Multiscale Modeling of CO2 Electrochemical Reduction on Copper Electrocatalysts: A Review of Advancements, Challenges, and Future Directions

ChemSusChem, Год журнала: 2024, Номер unknown

Опубликована: Июль 18, 2024

Abstract Although CO 2 contributes significantly to global warming, it also offers potential as a raw material for the production of hydrocarbons such CH 4 , C H and 3 OH. Electrochemical reduction reaction ( e RR) is an emerging technology that utilizes renewable energy convert into valuable fuels, solving environmental problems simultaneously. Insights gained at any individual scale can only provide limited view specific scale. Multiscale modeling, which involves coupling atomistic‐level insights (density functional theory, DFT) (Molecular Dynamics, MD), with mesoscale (kinetic Monte Carlo, KMC, microkinetics, MK) macroscale (computational fluid dynamics, CFD) simulations, has received significant attention recently. While multiscale modeling eCO RR on electrocatalysts across all scales due its complexity, this review overview recent works single two three scales, “DFT+MD”, “DFT+KMC”, “DFT+MK”, “KMC/MK+CFD” “DFT+MK/KMC+CFD”, focusing particularly Cu‐based copper known be excellent electrocatalyst RR. This sets apart from other reviews solely focus exclusively or combination DFT MK/KMC scales. Furthermore, concise machine learning (ML) applications RR, approach not yet been reviewed. Finally, highlights key challenges, research gaps perspectives

Язык: Английский

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Catalysis for Carbon‐Circularity: Emerging Concepts and Role of Inorganic Chemistry

ChemSusChem, Год журнала: 2024, Номер 17(21)

Опубликована: Май 28, 2024

Carbon circularity is crucial for achieving a circular economy but has wider implications and impacts with respect to the of materials. It an in-depth transformative effect on economy. CO

Язык: Английский

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Recent Advances in Electrocatalytic Conversion of CO2-to-Ethylene: from Reaction Mechanisms to Tuning Strategies

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер unknown, С. 124822 - 124822

Опубликована: Ноя. 1, 2024

Язык: Английский

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Cooperative Effects Associated with High Electrolyte Concentrations in Driving the Conversion of CO2 to C2H4 on Copper

Опубликована: Июнь 14, 2024

Increasing the product selectivity and decreasing cost of separation is critical for large scale application electrochemical CO2 reduction (ECO2R). We hypothesize that highly concentrated aqueous electrolytes can tune microenvironment catalyst/electrolyte interface improve selectivity. Compared to a conventional electrolyte concentration 1 M HCOOK, use 7.1 HCOOK increases FE ratio C2H4/CO from 2.2 ± 0.3 18.3 4.8 at -1.08 V vs RHE on Cu gas diffusion electrode. Based analysis AIMD simulation, identity cation anion play more important roles in controlling CO2R reaction pathway than bulk solubility pH electrolytes. In-situ ATR-SEIRAS suggests that, unlike *CO-bridge binding mode dominant electrolyte, which potentially results less CO release higher yield C2H4. This study demonstrates while we tailor composition shift selectivity, factors control are numerous cannot be distilled down into one correlated property-reactivity relationship. Thus, when conditions changed, care must taken understand their effects properties electrode-electrolyte interface.

Язык: Английский

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Unconventional Electrocatalytic CO Conversion to C2 Products on Single‐Atomic Pd‐Agn Sites

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Июль 12, 2024

Abstract The electrochemical reduction of CO or 2 into C 2+ products has mostly been focused on Cu‐based catalysts. Although Ag also predicted as a possible catalyst for the CO‐to‐C conversion from thermodynamic point view, however, due to its weak binding strength, rapidly desorbs surface rather than participates in deep reduction. In this work, we demonstrate that single‐atomic Pd sites doped lattice can tune adsorption behavior and promote toward products. monodispersed Pd−Ag n enable with both Pd‐atop (Pd L ) bridge (PdAg B configurations, which increase coverage reduce C−C coupling energy barrier. Under room temperature ambient pressure, 1 10 alloy exhibited total Faradaic efficiency ~37 % at −0.83 V, appreciable current densities stability, thus featuring unconventional non‐Cu electrocatalytic capability.

Язык: Английский

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Unconventional Electrocatalytic CO Conversion to C2 Products on Single‐Atomic Pd‐Agn Sites

Angewandte Chemie, Год журнала: 2024, Номер 136(43)

Опубликована: Июль 12, 2024

Abstract The electrochemical reduction of CO or 2 into C 2+ products has mostly been focused on Cu‐based catalysts. Although Ag also predicted as a possible catalyst for the CO‐to‐C conversion from thermodynamic point view, however, due to its weak binding strength, rapidly desorbs surface rather than participates in deep reduction. In this work, we demonstrate that single‐atomic Pd sites doped lattice can tune adsorption behavior and promote toward products. monodispersed Pd−Ag n enable with both Pd‐atop (Pd L ) bridge (PdAg B configurations, which increase coverage reduce C−C coupling energy barrier. Under room temperature ambient pressure, 1 10 alloy exhibited total Faradaic efficiency ~37 % at −0.83 V, appreciable current densities stability, thus featuring unconventional non‐Cu electrocatalytic capability.

Язык: Английский

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Electrochemical Reduction of Co2 on Pure and Doped Cu2o(111)

Опубликована: Янв. 1, 2024

Язык: Английский

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Fluorinated polymer zwitterions on gold nanoparticles: patterned catalyst surfaces guide interfacial transport and electrochemical CO₂ reduction

Nanoscale, Год журнала: 2024, Номер 16(33), С. 15558 - 15567

Опубликована: Янв. 1, 2024

We report the use of fluorinated polymer zwitterions to build hybrid systems for efficient CO 2 electroreduction.

Язык: Английский

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Thermodynamic and Economic Assessments of Electrochemical CO₂ Conversion to Dimethyl Ether: Trade-off between Hydrogen Gas and Water Vapor as a Proton Source

Industrial & Engineering Chemistry Research, Год журнала: 2024, Номер 63(33), С. 14582 - 14589

Опубликована: Авг. 8, 2024

Electrochemical conversion of carbon dioxide (CO2) to valuable products could provide a transformative pathway produce renewable fuels while adding value the CO2 captured at point sources. Here, we investigate thermodynamic feasibility and economic viability electrochemical reduction reaction various carbon-containing fuels. In particular, explore pathways for dimethyl ether (DME), liquid propane gas, natural gas. We compare contrast use two different proton sources, including hydrogen gas water vapor anode, on capital operating costs (OPEX) systems DME. The results indicate that electrical are most significant portion OPEX, demonstrating 0.2–0.6 $/kWh per metric ton DME production using monoxide formic acid as intermediates proved be cost-effective, levelized energy 0.28 with over 0.15 cost recovery possible through tax credits oxygen recovery.

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, Год журнала: 2024, Номер 136(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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