Defect engineering for electrochemical nitrogen reduction reaction to ammonia

Yang, Chenhuai; Zhu, Yating; Liu, Jiaqi; Qin, Yuchen; Wang, Haiqing; Liu, Huiling; Chen, Yanan; Zhang, Zhicheng; Hu, Wenping

doi:10.1016/j.nanoen.2020.105126

Cited by 173 publications

(118 citation statements)

References 155 publications

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“…The electrochemical reduction of N 2 to NH 3 occurring at the heterogeneous catalyst surface typically follows the dissociative pathway, the associative alternating pathway and the associative distal pathway according to the different intermediates involved during electrocatalysis. [148] Therefore, developing electrocatalyst with high performances, in terms of yield and Faradaic efficiency, for NRR becomes the key segment in this high technology. [149][150][151] This depends on the catalyst composition and structure design to effectively adsorb and activate N 2 and retard the competition of kinetically favorable HER.…”

Section: Application Of Ceo -Based Electrocatalysts In Nrrmentioning

confidence: 99%

“…From the perspective of kinetic barrier, there is a large energy gap between the highest occupied and the lowest unoccupied orbitals, which is not conducive to the electron transfer reaction. The electrochemical reduction of N 2 to NH 3 occurring at the heterogeneous catalyst surface typically follows the dissociative pathway, the associative alternating pathway and the associative distal pathway according to the different intermediates involved during electrocatalysis [148] . Therefore, developing electrocatalyst with high performances, in terms of yield and Faradaic efficiency, for NRR becomes the key segment in this high technology [149–151] .…”

Section: Application Of Ceo2‐based Electrocatalysts In Nrrmentioning

confidence: 99%

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Recent Advances of CeO₂‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

2021

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wards the oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and nitrogen reduction reaction (NRR) are summarized. This Review also highlights the key role of CeO 2 and the structural design strategies in the hybrid electrocatalysts, including ion doping, interface and defect engineering, electronic structure optimization, and morphology control for catalytic output enhancement. Lastly, some scientific challenges and perspectives have been proposed, aiming to promote the development of other CeO 2-based hybrids for energy related electrocatalysis.

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Section: Application Of Ceo -Based Electrocatalysts In Nrrmentioning

confidence: 99%

Section: Application Of Ceo2‐based Electrocatalysts In Nrrmentioning

confidence: 99%

Recent Advances of CeO₂‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

2021

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“…Thanks to the large number of unsaturated coordination, facets with low‐coordinated atoms display higher surface energies and thus greater reactivity than low‐energy facets. [ 203 ] Lai et al designed and synthesized a series of Cr 2 O 3 catalysts with different fractions of high energy facet by introducing TiO 2 as inhibitor to inhibit the growth of low energy facets (i.e., {012} Cr 2 O 3 ). [ 204 ] It mainly gives the credit to the small lattice mismatch (3.4%) between the dominating facet (101) TiO 2 and the low‐energy facets of Cr 2 O 3 (Figure 7b).…”

Section: Cathodementioning

confidence: 99%

Challenges and Strategy on Parasitic Reaction for High‐Performance Nonaqueous Lithium–Oxygen Batteries

Zhang

Ding

et al. 2020

Advanced Energy Materials

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is restricted to their inferior energy densities (≈250 Wh kg −1) due to intercalation chemistry. Consequently, "beyond Li-ion batteries" such as lithium-sulfur batteries and metal-air batteries, which have fundamental discrepant energy storage mechanism, have been attracted worldwide attention recently. [4,5] Of all the candidates, rechargeable lithium-oxygen battery (LOB) is considered to be one of the most fascinating next-generation batteries with extremely high theoretical energy density (≈3500 Wh kg −1). [6,7] The low-cost and environmental positive active material oxygen originates from air, endowing LOBs more attractive to satisfy the soaring demand of large-scale energy storage system. Generally, there are four architecture systems of LOBs determined by different electrolyte: aqueous, nonaqueous, hybrid, and all-solid-state. [8-11] In 1996, Abraham and Jiang first reported the rechargeable lithium-oxygen battery consisted of Li metal anode, solid polymer electrolyte membrane, and composite carbon cathode. [12] After ten years, nonaqueous LOBs actually caught worldwide attention due to the outstanding capacity and reversibility. [6] A typical nonaqueous lithium-oxygen battery comprises a metallic Li anode, organic electrolyte containing Li salt, a separator, and a porous gas diffusion cathode loading with catalysts (Figure 1). [13] Generally, the electrochemical reactions of nonaqueous lithium-oxygen battery can be described as following equations [14-16] Overall reaction E 2Li O Li O 2.96 V vs Li/Li 2 2 2 () + ↔°= + (1) Cathodic process (oxygen reduction reaction (ORR))

