Carbon-nitrogen bond formation on Cu electrodes during CO2 reduction in NO3- solution

Krzywda, Piotr; Rodríguez, Ainoa Paradelo; Benes, Nieck Edwin; Mei, Bastian; Mul, Guido

doi:10.1016/j.apcatb.2022.121512

Cited by 43 publications

(24 citation statements)

References 47 publications

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“…In the case of the reaction system for urea electrosynthesis from coreduction of NO 3 − and CO 2 , Mul et al demonstrated the formation of Cu−C≡N-like species on the Cu electrode surface during simultaneous reduction of NO 3 − and CO 2 by Raman Spectroscopy. 19 Similarly, Yu's group reported the formation of a C−N bond on V O -InOOH cayalysts during simultaneous reduction of NO 3 − and CO 2 was confirmed by SR-FTIR. 18 Specifically, Figure 5a shows the SR-FTIR signals in the range of 800 to 1800 cm −1 were collected between the potential window from −0.3 to −1.0 V vs RHE on the V O -InOOH catalyst.…”

Section: Urea Synthesis From Electrocatalytic C−n Coupling Nomentioning

confidence: 84%

“…In the case of the reaction system for urea electrosynthesis from coreduction of NO 3 – and CO 2 , Mul et al demonstrated the formation of Cu–C≡N-like species on the Cu electrode surface during simultaneous reduction of NO 3 – and CO 2 by Raman Spectroscopy . Similarly, Yu’s group reported the formation of a C–N bond on V O -InOOH cayalysts during simultaneous reduction of NO 3 – and CO 2 was confirmed by SR-FTIR .…”

Section: Discussionmentioning

confidence: 96%

“…It is key to understand the C–N coupling reaction mechanism during the electrochemical coreduction reaction of CO 2 and NO 3 – , NO 2 – , N 2 , or NO for designing highly efficient electrocatalytic urea synthesis catalysts. To date, the C–N coupling reaction mechanism during the electrochemical coreduction reaction of CO 2 and nitrogenous species was investigated by DFT calculations , and extensive in situ spectroscopy characterization methods including the Raman spectroscopy, synchrotron radiation-Fourier transform infrared spectroscopy (SR-FTIR), , online differential electrochemical mass spectrometry (DEMS), and sum frequency generation spectroscopy (SFG), respectively.…”

Section: Discussionmentioning

confidence: 99%

“…This work provides more avenues for seeking appropriate nitrogen sources for electrocatalytic urea synthesis. calculations 21,28 and extensive in situ spectroscopy characterization methods including the Raman spectroscopy, 19 synchrotron radiation-Fourier transform infrared spectroscopy (SR-FTIR), 17,18 online differential electrochemical mass spectrometry (DEMS), 10 and sum frequency generation spectroscopy (SFG), 21 respectively. Electrochemical Coreduction of CO 2 and NO 3 − .…”

Section: Urea Synthesis From Electrocatalytic C−n Coupling Nomentioning

confidence: 99%

“…Subsequently, Furuya’s group also used different metal phthalocyanine (M-Pc) catalysts for the electrochemical coreduction of CO 2 and NO 3 – /NO 2 – , with a maximum Faradaic efficiency (FE) of 40% achieved for urea synthesis on a Ni-Pc catalyst . In recent years, an increasing number of studies have been conducted to enhance the catalytic performance for the electrochemical coreduction of CO 2 and NO 3 – /NO 2 – for urea synthesis using a Pd-, Zn-, In-, , Cu-, Ti-, or Ce-based catalyst in a H-type cell with two compartments separated by a proton exchange membrane. In addition to using NO 3 – /NO 2 – as the nitrogen source, some researchers have proposed N 2 as a nitrogen source, specifically the electrochemical coreduction of CO 2 and N 2 for urea synthesis. ,,− This concept of electrochemical coreduction of CO 2 and N 2 for urea synthesis was verified by Köleli and colleagues in 2016 .…”

Section: Introductionmentioning

confidence: 99%

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Review on Electrocatalytic Coreduction of Carbon Dioxide and Nitrogenous Species for Urea Synthesis

et al. 2023

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The electrochemical coreduction of carbon dioxide (CO 2 ) and nitrogenous species (such as NO 3 − , NO 2 − , N 2 , and NO) for urea synthesis under ambient conditions provides a promising solution to realize carbon/nitrogen neutrality and mitigate environmental pollution. Although an increasing number of studies have made some breakthroughs in electrochemical urea synthesis, the unsatisfactory Faradaic efficiency, low urea yield rate, and ambiguous C−N coupling reaction mechanisms remain the major obstacles to its large-scale applications. In this review, we present the recent progress on electrochemical urea synthesis based on CO 2 and nitrogenous species in aqueous solutions under ambient conditions, providing useful guidance and discussion on the rational design of metal nanocatalyst, the understanding of the C−N coupling reaction mechanism, and existing challenges and prospects for electrochemical urea synthesis. We hope that this review can stimulate more insights and inspiration toward the development of electrocatalytic urea synthesis technology.

