Electrochemical C–N coupling of CO<sub>2</sub>and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds

Peng, Xianyun; Zeng, Libin; Wang, Dashuai; Liu, Zhibin; Li, Yan; Li, Zhongjian; Yang, Bin; Lei, Lecheng; Dai, Liming; Hou, Yang

doi:10.1039/d2cs00381c

Cited by 106 publications

(52 citation statements)

References 311 publications

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“…For example, the electrochemical C–N coupling of CO 2 and nitrogenous small molecules ( e.g. NO and NO 2 ) can simultaneously eliminate greenhouse gas emissions and environmental pollutants; 106 the CO 2 electrochemical reduction on Cu-based catalysts can produce other high-value products ( e.g. ethylene or ethanol) under ambient conditions.…”

Section: Perspectivesmentioning

confidence: 99%

Copper-based catalysts for CO₂ hydrogenation: a perspective on active sites

Shi¹,

Ma²,

Liu³

2023

EES. Catal.

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Section: Perspectivesmentioning

confidence: 99%

Copper-based catalysts for CO₂ hydrogenation: a perspective on active sites

Shi¹,

Ma²,

Liu³

2023

EES. Catal.

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“…Therefore, summarizing past research work will understand the hardships faced in this territory and have a zealous and far-reaching impact on the future of the field. Up to now, although some good review work has discussed the electrochemical C─N coupling reaction, they have limitations in understanding this field fully and deeply; for example, only focusing on the synthesis of urea 39,40 ; or using sole CO 2 as a carbon source [41][42][43][44] ; and lacking indepth summary on the design of electrocatalysts and the mechanism of C─N coupling. 24 However, the utilization of biomass serves as a valuable complement to CO 2 conversion.…”

Section: Introductionmentioning

confidence: 99%

Toward effective electrocatalytic C–N coupling for the synthesis of organic nitrogenous compounds using CO₂ and biomass as carbon sources

Jiang,

Wu,

Zhang

et al. 2023

SusMat

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Thermochemical conversion of fossil resources into fuels, chemicals, and materials has rapidly increased atmospheric CO2 levels, hindering global efforts toward achieving carbon neutrality. With the increasing push for sustainability, utilizing electrochemical technology to transform CO2 or biomass into value‐added chemicals and to close the carbon cycle with sustainable energy sources represents a promising strategy. Expanding the scope of electrosynthesis technology is a prerequisite for the electrification of chemical manufacturing. To this end, constructing the C─N bond is considered a priority. However, a systematic review of electrocatalytic processes toward building C─N bonds using CO2 and biomass as carbon sources is not available. Accordingly, this review highlights the research progress in the electrosynthesis of organic nitrogen compounds from CO2 and biomass by C─N coupling reactions in view of catalytic materials, focusing on the enlightenment of traditional catalysis on C─N coupling and the understanding of the basis of electrochemical C─N coupling. The possibility of C─N bond in electrocatalysis is also examined from the standpoints of activation of substrates, coupling site, mechanism, and inhibition of hydrogen evolution reaction (HER). Finally, the challenges and prospects of electrocatalytic C─N coupling reactions with improved efficiency and selectivity for future development are discussed.

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“…As an important carrier of nitrogen energy, nitrogen oxide (NO) is predominantly utilized as an alternative precursor for ammonia (NH 3 ) synthesis to avoid dissociating the inert NN bond in N 2 molecules. − Since the 1990s, many advanced approaches, by the application of electro-, photo-, and plasmon-driven routes, have been developed to conduct the NO reduction reaction (NORR) for its value-added conversion under ambient conditions. − Although the NH 3 synthesis rate from NORR is significantly promoted in recent literature, − the key challenge still lies in that the conversion ratio of NO is far below practicability as a result of the ultralow solubility of NO in reaction solutions. Unlike harmless N 2 that is the feedstock for Haber–Bosch NH 3 synthesis, NO is one of the major air pollutants. − That is, the limited conversion ratio of the current NORR route would potentially contribute more to the emission of the contaminant than to its upcycling.…”

Section: Introductionmentioning

confidence: 99%

Continuous NO Upcycling into Ammonia Promoted by SO₂ in Flue Gas: Poison Can Be a Gift

Chen

Wang

et al. 2023

Environ. Sci. Technol.

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Although ammonia (NH3) synthesis efficiency from the NO reduction reaction (NORR) is significantly promoted in recent years, one should note that NO is one of the major air pollutants in the flue gas. The limited NO conversion ratio is still the key challenge for the sustainable development of the NORR route, which potentially contributes more to contaminant emissions rather than its upcycling. Herein, we provide a simple but effective approach for continuous NO reduction into NH3, promoted by coexisting SO2 poison as a gift in the flue gas. It is significant to discover that SO2 plays a decisive role in elevating the capacity of NO absorption and reduction. A unique redox pair of SO2–NO is constructed, which contributes to the exceptionally high conversion ratio for both NO (97.59 ± 1.42%) and SO2 (99.24 ± 0.49%) in a continuous flow. The ultrahigh selectivity for both NO-to-NH3 upcycling (97.14 ± 0.55%) and SO2-to-SO4 2– purification (92.44 ± 0.71%) is achieved synchronously, demonstrating strong practicability for the value-added conversion of air contaminants. The molecular mechanism is revealed by comprehensive in situ technologies to identify the essential contribution of SO2 to NO upcycling. Besides, realistic practicality is realized by the efficient product recovery and resistance ability against various poisoning effects. The proposed strategy in this work not only achieves a milestone efficiency for NH3 synthesis from the NORR but also raises great concerns about contaminant resourcing in realistic conditions.

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Electrochemical C–N coupling of CO₂and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds

Abstract: Electrochemical C–N coupling reaction by renewable electricity for the electrosynthesis of organonitrogen compounds with the abundant CO2 and nitrogenous small molecules as carbon and nitrogen sources, respectively, is a promising sustainable synthetic strategy.

Cited by 106 publications

References 311 publications

Copper-based catalysts for CO₂ hydrogenation: a perspective on active sites

Copper-based catalysts for CO₂ hydrogenation: a perspective on active sites

Toward effective electrocatalytic C–N coupling for the synthesis of organic nitrogenous compounds using CO₂ and biomass as carbon sources

Continuous NO Upcycling into Ammonia Promoted by SO₂ in Flue Gas: Poison Can Be a Gift

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Electrochemical C–N coupling of CO2and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds

Abstract: Electrochemical C–N coupling reaction by renewable electricity for the electrosynthesis of organonitrogen compounds with the abundant CO2 and nitrogenous small molecules as carbon and nitrogen sources, respectively, is a promising sustainable synthetic strategy.

Cited by 106 publications

References 311 publications

Copper-based catalysts for CO2 hydrogenation: a perspective on active sites

Copper-based catalysts for CO2 hydrogenation: a perspective on active sites

Toward effective electrocatalytic C–N coupling for the synthesis of organic nitrogenous compounds using CO2 and biomass as carbon sources

Continuous NO Upcycling into Ammonia Promoted by SO2 in Flue Gas: Poison Can Be a Gift

Contact Info

Product

Resources

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Electrochemical C–N coupling of CO₂and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds

Copper-based catalysts for CO₂ hydrogenation: a perspective on active sites

Copper-based catalysts for CO₂ hydrogenation: a perspective on active sites

Toward effective electrocatalytic C–N coupling for the synthesis of organic nitrogenous compounds using CO₂ and biomass as carbon sources

Continuous NO Upcycling into Ammonia Promoted by SO₂ in Flue Gas: Poison Can Be a Gift