Predicting electrocatalytic urea synthesis using a two-dimensional descriptor

Communications Chemistry, Journal Year: 2025, Volume and Issue: 8(1)

Published: Feb. 3, 2025

Electrochemical synthesis routes powered by renewable electricity can provide sustainable chemical commodities replacing conventional fossil-based processes. Increasing research focuses on value-added chemicals like the indispensable fertilizer urea, which also constitutes a study case for electrochemical CN-coupling. To guide identification of highly selective catalysts, we aim to new insight analysing existing experimental data selectivity transition metal catalysts towards electrochemically synthesized urea. Firstly, project high dimensional using principal component analysis (PCA) lower dimensions, and thereby confirm that urea is correlated with CO NH3. Furthermore, identified most suitable two-dimensional descriptors prediction out various adsorption energies calculated density functional theory (DFT). We suggest *H *O slabs predict in co-reduction CO2 nitrite ( NO2- ).

Language: Английский

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Cu–Bi Bimetallic Catalysts Derived from Metal–Organic Framework Arrays on Copper Foam for Efficient Glycine Electrosynthesis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 30, 2024

Abstract Glycine as one of the most abundant amino acids in human proteins, with extensive applications both life and industry, is conventionally synthesized through complex procedures or toxic feedstocks. In this study, we present a facile benign electrochemical pathway for synthesis glycine reductive coupling glyoxylic acid nitrate over copper‐bismuth bimetal catalyst derived from metal–organic framework (MOF) array on copper foam (Cu/Bi−C@CF). Remarkably, Cu/Bi−C@CF achieves fantastic selectivity 89 %, corresponding high Faraday efficiency 65.9 %. From control experiments, introduction Bi caused binding energy Cu shift to lower state, which leads towards formation key intermediate hydroxylamine rather than ammonia product, facilitating oxime providing additional sites subsequent hydrogenation reaction way glycine. Moreover, derivation MOF arrays ensures effective dispersion enhances stability Cu/Bi−C@CF. This innovative approach not only presents sustainable pathways production value‐added organonitrogen compounds utilizing readily available carbon nitrogen sources, but also provides novel insights into design multistage structural catalysts sequential reactions.

Language: Английский

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Capturing Copper Single Atom in Proton Donor Stimulated O‐End Nitrate Reduction

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

Published: Feb. 18, 2025

Abstract Ammonia (NH 3 ) is vital in global production and energy cycles. Electrocatalytic nitrate reduction (e‐NO RR) offers a promising route for nitrogen (N) conversion NH synthesis, yet it faces challenges like competing reactions low catalyst activity. This study proposes synergistic mechanism incorporating proton donor to mediate O‐end e‐NO RR, addressing these limitations. A novel method combining ultraviolet radiation reduction, confined microwave treatment was developed create model embedding Cu single atoms on La‐based nanoparticles ( p ‐CNCu s La n ‐m). DFT analysis emphasizes the critical role of clusters as donors while situ characterization reveals an adsorption mechanism. The achieves remarkable Faraday efficiency (FE NH3 97.7%, producing 10.6 mol g metal −1 h , surpassing most prior studies. In flow cell, demonstrated exceptional stability, with only 9% decrease current density after 111 hours rate 1.57 mg /h/cm −2 . mechanism's effectiveness highlights its potential advancing electrocatalyst design. Beyond production, opens avenues exploring molecular‐oriented coupling paving way innovative electrochemical synthesis applications.

Language: Английский

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Multiple active site metal-based catalysts for C-N coupling reactions and the beyond

Next Materials, Journal Year: 2025, Volume and Issue: 8, P. 100555 - 100555

Published: Feb. 21, 2025

Language: Английский

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Progress and Perspectives in the Electrochemical Synthesis of Carbon Nanomaterials

Carbon, Journal Year: 2025, Volume and Issue: unknown, P. 120151 - 120151

Published: Feb. 1, 2025

Language: Английский

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2D Catalysts for Electrocatalytic Nitrate Reduction and C–N Coupling Reactions

