Synergistic Cu Single Atoms and MoS2‐Edges for Tandem Electrocatalytic Reduction of NO3− and CO2 to Urea DOI

Wenyu Du,

Zeyi Sun,

Kai Chen

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(43)

Published: Aug. 16, 2024

Abstract Urea electrosynthesis from co‐electrolysis of NO 3 − and CO 2 (UENC) under ambient conditions is recognized as an appealing approach for effective sustainable urea production, while it requires high‐efficiency UENC electrocatalysts to promote the C─N coupling hydrogenation processes. Herein, single‐atom Cu anchored on MoS (Cu 1 ‐MoS ) explored a highly active selective catalyst. Theoretical calculations operando spectroscopic characterizations unveil synergistic tandem catalysis UENC, where single atoms trigger early coupling, ‐edges key step * NH COOHNH generation. Strikingly, equipped in flow cell achieves excellent performance with maximum urea‐Faradaic efficiency 57.02% at −0.6 V corresponding yield rate 23.3 mmol h −1 g , surpassing nearly all previously reported catalysts.

Language: Английский

Review on strategies for improving the added value and expanding the scope of CO2 electroreduction products DOI
Minghang Jiang, Huaizhu Wang, Mengfei Zhu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(10), P. 5149 - 5189

Published: Jan. 1, 2024

This review summarizes promising strategies including the design of catalysts and construction coupled electrocatalytic reaction systems, aimed at achieving selective production various products from CO 2 electroreduction.

Language: Английский

Citations

75
Sequential co-reduction of nitrate and carbon dioxide enables selective urea electrosynthesis DOI Creative Commons
Yang Li,

Shisheng Zheng,

Hao Liu

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Jan. 2, 2024

Abstract Despite the recent achievements in urea electrosynthesis from co-reduction of nitrogen wastes (such as NO 3 − ) and CO 2 , product selectivity remains fairly mediocre due to competing nature two parallel reduction reactions. Here we report a catalyst design that affords high by sequentially reducing at dynamic catalytic centre, which not only alleviates competition issue but also facilitates C−N coupling. We exemplify this strategy on nitrogen-doped carbon catalyst, where spontaneous switch between paths is enabled reversible hydrogenation functional groups. A yield rate 596.1 µg mg −1 h with promising Faradaic efficiency 62% obtained. These findings, rationalized situ spectroscopic techniques theoretical calculations, are rooted proton-involved evolution mitigates overwhelming reactants thereby minimizes formation side products.

Language: Английский

Citations

70
Oxygen Vacancies‐Rich Metal Oxide for Electrocatalytic Nitrogen Cycle DOI
Xiaoxiao Wei, Chen Chen, Xian‐Zhu Fu

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 14(1)

Published: Nov. 13, 2023

Abstract The development of industry and agriculture has been accompanied by an artificially imbalanced nitrogen cycle, which threatens human health ecological environments. Electrocatalytic systems have emerged as a sustainable way converting nitrogen‐containing molecules into high value‐added chemicals. However, the construction high‐performance electrocatalysts remains challenging. oxygen vacancy engineering strategy promoted more research efforts to explore structure‐activity relationship between catalytic activity vacancies. This review systematically summarizes recent vacancies‐rich metal oxides for electro‐catalyzing cycling systems, involving electrocatalytic nitrate reduction reaction, nitric oxide C─N coupling, urea oxidation reaction. First, methods characterization vacancies are summarized. Then, effect on is discussed in terms regulating electronic structures electrocatalysts, improving electroconductivity catalysts, lowing energy barrier, strengthening adsorption activation intermediate species. Finally, future directions cycle anticipated.

Language: Английский

Citations

57
Coactivation of Multiphase Reactants for the Electrosynthesis of Urea DOI
Zheng Lv,

Shuanglong Zhou,

Liang Zhao

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(25)

Published: May 24, 2023

Abstract N 2 and CO fixation is an environmentally friendly waste‐to‐energy technology that can replace tedious demanding industrial urea productive processes. Here, V ‐Cu 3 N‐300 catalysts with tip vacancy structures are designed for the coactivation of multiphase reactants in electrosynthesis process. Under environmental conditions, yield 81 µg h −1 cm −2 , this first report high area active electrocatalyst, corresponding Faraday efficiency able to reach 28.7%. The full‐cell electrolysis exhibits good stability, providing a current density 0.7 mA at 2.1 V. electrolyte after continuous 48 subjected being evaporated recrystallized, it determined by 1 H NMR purity 100%. Comprehensive analysis shows local electric field formed effect effectively promote adsorption activation . presence surface nitrogen vacancies promotes formation *NN* intermediates, ensuring CN coupling, also optimizing dissociation process water, proton supply synthesis urea. Thus, rate‐determining step altered ensured.

Language: Английский

Citations

45
One-step Formation of Urea from Carbon Dioxide and Nitrogen Using Water Microdroplets DOI
Xiaowei Song, Chanbasha Basheer, Yu Xia

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(47), P. 25910 - 25916

Published: Nov. 15, 2023

Water (H2O) microdroplets are sprayed onto a graphite mesh covered with CuBi2O4 coating using 1:1 mixture of N2 and CO2 as the nebulizing gas. The resulting contain urea [CO(NH2)2] detected by both mass spectrometry 13C nuclear magnetic resonance. This gas-liquid-solid heterogeneous catalytic system synthesizes in one step on 0.1 ms time scale. conversion rate reaches 2.7 mmol g-1 h-1 at 25 °C 12.3 65 °C, no external voltage applied. serve hydrogen source electron transfer medium for contact CuBi2O4. Water-gas water-solid electrification speculated to drive reaction process. strategy couples fixation utilization an ecofriendly process produce urea, converting greenhouse gas into value-added product.

