Atomically Dispersed Ga Synergy Lewis Acid‐Base Pairs in F‐doped Mesoporous Cu₂O for Efficient Eletroreduction of CO₂ to C₂₊ Products

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

Published: April 22, 2024

Abstract Electroreduction of CO 2 into high‐value chemicals and fuels driven is an effective way to alleviate the environmental crisis, but it suffers from poor activity low selectivity catalyst. Single‐atom catalysts have excellent highest atomic efficiency, are widely used in 2‐electron transfer produce CO. However, electroreduction C 2+ products involves complex processes such as multi‐electron reaction competitive adsorption, so single‐atom catalysis often powerless. Herein, a Ga‐anchored F‐doped Cu O catalyst with dual active sites reported. The Lewis acid‐base pairs Ga single atom promote adsorption/activation dissociation water molecules, respectively, enhance coverage *CO *H, their synergy optimizes path. At high current density 600 mA cm −2 , FE C2+ reached 72.8 ± 3.2% remarkable stability. Experiments theory calculations demonstrate that increase key intermediate transformed *CHO through protonation reaction, which changes path C─C coupling (*OCCO) followed by (*OCCHO) energy barrier, greatly improving for products.

Language: Английский

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Atomically Dispersed Cu Active Centers: Local Structure and Mechanism Modulation for Carbon Dioxide Reduction

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

Published: Jan. 10, 2025

Abstract Reducing carbon dioxide （CO 2 ）to high‐value products using green renewable energy is a promising approach for addressing and greenhouse effect issues. Consequently, electrocatalytic CO reduction reaction (CO RR) technology has become current research hotspot. Since the discovery of high activity selectivity copper in RR, atomically dispersed Cu catalysts have garnered widespread attention due to their efficient atom utilization, unique electronic structure, outstanding catalytic performance. However, great challenge remains providing rational catalyst design principles achieve regulation product distribution. A clear understanding materials an in‐depth interpretation mechanism as well elucidation strategy progress toward different are keys building solving above problem. Therefore, this review starts with introduction advanced characterization techniques reveal structure mechanisms. Then, various optimization strategies applications producing targeted summarized discussed. Finally, perspectives on RR field future development offered.

Language: Английский

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Engineering Atom‐Scale Cascade Catalysis via Multi‐Active Site Collaboration for Ampere‐Level CO₂ Electroreduction to C₂₊ Products

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

Published: Jan. 15, 2025

Electrochemical reduction of CO2 to value-added multicarbon (C2+) productions offers an attractive route for renewable energy storage and utilization, but it remains challenging achieve high C2+ selectivity at industrial-level current density. Herein, a Mo1Cu single-atom alloy (SAA) catalyst is reported that displays remarkable Faradaic efficiency 86.4% under 0.80 A cm-2. Furthermore, the partial density over reaches 1.33 cm-2 with surpasses 74.3%. The combination operando spectroscopy functional theory (DFT) indicates as-prepared SAA enables atom-scale cascade catalysis via multi-active site collaboration. introduced Mo sites promote H2O dissociation fabricate active *H, meanwhile, Cu (Cu0) far from atom are activation toward CO. Further, CO *H captured by adjacent (Cu&+) near atom, accelerating conversion C─C coupling process. Our findings benefit design tandem electrocatalysts atomic scale transforming products rate.

Language: Английский

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Unveiling the role of heteroatom doping and strain in Core-Shell catalysts for CO2RR

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 160155 - 160155

Published: Feb. 1, 2025

Language: Английский

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Enhancing C-C Coupling in CO2 Electroreduction by Engineering Pore Size of Porous Carbon-Supported Cu Catalysts

Catalysts, Journal Year: 2025, Volume and Issue: 15(3), P. 199 - 199

Published: Feb. 20, 2025

The electroreduction of CO2 (CO2RR) is a promising and environmentally sustainable approach to closing the carbon cycle. However, achieving high activity selectivity for multicarbon (C2₊) products remains significant challenge due complexity reaction pathways. In this study, porous carbon-supported copper catalysts (CuHCS) with pore sizes 120 nm (CuHCS120) 500 (CuHCS500) were synthesized tailor microenvironment at electrode–electrolyte interface enhance product selectivity. CuHCS120 achieved maximum faradaic efficiency (FE) C2₊ 46%, double that CuHCS500 (23%). contrast, showed higher FE CO (36%) compared (14%) same potential. In-depth ex situ in investigations revealed smaller pores promote enrichment adsorption *CO intermediates, thereby enhancing C–C coupling formation products. These findings underscore critical role structural confinement modulating catalytic provide valuable insights rational design advanced CO2RR.