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Section: Urea Synthesis From Electrocatalytic C−n Coupling Nomentioning

confidence: 84%

Section: Discussionmentioning

confidence: 96%

Section: Discussionmentioning

confidence: 99%

Section: Urea Synthesis From Electrocatalytic C−n Coupling Nomentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Review on Electrocatalytic Coreduction of Carbon Dioxide and Nitrogenous Species for Urea Synthesis

et al. 2023

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Urea Electrosynthesis Accelerated by Theoretical Simulations

Liu,

Guo,

Frauenheim

et al. 2023

Adv Funct Materials

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Urea is not only a primary fertilizer in modern agriculture but also a crucial raw material for the chemical industry. In the past hundred years, the prevailing industrial synthesis of urea heavily relies on the Bosch–Meiser process to couple NH3 and CO2 under harsh conditions, resulting in high carbon emissions and energy consumption. The conversion of carbon‐ and nitrogen‐containing species into urea through electrochemical reactions under ambient conditions represents a sustainable strategy. Despite the increasing reports on urea electrosynthesis, a comprehensive review that delves into a profound, atomic‐level comprehension of the fundamental reaction mechanisms is currently absent. In this Perspective, recent advancements in electrochemical urea synthesis from CO2/CO and various nitrogenous species (i.e., N2, NOx−, and NO) under ambient conditions are presented, with special emphasis on theoretical understanding of the C─N coupling reaction mechanisms. Several key strategies to facilitate the C─N coupling are then pinpointed, which not only enhance their applicability in practical experiments but also highlight the significant progress achieved in this field. At the end, the major obstacles and potential opportunities in advancing urea electrosynthesis accelerated by theoretical simulations and in situ techniques are discussed. This review is hoped to act as a roadmap to ignite fresh insights and inspiration for the development of electrocatalytic urea synthesis.

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Fundamentals and Rational Design of Heterogeneous C‐N Coupling Electrocatalysts for Urea Synthesis at Ambient Conditions

Wan,

Zheng,

Yan

et al. 2024

Advanced Energy Materials

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Electrocatalytic C‐N coupling reaction is regarded as a promising strategy for achieving clean and sustainable urea production by coreducing CO2 and nitrogen species, thus contributing to carbon neutrality and the artificial nitrogen cycle. However, restricted by the sluggish adsorption of reactants, competitive side reactions, and multistep reaction pathways, the electrochemical urea production suffers from a low urea yield rate and low selectivity so far. In order to comprehensively improve urea synthesis performance, it is crucial to develop highly efficient catalysts for electrochemical C‐N coupling. In this article, the catalyst‐designing strategies, C‐N coupling mechanisms, and fundamental research methods are reviewed. For the coreduction of CO2 and different nitrogen species, several prevailing reaction mechanisms are discussed. With the aim of establishing the standard research system, the fundamentals of electrocatalytic urea synthesis research are introduced. The most important catalyst‐designing strategies for boosting the electrocatalytic urea production are discussed, including heteroatom doping, vacancy engineering, crystal facet regulation, atom‐scale modulation, alloying and heterostructure construction. Finally, the challenges and perspectives are proposed for future industrial applications of electrochemical urea production by C‐N coupling.

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Carbon-nitrogen bond formation on Cu electrodes during CO2 reduction in NO3- solution

Cited by 43 publications

References 47 publications

Review on Electrocatalytic Coreduction of Carbon Dioxide and Nitrogenous Species for Urea Synthesis

Review on Electrocatalytic Coreduction of Carbon Dioxide and Nitrogenous Species for Urea Synthesis

Urea Electrosynthesis Accelerated by Theoretical Simulations

Fundamentals and Rational Design of Heterogeneous C‐N Coupling Electrocatalysts for Urea Synthesis at Ambient Conditions

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