Oxygen-Bridged Cu Binuclear Sites for Efficient Electrocatalytic CO₂ Reduction to Ethanol at Ultralow Overpotential

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(13), P. 9365 - 9374

Published: March 21, 2024

Electrocatalytic CO2 reduction (CO2RR) to alcohols offers a promising strategy for converting waste into valuable fuels/chemicals but usually requires large overpotentials. Herein, we report catalyst comprising unique oxygen-bridged Cu binuclear sites (CuOCu-N4) with Cu···Cu distance of 3.0–3.1 Å and concomitant conventional Cu–N4 mononuclear on hierarchical nitrogen-doped carbon nanocages (hNCNCs). The exhibits state-of-the-art low overpotential 0.19 V (versus reversible hydrogen electrode) ethanol an outstanding Faradaic efficiency 56.3% at ultralow potential −0.30 V, high-stable active-site structures during the CO2RR as confirmed by operando X-ray adsorption fine structure characterization. Theoretical simulations reveal that CuOCu-N4 greatly enhance C–C coupling potentials, while Cu-N4 hNCNC support increase local CO concentration production CuOCu-N4. This study provides convenient approach advanced site catalysts deep understanding mechanism.

Language: Английский

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Integrated comprehensive protection coating achieved by ligand engineering modulated MXene@LDH heterojunction with anti-corrosion, electromagnetic wave absorption and fire safety

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 486, P. 150444 - 150444

Published: March 15, 2024

Language: Английский

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Anion Modulation of Ag‐Imidazole Cuboctahedral Cage Microenvironments for Efficient Electrocatalytic CO2 Reduction

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(31)

Published: May 20, 2024

How to achieve CO

Language: Английский

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MOF-Based Electrocatalysts: An Overview from the Perspective of Structural Design

Chemical Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 18, 2025

The electrocatalytic technique, as an efficient energy storage and conversion technology, has attracted significant attention to address exhaustion environmental pollution. Usually, the activity selectivity of reactions are largely dominated by dynamic process occurring on electrocatalysts. Therefore, high-performance electrocatalysts, which can dominate pathway barrier reactions, great significance for advancement technique. Metal-organic frameworks (MOFs), emerging crystalline porous materials, present structural component advantages including well-defined structure, high surface area, large porosity, diverse components, easy tailorability, demonstrating fantastic potential precise fabrication In this Review, strategies in electrocatalysts based MOF-related materials specifically introduced from aspects catalytic site design microenvironment modulation around sites. Furthermore, representative progress achieved various applications employing MOF-based is systematically summarized, with special emphasis MOFs performance optimization. Finally, remaining challenges future perspectives further highlighted.

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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Assembly of Amorphizing Porous Bimetallic Metal‐Organic Frameworks Spheres with Zn─O─Fe Cluster and Coordination Deficiency via Ligand Competition for Efficient Electro‐Fenton Catalysis

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(36)

Published: April 23, 2024

Abstract Electro‐Fenton process stands out as a highly promising approach for generating reactive oxygen‐containing radicals to address the escalating issue of environmental pollution. However, long‐term goal application necessitates ongoing pursuit high‐quality catalysts with both sufficient activity and stability. Herein, general route is reported large‐scale synthesis amorphizing porous bimetallic metal‐organic framework (MOF) spheres Zn─O─Fe structure coordination deficiency through facile low‐cost ligand competition. Assisted by modulator, deprotonation terephthalic acid accelerated rapid amorphous MOF successfully achieved at room temperature. As inactive metal Zn introduced into clusters MOFs, cycling efficiency Fe 3+ /Fe 2+ improved secondary building unit constructed, greatly accelerating electron conduction rate. Compared crystalline spindle cMIL‐88B(Fe 2 Zn) traditional solvothermal route, aMIL‐88B(Fe has unique spherical larger surface area, higher conductivity, more exposed active sites. Endowed textural chemistry, exhibits superior catalytic in degradation refractory organic pollutants. The progress offers feasible way rational design iron‐based hybrid materials tunable structures enhance properties various applications.

Language: Английский

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Precise synthesis of dual atom sites for electrocatalysis

Nano Research, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 17, 2024

Language: Английский

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Promotion of C─C Coupling in the CO₂ Electrochemical Reduction to Valuable C₂₊ Products: From Micro‐Foundation to Macro‐Application

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

Published: Feb. 2, 2025

Abstract The electrochemical CO 2 reduction reaction (CO RR) to valuable C 2+ products emerges as a promising strategy for converting intermittent renewable energy into high‐energy‐density fuels and feedstock. Leveraging its substantial commercial potential compatibility with existing infrastructure, the conversion of multicarbon hydrocarbons oxygenates (C ) holds great industrial promise. However, process is hampered by complex multielectron‐proton transfer reactions difficulties in reactant activation, posing significant thermodynamic kinetic barriers commercialization production. Addressing these necessitates comprehensive approach encompassing multiple facets, including effective control C─C coupling electrolyzers using efficient catalysts optimized local environments. This review delves advancements outstanding challenges spanning from microcosmic macroscopic scales, design nanocatalysts, optimization microenvironment, development electrolyzers. By elucidating influence electrolyte environment, exploring flow cells, guidelines are provided future research aimed at promoting coupling, thereby bridging microscopic insights applications field electroreduction.

Language: Английский

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Progress of pristine metal-organic frameworks for electrocatalytic applications

Journal of Material Science and Technology, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 1, 2025

Language: Английский

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Regulating the Critical Intermediates of Dual‐Atom Catalysts for CO₂ Electroreduction

Small, Journal Year: 2024, Volume and Issue: unknown

Published: May 27, 2024

Electrocatalysis is a very attractive way to achieve sustainable carbon cycle by converting CO

Language: Английский

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