Oxygen vacancies enhanced cooperative electrocatalytic reduction of carbon dioxide and nitrite ions to urea

Cao, Na; Quan, Yueli; Guan, Anxiang; Yang, Chao; Ji, Yali; Zhang, Lijuan; Zheng, Gengfeng

doi:10.1016/j.jcis.2020.05.014

Cited by 180 publications

(160 citation statements)

References 32 publications

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“…6b and 6c). It is comparable to the recently reported performance of ZnO-V porous nanosheets 24 , lies between those of Te-Doped Pd Nanocrystal 23 and oxygen vacancy-rich anatase TiO 2 25 . As the potential further decreases, the FE of urea decreases due to enhanced side reactions.…”

Section: Electrochemical Performances Of the Urea Production By Coupling Co 2 Rr With No 2 − Rrsupporting

confidence: 87%

“…The generated urea was decomposed into NH 3 by urease. 23,25 The absorption intensity of NH 3 converted from urea was measured by UV-Vis spectrophotometry, and the concentration was further determined from the calibration curve (Fig. S14).…”

Section: Electrochemical Performances Of the Urea Production By Coupling Co 2 Rr With No 2 − Rrmentioning

confidence: 99%

“…24 However, this strategy has parallel CO 2 RR and the NO 2 − RR, which will generate complex product distribution, thus reducing the FE of the urea and increasing the di culty of separating urea from the product. 25,26 Therefore, the design and construction of electrocatalysts with high catalytic activity and selectivity are essential for the electrochemical synthesis of urea.…”

Section: Introductionmentioning

confidence: 99%

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AuCu nanofibers for electrosynthesis of urea from carbon dioxide and nitrite

Liu

Yin

Wang

et al. 2021

Preprint

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Carbon dioxide reduction reaction (CO2RR) is a promising technology for mitigating greenhouse gas emission and achieving carbon neutrality. However, coupling CO2RR with other reactions to produce high value-added chemicals remains a challenge. In this work, we report self-assembled nanofibers composed of ultra-thin AuCu alloy nanowires possessing a Boerdijk-Coxeter structure with (111)-dominant facets for the electrosynthesis of urea by coupling CO2RR with nitrite reduction reaction (NO2−RR). The rich structural defects and AuCu bimetallic alloy composition provide a large number of highly catalytically active sites. The constructed AuCu nanofibers display excellent urea synthesis performance in the electrolyte solution containing 0.01 M KNO2 with continuous drumming of CO2, achieving a high urea yield rate of up to 3889.6 µg h− 1 mg− 1cat. and a high Faraday efficiency of 24.7% at -0.9 V. This work provides a feasible method for the rational design of self-assembled bimetallic nanofibers for electrosynthesis of urea under ambient conditions.

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Section: Electrochemical Performances Of the Urea Production By Coupling Co 2 Rr With No 2 − Rrsupporting

confidence: 87%

Section: Electrochemical Performances Of the Urea Production By Coupling Co 2 Rr With No 2 − Rrmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

AuCu nanofibers for electrosynthesis of urea from carbon dioxide and nitrite

Liu

Yin

Wang

et al. 2021

Preprint

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“…Thea nticipated simultaneous activation of multiple reactants and intermediates can also be achieved by optimizing the strongly coupled metal-support interface.D istinct active sites on the support and metals catalyze two separate reaction pathways,a nd their spatial proximity facilitates subsequent coupling of different intermediates (Figure 8c). In addition, the strong metal-support interaction will induce electronic modification on the supported metals,i mpact adsorption behaviors,a nd eventually influence the catalytic activity and selectivity.I nt he case of C-N coupling to produce urea, the oxygen-vacancy-rich TiO 2 support was demonstrated to serve as aparallel catalyst itself for nitrite reduction [85] and also to optimize the electronic structure of supported PdCu nanoparticles to boost catalytic activity. [84] Them etal-support interface and catalytic performance is highly influenced by the size and configuration of supported metals.…”

Section: Multiple Functional Sitesmentioning

confidence: 99%

Electrocatalytic Refinery for Sustainable Production of Fuels and Chemicals

et al. 2021

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Compared to modern fossil‐fuel‐based refineries, the emerging electrocatalytic refinery (e‐refinery) is a more sustainable and environmentally benign strategy to convert renewable feedstocks and energy sources into transportable fuels and value‐added chemicals. A crucial step in conducting e‐refinery processes is the development of appropriate reactions and optimal electrocatalysts for efficient cleavage and formation of chemical bonds. However, compared to well‐studied primary reactions (e.g., O2 reduction, water splitting), the mechanistic aspects and materials design for emerging complex reactions are yet to be settled. To address this challenge, herein, we first present fundamentals of heterogeneous electrocatalysis and some primary reactions, and then implement these to establish the framework of e‐refinery by coupling in situ generated intermediates (integrated reactions) or products (tandem reactions). We also present a set of materials design principles and strategies to efficiently manipulate the reaction intermediates and pathways.

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“…Currently, the synthesis of these molecules is all dominated by the thermocatalytic transformation of NH 3 precursors under harsh conditions, which consumes more than half of the global ammonia production [84] . In contrast, electrocatalytic C–N coupling reactions are highly advantageous because they can directly convert abundant feedstocks (e.g., N 2 , CH 4 ) and even wastes (e.g., CO 2 , NO 3 − ) into targeted complex molecules under ambient conditions [84, 85] . Herein, two main promising approaches involving different key intermediates are introduced to form different chemical bonds and products (Figure 4), including (*CO + *NH y ) coupling for amides and (*CH x + *NH y ) coupling for amines or nitriles.…”

Section: Integrated Electrocatalytic Reactionsmentioning

confidence: 99%