Enhanced Local CO Coverage on Cu Quantum Dots for Boosting Electrocatalytic CO₂ Reduction to Ethylene

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Окт. 29, 2024

Abstract Ethylene (C 2 H 4 ) electrosynthesis from the electrocatalytic CO reduction process holds enormous potential applications in industrial production. However, sluggish kinetics of C─C coupling often result low yield and poor selectivity for C Herein, performance Cu catalysts varying sizes is investigated, prepared via a cryo‐mediated liquid phase exfoliation technique, electrochemical to . The activity gradually increase as size decreases tens nanometers few nanometers. Impressively, 5 nm quantum dots (Cu‐5) achieve maximum Faradaic efficiency (FE) 81.5% half‐cell cathodic energy (CEE) 42.2% with large partial current density 1.1 A cm −2 at −0.93 V versus reversible hydrogen electrode. Structural characterization situ spectroscopic analysis reveal that Cu‐5 dots, dominated by (100) facet, provide an abundance active sites enhance adsorption activation, promoting formation *CO intermediates. accumulation intermediates on facilitates CO‐CHO reaction, thus enhancing production rate.

Язык: Английский

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Promoting CO2 Electroreduction to Hydrocarbon Products via Sulfur‐Enhanced Proton Feeding in Atomically Precise Thiolate‐Protected Cu Clusters

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(48)

Опубликована: Авг. 22, 2024

Abstract Thiolate‐protected Cu clusters with well‐defined structures and stable low‐coordinated + species exhibit remarkable potential for the CO 2 RR are ideal model catalysts establishing structure‐electrocatalytic property relationships at atomic level. However, extant employed in predominantly yield 2e − products. Herein, two 4 (MMI) 8 ( t BuS) (MMI=2‐mercapto‐1‐methylimidazole) prepared to investigate synergistic effect of adjacent S sites on RR. can reduce deep‐reduced products a 91.0 % Faradaic efficiency (including 53.7 CH ) while maintaining stability. Conversely, shows preference C 2+ products, achieving maximum FE 58.5 current density 152.1 mA⋅cm −2 . In situ XAS ex XPS spectra reveal preservation during RR, extensively enhancing adsorption capacity *CO intermediate. Moreover, kinetic analysis theoretical calculations confirm that facilitate H O dissociation into *H species, which directly participate protonation process *CHO. This study highlights important role Cu−S dual provides mechanistic insights pathway

Язык: Английский

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Electrified Carbon Cycling for Neutralizing the Steelmaking Industry

Carbon Energy, Год журнала: 2025, Номер unknown

Опубликована: Март 24, 2025

ABSTRACT The conventional steelmaking process emits 1.8 tons of CO 2 to produce 1 ton crude steel, making the steel industry world's largest emitting manufacturing sector. Here, we propose and demonstrate a renewable route based on electrified carbon cycling, which significantly reduces emission by 83%. critical step involves electrochemical reduction (CO RR) CO‐rich syngas, iron ore into metallic (Fe x O y ‐to‐Fe), effectively closing cycling. A technoeconomic analysis (TEA) reveals that energy efficiency this novel is dependent operating parameters RR, with optimal occurring at current density range 150‐200 mA cm −2 . As proof‐of‐concept study, sulfur vacancy (V S )‐engineered Ag 3 CuS was developed as high‐performance RR electrocatalyst. This catalyst yields syngas high Faradaic ( FE ) close 100% cell voltage 2.5 V. RR‐produced reduced oxide iron. implementation cycling increases utilization electricity in production, reaching 88.7%. research describes sustainable way reshape ironmaking ultimately neutralize industry.

Язык: Английский

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From CO₂ to Sustainable Aviation Fuel: Navigating the Technology Landscape

ACS Sustainable Chemistry & Engineering, Год журнала: 2024, Номер 12(32), С. 12143 - 12160

Опубликована: Июль 22, 2024

Sustainable jet fuel plays a crucial role in reducing aviation's carbon footprint, offering promising approach toward net-zero emissions the aviation sector. This work investigates pathways for producing fuels directly from CO2. Given early stage of many direct CO2 utilization technologies, identifying is essential. Our investigation focuses on three most important routes production, each which employs distinct intermediate compound. These are reverse water–gas shift and Fischer–Tropsch (RWGS-FT) route, methanol electrolysis employ syngas, methanol, ethylene as key intermediates, respectively. By performing comprehensive process simulations analyzing resulting energy intensity thermal efficiency these findings provide quantitative early-stage evaluations allow us to identify technical development requirements. results indicate that route exhibits lowest intensity, followed by RWGS-FT routes. H2 production accounts significant share demand The shows efficiency, while achieves 92% including recycle streams, highlighting its potential production. Furthermore, holds achieve close 100% requires significantly less feedstock. However, it faces challenges high demand. In addition, our study effects technology optimization, providing guideline research optimization.