Language: Английский

Citations

44
Electrocatalytic Systems for NOx Valorization in Organonitrogen Synthesis DOI Open Access
Peisen Liao, Jiawei Kang,

Runan Xiang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(3)

Published: Oct. 13, 2023

Inorganic nitrogen oxide (NO

Language: Английский

Citations

42
Electrocatalytic synthesis of C–N coupling compounds from CO2 and nitrogenous species DOI Creative Commons
Zheng Zhang, Danyang Li, Yunchuan Tu

et al.

SusMat, Journal Year: 2024, Volume and Issue: 4(2)

Published: March 12, 2024

Abstract The electrocatalytic synthesis of C–N coupling compounds from CO 2 and nitrogenous species not only offers an effective avenue to achieve carbon neutrality reduce environmental pollution, but also establishes a route synthesize valuable chemicals, such as urea, amide, amine. This innovative approach expands the application range product categories beyond simple carbonaceous in reduction, which is becoming rapidly advancing field. review summarizes research progress urea synthesis, using N , NO − 3 species, explores emerging trends electrosynthesis amide amine nitrogen species. Additionally, future opportunities this field are highlighted, including amino acids other containing bonds, anodic reactions water oxidation, catalytic mechanism corresponding reactions. critical captures insights aimed at accelerating development electrochemical reactions, confirming superiority method over traditional techniques.

Language: Английский

Citations

42
Dynamic Reconstruction of Two‐Dimensional Defective Bi Nanosheets for Efficient Electrocatalytic Urea Synthesis DOI
Yan Wang,

Shuai Xia,

Rui Cai

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(16)

Published: Feb. 22, 2024

Abstract Abstract:Catalyst surface dynamics drive the generation of active species for electrocatalytic reactions. Yet, understanding dominant site formation and reaction mechanisms is limited. In this study, we thoroughly investigate dynamic reconstruction two‐dimensional defective Bi nanosheets from exfoliated 2 Se 3 under electrochemical CO nitrate (NO − ) reduction conditions. The ultrathin obtained by NaBH 4 ‐assisted cryo‐mediated liquid‐phase exfoliation are more easily reduced reconstructed to with high‐density grain boundaries (GBs; GB‐rich Bi). catalyst affords a remarkable yield rate 4.6 mmol h −1 mg cat. Faradaic efficiency 32 % urea production at −0.40 V vs. RHE. Notably, 8.2 times higher than those low‐GB bulk catalysts, respectively. Theoretical analysis demonstrates that GB sites significantly reduce *CO *NH intermediate energy C−N coupling barrier, enabling selective electrosynthesis on catalyst. This work will trigger further research into structure‐activity interplay in processes using situ techniques.

Language: Английский

Citations

38
Fundamentals and Rational Design of Heterogeneous C‐N Coupling Electrocatalysts for Urea Synthesis at Ambient Conditions DOI
Yuchi Wan,

Muyun Zheng,

Yan Wei

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(28)

Published: Jan. 28, 2024

Abstract Electrocatalytic C‐N coupling reaction is regarded as a promising strategy for achieving clean and sustainable urea production by coreducing CO 2 nitrogen species, thus contributing to carbon neutrality the artificial cycle. However, restricted sluggish adsorption of reactants, competitive side reactions, multistep pathways, electrochemical suffers from low yield rate selectivity so far. In order comprehensively improve synthesis performance, it crucial develop highly efficient catalysts coupling. this article, catalyst‐designing strategies, mechanisms, fundamental research methods are reviewed. For coreduction different several prevailing mechanisms discussed. With aim establishing standard system, fundamentals electrocatalytic introduced. The most important strategies boosting discussed, including heteroatom doping, vacancy engineering, crystal facet regulation, atom‐scale modulation, alloying heterostructure construction. Finally, challenges perspectives proposed future industrial applications

Language: Английский

Citations

32
Selective Electrocatalytic Conversion of Nitric Oxide to High Value‐Added Chemicals DOI Creative Commons
Dongdong Wang, Xue Feng Lu, Deyan Luan

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(18)

Published: Jan. 25, 2024

The artificial disturbance in the nitrogen cycle has necessitated an urgent need for nitric oxide (NO) removal. Electrochemical technologies NO conversion have gained increasing attention recent years. This comprehensive review presents advancements selective electrocatalytic of to high value-added chemicals, with specific emphasis on catalyst design, electrolyte composition, mass diffusion, and adsorption energies key intermediate species. Furthermore, explores synergistic electrochemical co-electrolysis carbon source molecules, enabling synthesis a range valuable chemicals C─N bonds. It also provides in-depth insights into intricate reaction pathways underlying mechanisms, offering perspectives challenges prospects electrolysis. By advancing comprehension fostering awareness balance, this contributes development efficient sustainable systems from NO.

Language: Английский

Citations

29