Boosting Electrochemical Urea Synthesis via Cooperative Electroreduction Through the Parallel Reduction

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 16, 2025

Abstract Despite recent achievements in the co‐reduction electrosynthesis of urea from nitrogen wastes and CO 2 , selectivity yield products remain fairly average because competition NITRR, RR, HER. Here, a strategy involving FeNC catalysts disperse with oxygen‐vacancy‐rich CeO (FeNC‐Ce) is illustrated, which reversible hydrogenation defects, bimetallic catalytic centers enable spontaneous switching between reduction paths NO 3 − . The FeNC‐Ce electrocatalyst exhibits an extremely high Faraday efficiency (FE) 20969.2 µg mg −1 h 89.3%, respectively, highly superior to most reported values (maximum 200–2300 FE max 11.5%–83.4%). study findings, rationalize by situ spectroscopy theoretical calculations, are rooted evolution dynamic NITRR RR protons, alleviating overwhelming single‐system reactants thereby minimizing formation by‐products.

Language: Английский

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Ultrasonically Deposited Boron‐Doped Silicon Decorated with Laser‐Generated Iridium Nanoparticles as Manufacturing Approach for OER Electrodes in PEM Water Electrolysis

Advanced Materials Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 13, 2025

Abstract The study introduces flexible and scalable manufacturing approach for electrodes utilizing boron‐doped silicon as conductive support iridium nanoparticles, addressing the challenges of cost scarcity associated wit noble catalysts oxygen evolution reaction (OER). Colloidal Ir nanoparticles are synthesized via pulsed‐laser ablation (≈4–7 nm) decorated on B‐doped Si (≈100 through electrostatic adsorption. Titanium substrates ultrasonically sprayed with Si:B – very low loading 12 wt.%. Crystalline phases (Ir(111), Ir(200)) observed known to enhance OER mechanism. Additionally, atom probe tomography confirms that particles contained 0.03‐0.5 at% boron throughout entire particle, while electrical permittivity through‐plane measurements reveal a positive impact conductivity nanocatalysts ultralow‐loaded catalyst coated Ti (0.12 mg cm −2 ), respectively. Rotating disk electrode results show pronounced oxidation peaks nanoparticles. Si:B‐Ir 4 nm exhibits highest turonover frequency (2.62 s⁻¹) competitive electrochemical surface area (25 m 2 g −1 ) compared 7 (0.96 s⁻¹; 37.5 black (0.24 5 ). overall analysis parameters highlights performant catalytic efficiency, balancing activity kinetics effectively.

Language: Английский

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Positive shift of the d-Band center in Cu nanoparticles facilitates electrocatalytic hydrogenation of furfural under mild pH conditions

Journal of Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 116003 - 116003

Published: Feb. 1, 2025

Language: Английский

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CuPt Alloy Enabling the Tandem Catalysis for Reduction of HCOOH and NO₃⁻ to Urea at High Current Density

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 21, 2025

The formation of urea by electrocatalytic reduction C1-reactants and NO3 - is an attractive way to store renewable electricity, close the carbon cycle, eliminate nitrate contaminants from wastewater. Involving insufficient supply C1 reactants multiple electron transfers makes reaction difficult achieve high Faraday efficiency yield at current density. Here, a synthesis approach presented via reductive coupling between liquid HCOOH on copper foam (CF) loaded Cu4Pt catalyst with optimized ratios. A 40.08 mg h-1 cm-2 achieved FE up 58.1% density -502.3 mA cm-2, superior productivity previously reported catalysts. No degradation observed over 120-h continuous operation such rate. highly efficient activity Cu4Pt/CF can be attributed synergetic effect Pt Cu sites tandem catalysis, in which doped enrich reactants, promote intermolecular dehydration, form adsorb large amounts *CO key intermediates. generate quantities intermediate *NH2. adsorbed intermediates *NH2 are basis for subsequent thermodynamic spontaneous C─N coupling.

Language: Английский

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Tailoring Activation Intermediates of CO₂ Initiates C–N Coupling for Highly Selective Urea Electrosynthesis

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

Electrocatalyzed reduction of CO2 and NO3- to synthesize urea is a highly desirable, but challenging reaction. The bottleneck this reaction the C-N coupling intermediates. In particular, uncertainty multielectron intermediates severely affects selectivity activity processes involving multiple electron proton transfers. Here, we present novel tandem catalyst with two compatible single-atom active sites Au Cu on red phosphorus (RP-AuCu) that efficiently converts urea. Experimental theoretical prediction results confirmed center promotes transfer between molecules phosphorus, thereby regulating activation produce electrophilic *COOH. addition, can enhance attack *COOH species *NH2, thus promoting selective formation bonds. Consequently, RP-AuCu exhibited yield 22.9 mmol gcat.-1 h-1 Faraday efficiency 88.5% (-0.6 VRHE), representing one highest levels electrocatalytic synthesis. This work deepens understanding mechanism provides an interesting design approach for efficient sustainable production compounds.

