Multiscale CO₂ Electrocatalysis to C₂₊ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(17), P. 10530 - 10583

Published: Aug. 17, 2023

Electrosynthesis of value-added chemicals, directly from CO2, could foster achievement carbon neutral through an alternative electrical approach to the energy-intensive thermochemical industry for utilization. Progress in this area, based on electrogeneration multicarbon products CO2 electroreduction, however, lags far behind that C1 products. Reaction routes are complicated and kinetics slow with scale up high levels required commercialization, posing significant problems. In review, we identify summarize state-of-art progress synthesis a multiscale perspective discuss current hurdles be resolved generation reduction including atomistic mechanisms, nanoscale electrocatalysts, microscale electrodes, macroscale electrolyzers guidelines future research. The review ends cross-scale links discrepancies between different approaches extensions performance stability issues arise industrial environment.

Language: Английский

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Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(26)

Published: April 19, 2024

The electrocatalytic CO

Language: Английский

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Probing electrolyte effects on cation-enhanced CO2 reduction on copper in acidic media

Nature Catalysis, Journal Year: 2024, Volume and Issue: 7(7), P. 807 - 817

Published: June 24, 2024

Language: Английский

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Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Language: Английский

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A covalent molecular design enabling efficient CO2 reduction in strong acids

Nature Synthesis, Journal Year: 2024, Volume and Issue: 3(10), P. 1231 - 1242

Published: June 25, 2024

Language: Английский

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Addressing the Carbonate Issue: Electrocatalysts for Acidic CO₂ Reduction Reaction

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

Published: May 9, 2024

Abstract Electrochemical CO 2 reduction reaction (CO RR) powered by renewable energy provides a promising route to conversion and utilization. However, the widely used neutral/alkaline electrolyte consumes large amount of produce (bi)carbonate byproducts, leading significant challenges at device level, thereby impeding further deployment this reaction. Conducting RR in acidic electrolytes offers solution address “carbonate issue”; however, it presents inherent difficulties due competitive hydrogen evolution reaction, necessitating concerted efforts toward advanced catalyst electrode designs achieve high selectivity activity. This review encompasses recent developments RR, from mechanism elucidation design engineering. begins discussing mechanistic understanding pathway, laying foundation for RR. Subsequently, an in‐depth analysis advancements catalysts is provided, highlighting heterogeneous catalysts, surface immobilized molecular enhancement. Furthermore, progress made device‐level applications summarized, aiming develop high‐performance systems. Finally, existing future directions are outlined, emphasizing need improved selectivity, activity, stability, scalability.

Language: Английский

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Hydrophobic SiO₂ Armor: Stabilizing Cu^δ+ to Enhance CO₂ Electroreduction toward C₂₊ Products in Strong Acidic Environments

ACS Nano, Journal Year: 2024, Volume and Issue: 18(23), P. 15303 - 15311

Published: May 28, 2024

Electroreduction of CO2 in highly acidic environments holds promise for enhancing utilization efficiency. Due to the HER interference and structural instability, however, challenges improving selectivity stability toward multicarbon (C2+) products remain. In this study, we proposed an "armor protection" strategy involving deposition ultrathin, hydrophobic SiO2 onto Cu surface (Cu/SiO2) through a simple one-step hydrolysis. Our results confirmed effective inhibition by layer, leading high Faradaic efficiency (FE) up 76.9% C2+ at current density 900 mA cm–2 under strongly condition with pH 1. The observed performance surpassed reported most previously studied Cu-based catalysts CO2RR systems. Furthermore, ultrathin shell was demonstrated effectively prevent reconstruction preserve oxidation state Cuδ+ active sites during CO2RR. Additionally, it hindered accumulation K+ ions on catalyst diffusion situ generated OH– away from electrode, thereby favoring product generation. Raman analyses coupled DFT simulations further elucidated that proficiently modulated *CO adsorption behavior Cu/SiO2 reducing energy, facilitating C–C coupling. This work offers compelling rationally designing exploiting stable environments.

Language: Английский

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Acidic conditions for efficient carbon dioxide electroreduction in flow and MEA cells

Chem Catalysis, Journal Year: 2023, Volume and Issue: 3(8), P. 100670 - 100670

Published: June 21, 2023

Language: Английский

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Electrochemical CO₂ Reduction to Methanol by Cobalt Phthalocyanine: Quantifying CO₂ and CO Binding Strengths and Their Influence on Methanol Production

ACS Catalysis, Journal Year: 2023, Volume and Issue: 14(1), P. 366 - 372

Published: Dec. 19, 2023

Cobalt phthalocyanine (CoPc) is an active electrocatalyst for the sequential electrochemical reductions of CO2-to-CO and CO-to-methanol (CH3OH), it has been shown to be conversion CO2-to-CH3OH through a cascade catalysis reaction. However, in gas-fed flow electrolyzers equipped with gas diffusion electrodes (GDEs), reduction CO2 by CoPc selectively produces CO minimal CH3OH formation. Herein, we show that limited performance CO2–CO–CH3OH reactions primarily due competitive binding between species. Through microkinetic analyses, determine effective equilibrium constant three times higher than binding. The stronger suppresses CO-to-CH3OH reaction even at moderate local concentrations. Because GDE configuration enhances mass transport, exacerbate this suppression formation from CO2RR. In contrast, observed when concentration low, compared concentration. To promote methanol via reduction, propose applying modifications coordination environments strengthen regulate transport CO2.

Language: Английский

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Ultrathin, Cationic Covalent Organic Nanosheets for Enhanced CO₂ Electroreduction to Methanol

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(17)

Published: Nov. 7, 2023

Metalloporphyrins and metallophthalocyanines emerge as popular building blocks to develop covalent organic nanosheets (CONs) for CO

Language: Английский

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