High yield selective electrochemical conversion of N2 to NH3via morphology controlled silver phosphate under ambient conditions

Gupta, Divyani; Kafle, Alankar; Kaur, Sukhjot; Mohanty, Prajna Parimita; Das, Tisita; Chakraborty, Sudip; Ahuja, Rajeev; Nagaiah, Tharamani C.

doi:10.1039/d2ta04155c

Cited by 15 publications

(31 citation statements)

References 66 publications

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“…Figure plots works that did isotope tests and these are found in SI, Section 3. 3,4,7,25,[27][28][29][30][31][32][33][34][35][36][37][38][39][40][41][42][43] Non-aqueous ENRR. The non-aqueous media-based reports are presented in SI, Table S4.…”

Section: Successful Approaches For Achieving the High Selectivity Of ...mentioning

confidence: 99%

“…Seven aqueous works with Faradaic efficiency above 20% that were assessed as reliable with the reliability indicator are summarized in Table 5. The seven aqueous mediabased ENRR were conducted in a membrane-separated two-compartment cell under ambient conditions, in which the membrane was either proton-exchange or microporous (Nafion 211, 37 Celgard, 33,35 Nafion 117 31,36,38,39 ). The working electrode was a carbon paper 33,35 or a carbon cloth 36,37 deposited with catalyst or fabricated by coating the catalyst to a glassy carbon disc 31,38,39 .…”

Section: Successful Approaches For Achieving the High Selectivity Of ...mentioning

confidence: 99%

“…The seven aqueous mediabased ENRR were conducted in a membrane-separated two-compartment cell under ambient conditions, in which the membrane was either proton-exchange or microporous (Nafion 211, 37 Celgard, 33,35 Nafion 117 31,36,38,39 ). The working electrode was a carbon paper 33,35 or a carbon cloth 36,37 deposited with catalyst or fabricated by coating the catalyst to a glassy carbon disc 31,38,39 . Indeed, gas diffusion electrodes (GDEs) can be used to overcome the diffusion limitations of gaseous reactants in electrochemical reactions, enabling intimate contact between the gas, electrolyte, and catalyst.…”

Section: Successful Approaches For Achieving the High Selectivity Of ...mentioning

confidence: 99%

“…It is possible to achieve the ultimate specific activity with SACs, which contain atomically dispersed metal atoms in support materials. 48 Choi and co-workers 48 39 , which they modified metallic silver with inorganic phosphate to obtain silver phosphate Ag3PO4 catalyst. They applied a complexation-controlled synthetic approach for synthesis which resulted in an effective electrocatalyst for the ENRR in alkaline media under ambient conditions by exhibiting a high Faradaic efficiency of 26.67% at a positive potential of 0 V vs.…”

Section: Successful Approaches For Achieving the High Selectivity Of ...mentioning

confidence: 99%

“…Figure 3-Reliability distribution of reviewed studies in terms of Faradaic efficiency -the green articles are reliable works, the yellow articles are probably reliable, and the red articles are probably non-reliable, assessed using the methodology depicted in Fig 1 and specified in Table3. Figure plots works that did isotope tests and these are found in SI, Section 3 3,4,7,25,[27][28][29][30][31][32][33][34][35][36][37][38][39][40][41][42][43]. …”

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confidence: 99%

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Low-temperature electrochemical ammonia synthesis: measurement reliability and comparison to Haber-Bosch in terms of energy efficiency

Rezai

Læsaa

Şahin

et al. 2023

Preprint

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Recently several studies paved a way to nearly 100% selectivity of the electrochemical ammonia synthesis (EAS), which had been identified earlier as a main challenge. These results motivated us to benchmark the energy efficiency (EE) of EAS against the Haber-Bosch process. We present a method to calculate EE of EAS, which can be used by a broader audience. EAS studies historically suffered from reliability issues, and to avoid benchmarking of false-positive results, we established a method to calculate a reliability indicator to assess the measurement reliability of a published work. We used the indicator to evaluate the studies published in 2020, 2021 and 2022. We calculated the EE of EAS for works that were assessed as reliable with our indicator. We identified and discussed several promising systems and strategies enabling higher selectivity and EE. The EE of some aqueous EAS reports are up to 55%, and non-aqueous are below 15%.

