The development of catalysts for electrochemical nitrogen reduction toward ammonia: theoretical and experimental advances

Cui, Yuhuan; Sun, Changning; Qu, Yanbin; Dai, Tianyi; Zhou, Hu; Wang, Zhili; Jiang, Qigang

doi:10.1039/d2cc03410g

Cited by 9 publications

(3 citation statements)

References 106 publications

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“…On a broader perspective, the NRR proceeds via two main mechanisms: (a) associative and (b) dissociative, wherein, the associative mechanism could be distal as well as alternating, as shown in figure 2 [19]. In general, electrochemical NRR proceeds via three steps: (a) N 2 molecule adsorption on to the catalyst surface (b) subsequent dissociation of triple bonds along with the hydrogenation process resulting in the formation of ammonia (c) the dissorption of ammonia from the catalyst surface [20]. Based on the process of hydrogenation and sequence of cleavage of triple bond of N 2 , associative and dissociative pathways have been classified.…”

Section: Elementary Steps Of Nrr and Associated Problemsmentioning

confidence: 99%

Interlinking electronic band properties in catalysts with electrochemical nitrogen reduction performance: a direct influence

Biswas,

Samui,

Dey

2024

Electron. Struct.

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The wordwide energy demands and the surge towards a net-zero sustainable society let the researchers set a goal towards the end of carbon cycle. This has enormously exaggerated the electrocatalytic processes such as water splitting, CO2 capture and reduction and nitrogen reduction reaction (NRR) as a safe and green alternative as these involve the utilization of renewable green power. Interestingly, the NH3 produced from NRR has been realized as a future fuel in terms of safer green H2 storage and transportation. Nevertheless, to scale up the NH3 production electrochemically, a benevolent catalyst needs to be developed. More interestingly, the electronic features of the catalyst that actually contribute to the interaction and binding between the adsorbate and reaction intermediates should be analyzed such that these can be tuned based on our requirements to obtain the desired high-standard goals of NH3 synthesis. The current topical review aims to provide an illustrative understanding on the experimental and theoretical descriptors that are likely to influence the electronic structure of catalysts for NRR. We have widely covered a detailed explanation regarding work function, d-band center and electronic effect on the electronic structures of the catalysts. While summarizing the same, we realized that there are several discrepancies in this field, which have not been discussed and could be misleading for the newcomers in the field. Thus, we have briefed the limitations and diverging explanations and have provided a few directions that could be looked upon to overcome the issues.

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Section: Elementary Steps Of Nrr and Associated Problemsmentioning

confidence: 99%

Interlinking electronic band properties in catalysts with electrochemical nitrogen reduction performance: a direct influence

Biswas,

Samui,

Dey

2024

Electron. Struct.

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“…The reason for ammonia's popularity lies in its widespread applications ranging from the production of nitric acid and fertilizers to explosives and synthetic fibers. [ 1 ] Additionally, ammonia can be also exploited for the storage and transport of energy due to its high energy density of 3 kWh L −1 . [ 2 ] The Haber‐Bosch process, although developed in the early 20th century, is still the most significant process for producing ammonia on an industrial scale using nitrogen and hydrogen gases.…”

Section: Introductionmentioning

confidence: 99%

Tailored Metal‐Porphyrin Based Molecular Electrocatalysts for Enhanced Artificial Nitrogen Fixation to Green Ammonia

Salerno,

Bettucci,

Manfredi

et al. 2024

Global Challenges

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Electrochemical nitrogen reduction (E‐NRR) is one of the most promising approaches to generate green NH3. However, scarce ammonia yields and Faradaic efficiencies (FE) still limit their use on a large scale. Thus, efforts are focusing on different E‐NRR catalyst structures and formulations. Among present strategies, molecular electrocatalysts such as metal‐porphyrins emerge as an encouraging option due to their planar structures which favor the interaction involving the metal center, responsible for adsorption and activation of nitrogen. Nevertheless, the high hydrophobicity of porphyrins limits the aqueous electrolyte–catalyst interaction lowering yields. This work introduces a new class of metal‐porphyrin based catalysts, bearing hydrophilic tris(ethyleneglycol) monomethyl ether chains (metal = Cu(II) and CoII)). Experimental results show that the presence of hydrophilic chains significantly increases ammonia yields and FE, supporting the relevance of fruitful catalyst‐electrolyte interactions. This study also investigates the use of hydrophobic branched alkyl chains for comparison, resulting in similar performances with respect to the unsubstituted metal‐porphyrin, taken as a reference, further confirming that the appropriate design of electrocatalysts carrying peripheral hydrophilic substituents is able to improve device performances in the generation of green ammonia.

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“…7 As a promising alternative to the H-B method, electrochemical nitrogen (N 2 ) reduction to NH 3 using water as the hydrogen source and electricity as the impetus has been considered as a green and sustainable avenue. [8][9][10][11][12][13][14][15][16][17][18][19][20][21][22] However, its broad application is seriously impeded due to (1) the hard cleavage of NRN and (2) the ultralow aqueous solubility of N 2 , (3) the competition of the hydrogen evolution reaction (HER), which cause the unsatisfactory faradaic efficiency (FE) and NH 3 yield of the N 2 -to-NH 3 process. In contrast to N 2 , the low dissociation energy of the NQO bond and the high solubility of NO 3 À in aqueous media make it more favorable to synthesize NH 3 .…”

mentioning

confidence: 99%

Co/N-doped carbon nanospheres derived from an adenine-based metal organic framework enabled high-efficiency electrocatalytic nitrate reduction to ammonia

Chen

Gong²,

Hou³

et al. 2022

Chem. Commun.

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The development of catalysts for electrochemical nitrogen reduction toward ammonia: theoretical and experimental advances

Abstract: Ammonia (NH3) is essential for the production of fertilizers, pharmaceuticals, plastics, synthetic fibers, resins, and chemicals in industry and is also a promising carbon free energy carrier. The electrocatalytic nitrogen...

Cited by 9 publications

References 106 publications

Interlinking electronic band properties in catalysts with electrochemical nitrogen reduction performance: a direct influence

Interlinking electronic band properties in catalysts with electrochemical nitrogen reduction performance: a direct influence

Tailored Metal‐Porphyrin Based Molecular Electrocatalysts for Enhanced Artificial Nitrogen Fixation to Green Ammonia

Co/N-doped carbon nanospheres derived from an adenine-based metal organic framework enabled high-efficiency electrocatalytic nitrate reduction to ammonia

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