Язык: Английский

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Enhanced CO₂ Adsorption and Conversion in Diethanolamine‐Cu Interfaces Achieving Stable Neutral Ethylene Electrosynthesis

Advanced Energy Materials, Год журнала: 2024, Номер 14(43)

Опубликована: Авг. 7, 2024

Abstract Molecular modifications have shown tremendous potential in boosting the electrochemical CO 2 reduction (CO RR) to ethylene. However, key mechanisms of modulation at molecular level remain unclear, especially for adsorption and activation intermediates (e.g., * CO). Here, report that a diethanolamine (DEA)‐modified Cu catalyst can reduce ethylene with faradaic efficiency ≈50.5% partial current density ≈155.7 mA cm −2 neutral conditions, which surpasses without modification (≈28.5% ≈95.6 ). Density functional theory calculations demonstrate DEA on surface boosts following C–C coupling processes during RR‐to‐ethylene process. dynamics simulations suggest molecules distant from site enrichment effect. Operational stability achieved via introduction onto ketjen black, then successively immobilized nanoparticles polytetrafluoroethylene electrodes obtain stable tripe‐phase boundary, realizing constant selectivity 100 operating hours flow cell.

Язык: Английский

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Atomic Ordering-Induced Ensemble Variation in Alloys Governs Electrocatalyst On/Off States

Journal of the American Chemical Society, Год журнала: 2024, Номер unknown

Опубликована: Дек. 23, 2024

The catalytic behavior of a material is influenced by ensembles─the geometric configuration atoms on the surface. In conventional systems, ensemble effects and electronic structure are coupled because these strategies focus varying composition, making it difficult to understand role ensembles in isolation. This study introduces methodology that separates from structure. To tune Pd size catalyst surface, we compared reactivity structurally different but compositionally identical Pd3Bi intermetallic solid solution alloys. intermetallics display no for methanol oxidation (MOR), while their counterparts show significant (0.5 mA cmPd–2). Intermetallics form smaller (1, 3, 4, 5 across all low-energy facets), whereas has several facets support larger ensembles, with an average 5.25 up 6 atoms. A partially ordered (a mixed phase solution) alloy shows intermediate MOR activity (0.1 cmPd–2), confirming tracks size. All alloys maintained similar structures, as confirmed X-ray photoelectron spectroscopy (XPS) valence band absorption near edge (XANES) measurements, indicating differences arise variations induced atomic ordering. Our findings offer approach designing materials controllable active site configurations maintaining catalyst's structure, thereby enabling more efficient design.

Язык: Английский

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Comprehensive Insight Into Electronic Modulation of Rare‐Earth Elements for Enhancing Electrocatalytic Performance of Atomically Dispersed Materials

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 2, 2025

Abstract Atomically dispersed materials have been a thriving research field due to their maximum atomic utilization and remarkable performance in energy conversion storage systems. Owing the large radius, strong oxophilicity, unique electronic properties, rare‐earth (RE) elements widely investigated as oxide carriers promoters atomically manipulate regulate structure of active species. Single‐atom state with an adjustable coordination environment on N‐doped carbon endows RE metals special states outstanding catalytic performances. A thorough comprehension modulation mechanism paves way for construction advanced RE‐based electrocatalysts high activity, stability, selectivity. This review provides widespread insight into roles modulating properties combined structure–performance relationship electrocatalysis processes. The characteristic physical chemical are highlighted, synthetic strategy is discussed. Finally, summary perspectives rational design development highly efficient catalysts proposed. aims provide guideline promoting effective functional materials.

Язык: Английский

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Electrosynthesis of 1,4-diene derivatives bearing cyclopentene skeleton

iScience, Год журнала: 2025, Номер 28(3), С. 111976 - 111976

Опубликована: Фев. 10, 2025

1,n-Dual Π systems including 1,4-diene derivatives have been widely used as the elegant radical receptors to promote cascade additions give highly functionalized polycyclic scaffolds. However, tedious and complicated preparation of former deters broad utilization compromises practical value. Herein, a straightforward was developed from easily accessible alkynes γ,δ-unsaturated carboxylic acids via electrochemical oxidation cyclization Hofmann elimination. This transformation features with good excellent yields, functional group compatibility, selectivity without any Zaitsev elimination product detected.

Язык: Английский

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Cooperative effects associated with high electrolyte concentrations in driving the conversion of CO2 to C2H4 on copper

Chem Catalysis, Год журнала: 2025, Номер unknown, С. 101338 - 101338

Опубликована: Апрель 1, 2025

Язык: Английский

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Reaction-Driven Varieties of Active Sites on Cu(100) in Electrochemical CO₂ Reduction Reaction

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 6497 - 6506

Опубликована: Апрель 6, 2025

Язык: Английский

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