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

Published: March 16, 2025

Abstract Powering the electrochemical nitrate reduction reaction (NO 3 ⁻RR) by renewable energy is a sustainable way to restore environment and produce nitrogen–hydrogen compounds. However, process requires multiple electron transfers complex paths, making it essential understand mechanisms at molecular level. In this regard, 2D materials attract significant interest due their large surface area, tunable electronic structures, suitability as model catalysts for studying structure–activity relationships. Advances in use of electrocatalytic NO ⁻RR C–N coupling reactions are analyzed elucidated influence various catalyst design strategies on mechanisms. Using advanced situ/operando measurement techniques, conducting rigorous theoretical analyses, scaling up industrial electrolyzers pivotal unlocking practical potential beyond. A map developing next‐generation electrocatalysts devices provided enable efficient nitrogen cycle using electrocatalysis.

Language: Английский

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Electrifying CO₂ Coupling With Small Molecules

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

Published: March 25, 2025

Abstract Carbon capture and utilization (CCU) is pivotal for low‐carbon industry. Among varied techniques, coupling of carbon dioxide (CO 2 ) with small molecules to generate valuable‐added chemicals using renewable electricity stands out thanks its cost‐effectiveness sustainability. This review first highlights recent strategies in catalyst preparation improving the efficiency selectivity electrochemical reactions, including heterostructure catalysts, bimetallic defect engineering, coordination complexes. The progresses on mechanism investigation C─N, C─O, C─C situ spectroscopies online mass spectrometry are subsequently summarized. In addition, electrolyzer design techno–economic analysis about process optimization integration energy stressed. Finally, future challenges optimization, reaction elucidation, scale‐up implementation discussed.

Language: Английский

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Multifunctional Strategies of Advanced Electrocatalysts for Efficient Urea Synthesis

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

Published: Oct. 20, 2024

The electrochemical reduction of nitrogenous species (such as N

Language: Английский

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Frustrated Lewis Pair Meets Polyhedral Oligomeric Silsesquioxane: Water-Tolerant Hybrid Porous Networks for Robust, Efficient, and Recyclable CO₂ Catalysis

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 25, 2025

Frustrated Lewis pair chemistry (FLP) occupy a crucial position in nonmetal-mediated catalysis, especially toward activation of inert gas molecules. Yet, one formidable issue homogeneous FLP catalysts is their instability on preservation and recycling. Here we contribute general solution that marries the polyhedral oligomeric silsesquioxane (POSS) with structurally specific frustrated acid to fabricate porous polymer networks, which can form situ water-insensitive heterogeneous upon employing base substrates. The excellent resistance water derives from synergy superhydrophobicity cage multiscale micro/nano-structural effect formed networks. Using CO2 as C1 feedstock, FLP-POSS hybrid materials allow for catalytically conversion variety diamine substrates into medicinal benzimidazole derivatives. Not only units be immobilized networks meeting needs recyclable utilization but, more importantly, are also high catalytic efficiency capable working at near ambient condition owing favorable selectivity. Given this organic/inorganic catalyst features low cost, ease synthesis, little requirements internal structural ordering, it will pave way large-scale preparation amorphous low-cost, robust, sustainable conversion.

Language: Английский

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Tuning the CO₂ and CO Electroreduction by Rate-Determining and Selectivity-Determining Steps

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 16, 2025

The renewable electricity-driven CO2 and CO reduction represents a promising approach for reducing the footprint toward carbon neutrality. Substantial research developments have been achieved in designing catalysts reaction interfaces enhanced electrocatalytic activity selectivity, investigation understanding of complex mechanisms also extensively investigated by both situ characterizations theoretical investigations. Although quasi-equilibrium rate-determining step assumptions are widely used electrochemical kinetics, overall rate is generally determined series elementary steps, influence certain can be quantified based on degree control theory. For complicated networks CO(2) reduction, not only steps but subsequent selectivity-determining play critical roles, especially product selectivity. In this Perspective, we summarize strategies that tune selectivity their impacts respectively. addition, describe coupling electroreduction with other (electro)chemical reactions, such as nitrite methane oxidation, to form value-added products. At end, current challenges opportunities field discussed inspire further development next stage.

Language: Английский

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