bimetal atoms. A series of comparative experiments were subsequently conducted to reveal the origin of the activity and estimate the deviation due to ammonia contamination from the environment. Our results hold great promise for both the design of catalysts and the accurate quantification of catalytic activity for electrochemical NRR.

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Insights into the role of cation vacancy for significantly enhanced electrochemical nitrogen reduction

Cited by 81 publications

References 48 publications

Defective Structures in Metal Compounds for Energy‐Related Electrocatalysis

Defective Structures in Metal Compounds for Energy‐Related Electrocatalysis

Recent Advances in the Application of Structural‐Phase Engineering Strategies in Electrochemical Nitrogen Reduction Reaction

Ammonia Synthesis via Electrochemical Nitrogen Reduction Reaction on Iron Molybdate under Ambient Conditions

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