Language: Английский

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Rapid synthesis of metastable materials for electrocatalysis

Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Metastable materials are considered promising electrocatalysts for clean energy conversions by virtue of their structural flexibility and tunable electronic properties. However, the exploration synthesis metastable via traditional equilibrium methods face challenges because requirements high precise control. In this regard, rapid method (RSM), with efficiency ultra-fast heating/cooling rates, enables production under non-equilibrium conditions. relationship between RSM properties remains largely unexplored. review, we systematically examine unique benefits various techniques mechanisms governing formation materials. Based on these insights, establish a framework, linking electrocatalytic performance Finally, outline future directions emerging field highlight importance high-throughput approaches autonomous screening optimal electrocatalysts. This review aims to provide an in-depth understanding electrocatalysts, opening up new avenues both fundamental research practical applications in electrocatalysis.

Language: Английский

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Multiple Functional Engineering Strategies and Active Site Identification in Ru‐Based Electrocatalysts for Catalytic Conversion Reactions

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 3, 2025

Electrochemical conversion has been regarded as an ideal technology for achieving clean and sustainable energy, showing significant promise in addressing the increasingly serious energy crisis environmental pollution. Ru-containing electrocatalysts (RUCE) outperform other precious metals due to elevated intrinsic activity superior cost-effectiveness, developing into a promising candidate electrochemical reactions. A challenge field of catalyst discovery lies its heavy reliance on empirical methods, rather than approaches that are rooted rational design principles. This review first concentrates catalytically active sites critical factors governing catalytic performance durability. Then, comprehensive summary multifunctional modification strategies ranging from nanoscale atomic scale is explored control structure improve performance. By unveiling roles each component modified RUCE at level, their identified discussed establish structure-performance relationship catalysts. Finally, challenges perspectives Ru-based materials hydrogen, oxygen, nitrogen reactions presented inspire further efforts toward understanding meet ever-growing demand future.

Language: Английский

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Catalyst and gas diffusion electrode design toward C–N coupling for urea electrosynthesis

eScience, Journal Year: 2025, Volume and Issue: unknown, P. 100425 - 100425

Published: April 1, 2025

Language: Английский

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Spin Manipulation of Co sites in Co₉S₈/Nb₂CT_x Mott–Schottky Heterojunction for Boosting the Electrocatalytic Nitrogen Reduction Reaction

Advanced Science, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 3, 2024

Abstract Regulating the adsorption of an intermediate on electrocatalyst by manipulating electron spin state transition metal is great significance for promoting activation inert nitrogen molecules (N 2 ) during electrocatalytic reduction reaction (eNRR). However, achieving this remains challenging. Herein, a novel 2D/2D Mott–Schottky heterojunction, Co 9 S 8 /Nb CT x ‐P, developed as eNRR catalyst. This achieved through in situ growth cobalt sulfide (Co nanosheets over Nb MXene using solution plasma modification method. Transformation from low (t 2g 6 e g 1 to high 5 adjusting interface electronic structure and sulfur vacancy ‐P. The ability N optimized Co(II) with more unpaired electrons, significantly accelerating *N →*NNH kinetic process. ‐P exhibits NH 3 yield 62.62 µg h −1 mg cat. Faradaic efficiency (FE) 30.33% at −0.40 V versus reversible hydrogen electrode (RHE) 0.1 m HCl. Additionally, it achieves 41.47 FE 23.19% −0.60 RHE Na SO 4 . work demonstrates promising strategy constructing heterojunction electrocatalysts efficient eNRR.

Language: Английский

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Recent Advances in Urea Electrocatalysis: Applications, Materials and Mechanisms^†

Chinese Journal of Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 26, 2024

Comprehensive Summary Urea plays a vital role in human society, which has various applications organic synthesis, medicine, materials chemistry, and other fields. Conventional industrial urea production process is energy−intensive environmentally damaging. Recently, electrosynthesis offers greener alternative to efficient synthesis involving coupling CO 2 nitrogen sources at ambient conditions, affords an achievable way for diminishing the energy consumption emissions. Additionally, electrolysis, namely electrocatalytic oxidation reaction (UOR), another emerging approach very recently. When with hydrogen evolution reaction, UOR route potentially utilizes 93% less than water electrolysis. Although there have been many individual reviews discussing electrooxidation, critical need comprehensive review on electrocatalysis. The will serve as valuable reference design of advanced electrocatalysts enhance electrochemical electrocatalysis performance. In review, we present thorough two aspects: reaction. We summarize turn recently reported catalyst materials, multiple catalysis mechanisms principles Finally, major challenges opportunities are also proposed inspire further development technology. Key Scientists For electrosynthesis, Furuya et al. firstly investigated coreduction NO 3 − /NO using gas‐diffusion electrodes 1995. Then, Wang effectively achieved C—N bond formation PdCu alloy nanoparticles 2020. Shortly, Yan Yu *CO from *NO intermediates early stage In(OH) electrocatalyst 2021, employed defect engineering strategy facilitate NH protonation 2022. Amal al . Investigated that Cu‐N‐C coordination both RR RR. After that, Zhang's group developed In‐based artificial frustrated Lewis pairs urea, they offered systematic screening 2023. And sargent increased selectivity hybrid catalyst. Stevenson effect Sr substitution toward provided insights into electrooxidation β‐Ni(OH) electrode Qiao elucidated two‐stage pathway 2021.

Language: Английский

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