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“…Nitrogen conversion is a crucial reaction for many products such as fertilizers, drugs as well as chemicals [101][102][103][104] . Thanks to the difficulty of activation of the inertness of the triple bonds, nitrogen conversion is hard to achieve under ambient conditions.…”

Section: Nitrogen Reduction Reaction (Nrr)mentioning

confidence: 99%

Conductive Metal-Organic Frameworks for Electrocatalysis：Achievements, Challenges, and Opportunities

Gao¹,

Wang²,

Li³

et al. 2020

Acta Physico Chimica Sinica

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To fulfill the demands of green and sustainable energy, the production of novel catalysts for different energy conversion processes is critical. Owing to the intriguing advantages of the intrinsic active species, tunable crystal structure, remarkable chemical and physical properties, and good stability, metal-organic frameworks (MOFs) have been extensively investigated in various electrochemical energy conversions, such as the CO2 reduction reaction, N2 reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, and oxygen reduction reaction. More importantly, it is feasible to change the chemical environments, pore sizes, and porosity of MOFs, which will theoretically facilitate the diffusion of reactants across the open porous networks, thereby improving the electrocatalytic performance. However, owing to the high energy barriers of charge transfer and limited free charge carriers, most MOFs show poor electrical conductivity, thus limiting their diverse applications. As reported previously, MOFs were used as a porous substrate to confine the growth of nanoparticles or co-doped electrocatalysts after annealing. The conductive MOFs can combine the advantages of conventional MOFs with electronic conductivity, which significantly enhance the electrocatalytic performance. In addition, conductive MOFs can achieve conductivity via electronic or ionic routes without post-annealing treatment, thereby extending their potential applications. Different synthesis strategies have recently been developed to endow MOFs with electrical conductivity, such as post-synthesis modification, guest molecule introduction, and composite formatting. The performance of conductive MOFs can even outperform those of commercial RuO2 catalysts or Pt-group catalysts. However, it is difficult to endow most MOFs with high conductivity. This review summarizes the mechanisms of constructing conductive MOFs, such as redox hopping, through-bond pathways, through-space pathways, extended conjugation, and guest-promoted transport. Synthetic methods, including hydro/solvothermal synthesis and interface-assisted synthesis, are introduced. Recent advances in the use of conductive MOFs as heterogeneous catalysts in electrocatalysis have been comprehensively elucidated. It has been reported that conductive MOFs can demonstrate considerable catalytic activity, selectivity, and stability in different electrochemical reactions, revealing the immense potential for future displacement of Pt-group catalysts. Finally, the challenges and opportunities of conductive MOFs in electrocatalysis are discussed. Based on systematic synthesis strategies, more conductive MOFs can be constructed for electrocatalytic reactions. In addition, the morphology and structure of conductive MOFs, which can change the electrochemical accessibility between substrates and MOFs, are also crucial for catalysis, and thus, they should be extensively studied in the future. It is believed that a breakthrough for high-performance conductive MOF-based electrocatalysts could be ac...

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Defect engineering for electrochemical nitrogen reduction reaction to ammonia

Cited by 173 publications

References 155 publications

Recent Advances of CeO₂‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

Recent Advances of CeO₂‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

Challenges and Strategy on Parasitic Reaction for High‐Performance Nonaqueous Lithium–Oxygen Batteries

Conductive Metal-Organic Frameworks for Electrocatalysis：Achievements, Challenges, and Opportunities

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Defect engineering for electrochemical nitrogen reduction reaction to ammonia

Cited by 173 publications

References 155 publications

Recent Advances of CeO2‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

Recent Advances of CeO2‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

Challenges and Strategy on Parasitic Reaction for High‐Performance Nonaqueous Lithium–Oxygen Batteries

Conductive Metal-Organic Frameworks for Electrocatalysis：Achievements, Challenges, and Opportunities

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Product

Resources

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Recent Advances of CeO₂‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction

Recent Advances of CeO₂‐Based Electrocatalysts for Oxygen and Hydrogen Evolution as well as Nitrogen Reduction