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Section: Successful Approaches For Achieving the High Selectivity Of ...mentioning

confidence: 99%

Section: Successful Approaches For Achieving the High Selectivity Of ...mentioning

confidence: 99%

Section: Successful Approaches For Achieving the High Selectivity Of ...mentioning

confidence: 99%

Section: Successful Approaches For Achieving the High Selectivity Of ...mentioning

confidence: 99%

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confidence: 99%

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Low-temperature electrochemical ammonia synthesis: measurement reliability and comparison to Haber-Bosch in terms of energy efficiency

Rezai

Læsaa

Şahin

et al. 2023

Preprint

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Covalent Organic Framework: An Emerging Catalyst for Renewable Ammonia Production

2023

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Ammonia (NH3), a fertilizer feedstock and clean energy carrier, is produced primarily by the Haber‐Bosch method, which is environmentally hazardous and energy intensive. Therefore, there is an immediate need for a benign alternative, like catalytic nitrogen fixation, such as catalytic nitrogen reduction reaction (NRR). NRR must involve active, selective, scalable, and long‐lived catalysts to become a sustainable source of ammonia production. Recently, covalent organic frameworks (COFs) and COF‐based functional materials have been proposed as promising catalysts for NRR. COFs comprise repeating units of organic molecules connected by strong covalent bonds. By fine‐tuning the building blocks, various COFs can be designed with numerous active sites. This class of materials offers excellent modularity, porosity, stability, and low density. A novel type of nitrogen‐abundant COFs called covalent triazine framework (CTF) has been noted for its high electron density and ultra‐stability. This review examines the state‐of‐the‐art for the NRR using different COF‐based catalysts and discusses design principles for advancing it. The underlying mechanism of NRR with different strategies adopted for renewable ammonia production is also discussed for a clear understanding of the process. Furthermore, key parameters for improving ammonia synthesis‘s photo/electrocatalytic efficiency will also be highlighted to present new possibilities to this emerging field.

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Electrocatalytic Dinitrogen Reduction to Ammonia Using Easily Reducible N‐Fused Cobalt Porphyrins

Ganesan,

Hajiseyedjavadi,

Rathi

et al. 2024

Chemistry A European J

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Single‐site molecular electrocatalysts, especially those that perform catalytic conversion of N2 to NH3 under mild conditions, are highly desirable to derive fundamental structure‐activity relations and as potential alternatives to the current energy‐consuming Haber‐Bosch ammonia production process. Combining theoretical calculations with experimental evidence, it has been shown that easily reducible cobalt porphyrins catalyze the six‐electron, six‐proton reduction of dinitrogen to NH3 at neutral pH and under ambient conditions. Two easily reducible N‐fused cobalt porphyrins – CoNHF and CoNHF(Br)2 – reveal NRR activity with Faradic efficiencies between 6 ‐ 7.5% with ammonia yield rates of 300 ‐ 340 µmol g‐1 h‐1. Contrary to this, much harder‐to‐reduce N‐fused porphyrins – CoNHF(Ph)2 and CoNHF(PE)2 – reveal no NRR activity. The present study highlights the significance of tuning the redox and structural properties of single‐site NRR electrocatalysts for improved NRR activity under mild conditions.

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High yield selective electrochemical conversion of N₂ to NH₃via morphology controlled silver phosphate under ambient conditions

Abstract: Development of highly active catalyst for the synthesis of ammonia via electrochemical dinitrogen reduction (e-NRR) is of immense challenge. We report the modification of metallic Ag with inorganic phosphate to...

Cited by 15 publications

References 66 publications

Low-temperature electrochemical ammonia synthesis: measurement reliability and comparison to Haber-Bosch in terms of energy efficiency

Low-temperature electrochemical ammonia synthesis: measurement reliability and comparison to Haber-Bosch in terms of energy efficiency

Covalent Organic Framework: An Emerging Catalyst for Renewable Ammonia Production

Electrocatalytic Dinitrogen Reduction to Ammonia Using Easily Reducible N‐Fused Cobalt Porphyrins

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