Language: Английский

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

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

Published: Oct. 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.

Language: Английский

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Constructing Ag/Cu2O interface for efficient neutral CO2 electroreduction to C2H4

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

Published: Oct. 29, 2024

Abstract Neutral CO 2 electroreduction to multi‐carbons (C 2+ ) offers a promising pathway reduce the and energy losses originating from carbonate formation. However, sluggish kinetics of C−C coupling brings significant challenge achieving high selectivity single product (such as ethylene), especially at industrial‐relevant current densities (>300 mA cm −2 ). Here, we reported an optimized Ag‐Cu O interfacial catalyst that exhibited C Faradaic efficiency (FE) 73.6 % 650 in flow cell. Remarkably, it obtained FE C2H4 66.0 with partial density 429.1 , making stand out among Cu‐based electrocatalysts. In situ Raman spectra uncovered Ag/Cu interfaces enabled coverage *CO around partially reduced Cu + /Cu 0 active sites. Furthermore, theoretical calculations demonstrated enhanced formation interface. This work unprecedented neutral H 4 performance provided in‐depth comprehension role bimetallic

Language: Английский

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Catalyst design for the electrochemical reduction of carbon dioxide: from copper nanoparticles to copper single atoms

Microstructures, Journal Year: 2025, Volume and Issue: 5(1)

Published: Jan. 17, 2025

Carbon dioxide reduction reaction (CO2RR) is an efficacious method to mitigate carbon emissions and simultaneously convert CO2 into high-value products. The efficiency of CO2RR depends on the development highly active selective catalysts. Copper (Cu)-based catalysts can effectively reduce hydrocarbons oxygen-containing compounds because their unique geometric electronic structures. Most importantly, Cu multiple products (C2+). Therefore, this review aims outline recent research progress in Cu-based for CO2RR. After introducing mechanism electroreduction reaction, we summarize influence size, morphology, coordination environment single component performance, especially performance control that contain nano or single-atom sites. Then, synergistic regulation strategies doping other metals are summarized. Finally, supports used reviewed. prospects challenges discussed.

Language: Английский

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Stepwise Coordination Engineering of Pt₁/Au₂₅ Dual Catalytic Sites with Enhanced Electrochemical Activity and Stability

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

Published: Feb. 2, 2025

Dual-site catalysts hold significant promise for accelerating complex electrochemical reactions, but a major challenge remains in balancing high loading with precise dual-site architecture to achieve optimal activity, stability, and specificity simultaneously. Herein, strategy of stepwise targeted coordination engineering is introduced co-anchor Pt single atoms (Pt1, 1.41 wt.%) Au25(SG)18 nanoclusters (Au25, 18.92 loadings on graphitic carbon nitride (g-C3N4). This approach ensures that Pt1 Au25 occupy distinct surface sites the g-C3N4 substrate, providing excellent stability unprecedented activity. In catalysis As(III), sensitivity 8.32 µA ppb-1 achieved, more than double previously reported values under neutral conditions. The enhanced detection limit (0.2 ppb) crucial monitoring water quality protecting public health from arsenic contamination, environmental risk. Furthermore, formation Pt─As As─S bonds facilitates easier breakage As─O bonds, thereby lowering reaction barrier energy rate-determining step significantly enhancing arsenious acid efficiency. These results not only offer an intriguing constructing highly efficient heterogeneous also reveal atomic-scale catalytic mechanisms drive

Language: Английский

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Progress in Cu‐Based Catalyst Design for Sustained Electrocatalytic CO₂ to C₂₊ Conversion

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

Published: Feb. 27, 2025

Abstract The electrocatalytic conversion of CO 2 into valuable multi‐carbon (C 2+ ) products using Cu‐based catalysts has attracted significant attention. This review provides a comprehensive overview recent advances in catalyst design to improve C selectivity and operational stability. It begins with an analysis the fundamental reaction pathways for formation, encompassing both established emerging mechanisms, which offer critical insights design. In situ techniques, essential validating these by real‐time observation intermediates material evolution, are also introduced. A key focus this is placed on how enhance through manipulation, particularly emphasizing catalytic site construction promote C─C coupling via increasing * coverage optimizing protonation. Additionally, challenge maintaining activity under conditions discussed, highlighting reduction active charged Cu species materials reconstruction as major obstacles. To address these, describes strategies preserve sites control including novel utilization mitigation reconstruction. By presenting developments challenges ahead, aims guide future conversion.

Language: Английский

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