Direct Electrochemical Reduction of CO₂ to C₂₊ Chemicals: Catalysts, Microenvironments, and Mechanistic Understanding

ACS Energy Letters, Journal Year: 2025, Volume and Issue: 10(1), P. 600 - 619

Published: Jan. 2, 2025

The electrochemical reduction reaction of CO2 (eCO2RR) to chemicals presents a viable solution for addressing climate change and sustainable manufacturing. In this Review, we describe the recent advancements in eCO2RR multicarbon (C2+) production from aspects catalyst structure, microenvironments, mechanistic understanding. We draw experimental theoretical comparisons between systems containing bulk highly dispersed metals, alloys, metal compounds recount new results microenvironmental impacts as well catalytic mechanism. From our own studies, offer some viewpoints on electrocatalytic mechanism during complex multistep proton-coupled electron transfers propose several research directions unlocking full potential scalable industrial CO2-to-C2+ conversion.

Language: Английский

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Probing Photocatalytic Reduction Pathways of CO₂ by Catalyst PbBiO₂Br Using In-Situ Raman Spectroscopy

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 3153 - 3161

Published: Feb. 6, 2025

Language: Английский

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Selective CO₂ electroreduction to multicarbon products exceeding 2 A cm⁻² in strong acids via a hollow-fiber Cu penetration electrode

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(2), P. 510 - 517

Published: Dec. 13, 2023

Sufficient CO 2 feeding induced by the hollow-fiber penetration configuration greatly improved coverage on Cu active sites in strong acids, favoring activation, *CHO and *CO formation, their couplings to C 2+ products.

Language: Английский

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Cu-based catalyst designs in CO₂ electroreduction: precise modulation of reaction intermediates for high-value chemical generation

Chemical Science, Journal Year: 2023, Volume and Issue: 14(47), P. 13629 - 13660

Published: Jan. 1, 2023

The massive emission of excess greenhouse gases (mainly CO

Language: Английский

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A review on electrocatalytic CO₂ conversion via C–C and C–N coupling

Carbon Energy, Journal Year: 2024, Volume and Issue: 6(2)

Published: Feb. 1, 2024

Abstract Electrochemical C–C and C–N coupling reactions with the conversion of abundant inexpensive small molecules, such as CO 2 nitrogen‐containing species, are considered a promising route for increasing value reduction products. The development high‐performance catalysts is key to both electrocatalytic reactions. In this review, we present systematic summary reaction systems reduction, along mechanisms bonds over outstanding materials recently developed. intermediate species pathways related well catalyst‐structure relationship will be also discussed, aiming provide insights guidance designing efficient systems.

Language: Английский

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Microenvironment Engineering of Heterogeneous Catalysts for Liquid-Phase Environmental Catalysis

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(20), P. 11348 - 11434

Published: Oct. 9, 2024

Environmental catalysis has emerged as a scientific frontier in mitigating water pollution and advancing circular chemistry reaction microenvironment significantly influences the catalytic performance efficiency. This review delves into engineering within liquid-phase environmental catalysis, categorizing microenvironments four scales: atom/molecule-level modulation, nano/microscale-confined structures, interface surface regulation, external field effects. Each category is analyzed for its unique characteristics merits, emphasizing potential to enhance efficiency selectivity. Following this overview, we introduced recent advancements advanced material system design promote (e.g., purification, transformation value-added products, green synthesis), leveraging state-of-the-art technologies. These discussions showcase was applied different reactions fine-tune regimes improve from both thermodynamics kinetics perspectives. Lastly, discussed challenges future directions engineering. underscores of intelligent materials drive development more effective sustainable solutions decontamination.

Language: Английский

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Unveiling Photochemical CO2 Reduction Processes on PbBiO2I/GO Surfaces: Insights from In-Situ Raman Spectroscopy

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124844 - 124844

Published: Nov. 1, 2024

Language: Английский

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Metal‐Organic Frameworks‐Based Copper Catalysts for CO₂ Electroreduction Toward Multicarbon Products

Exploration, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 12, 2025

ABSTRACT Copper (Cu) is the most promising catalyst for electrochemical CO 2 ‐to‐C 2+ conversion, whereas performance remains below practical thresholds due to high energy barrier of C−C coupling and lack effective approaches steer reaction pathway. Recent advances show that metal‐organic frameworks (MOF) could be a platform as support, pre‐catalyst, co‐catalyst modify electronic structure local environment Cu catalysts promoting reduction by virtue their great tunability over compositions pore architectures. In this review, we discussed general design principles, catalytic mechanisms, achievements MOF‐based catalysts, aiming boost refinement steering pathway C products. The fundamentals challenges are first introduced. Then, summarized conceptions from three aspects: engineering properties Cu, regulating environment, managing site exposure mass transport. Further, latest progress products namely Cu‐based MOF, MOF‐derived Cu@MOF hybrid discussed. Finally, future research opportunities strategies suggested innovate rational advanced electrifying transformation.

Language: Английский

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Establishment of Gas–Liquid–Solid Interface on Multilevel Porous Cu₂O for Potential-Driven Selective CO₂ Electroreduction toward C₁ or C₂ Products

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

Published: Jan. 20, 2025

Copper-based catalysts demonstrate distinctive multicarbon product activity in the CO2 electroreduction reaction (CO2RR); however, their low selectivity presents significant challenges for practical applications. Herein, we have developed a multilevel porous spherical Cu2O structure, wherein mesopores are enriched with catalytic active sites and effectively stabilize Cu+, while macropores facilitate formation of "gas–liquid–solid" three-phase interface, thereby creating microenvironment an increasing water concentration gradient from interior to exterior. Potential-driven phase engineering protonation synergistically optimize pathway, facilitating switch between CO C2H4. At current density 100 mA cm–2, faradaic efficiency (FE) reaches impressive 96.97%. When increases 1000 FEC2H4 attains 53.05%. Experiments theoretical calculations indicate that at lower potentials, pure diminishes adsorption *CO intermediates, weak inhibits hydrogen evolution reactions, promoting production. Conversely, more negative Cu0/Cu+ interface strong generate locally elevated concentrations *COOH which enhance C–C coupling deep hydrogenation, ultimately improving toward C2+ products. This study provides novel insights into rational design copper-based customizable

Language: Английский

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Enhancing C₂₊ product selectivity in CO₂ electroreduction by enriching intermediates over carbon-based nanoreactors

Chemical Science, Journal Year: 2024, Volume and Issue: 15(22), P. 8451 - 8458

Published: Jan. 1, 2024

A carbon-based nanoreactor could enrich *CO intermediates through steric confinement, thus facilitating electrocatalytic C–C coupling.

Language: Английский

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