Crystal Engineering Enables Cobalt-Based Metal–Organic Frameworks as High-Performance Electrocatalysts for H₂O₂ Production

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(14), P. 7791 - 7799

Published: March 10, 2023

Metal-organic frameworks (MOFs) with highly adjustable structures are an emerging family of electrocatalysts in two-electron oxygen reduction reaction (2e-ORR) for H2O2 production. However, the development MOF-based 2e-ORR catalysts high selectivity and production rate remains challenging. Herein, elaborate design fine control over MOFs at both atomic nano-scale is demonstrated, enabling well-known Zn/Co bimetallic zeolite imidazole (ZnCo-ZIFs) as excellent electrocatalysts. Experimental results combined density functional theory simulation have shown that level can regulate role water molecules participating ORR process, morphology desired facet exposure adjusts coordination unsaturation degree active sites. The structural regulation two length scales leads to synchronous kinetics thermodynamics on ZIF catalysts. optimized ZnCo-ZIF a molar ratio 9/1 predominant {001} exhibits 2e- ∼100% yield 4.35 mol gcat-1 h-1. findings pave new avenue toward multivariate advanced

Language: Английский

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Metal-support interaction promoted multifunctional electrocatalysis on PtCo/NC with ultralow Pt loading for oxygen reduction reaction and zinc-air battery

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 337, P. 122976 - 122976

Published: June 9, 2023

Language: Английский

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Advances in electrochemistry of intrinsic conductive metal-organic frameworks and their composites: Mechanisms, synthesis and applications

Nano Energy, Journal Year: 2024, Volume and Issue: 122, P. 109333 - 109333

Published: Jan. 25, 2024

Language: Английский

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Understanding Advanced Transition Metal‐Based Two Electron Oxygen Reduction Electrocatalysts from the Perspective of Phase Engineering

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(25)

Published: March 8, 2024

Abstract Non‐noble transition metal (TM)‐based compounds have recently become a focal point of extensive research interest as electrocatalysts for the two electron oxygen reduction (2e − ORR) process. To efficiently drive this reaction, these TM‐based must bear unique physiochemical properties, which are strongly dependent on their phase structures. Consequently, adopting engineering strategies toward structure has emerged cutting‐edge scientific pursuit, crucial achieving high activity, selectivity, and stability in electrocatalytic This comprehensive review addresses intricate field applied to non‐noble 2e ORR. First, connotation fundamental concepts related kinetics thermodynamics succinctly elucidated. Subsequently, focus shifts detailed discussion various approaches, including elemental doping, defect creation, heterostructure construction, coordination tuning, crystalline design, polymorphic transformation boost or revive ORR performance (selectivity, stability) catalysts, accompanied by an insightful exploration phase‐performance correlation. Finally, proposes fresh perspectives current challenges opportunities burgeoning field, together with several critical directions future development electrocatalysts.

Language: Английский

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Rational Design of Organic Electrocatalysts for Hydrogen and Oxygen Electrocatalytic Applications

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(25)

Published: March 8, 2024

Abstract Efficient electrocatalysts are pivotal for advancing green energy conversion technologies. Organic electrocatalysts, as cost‐effective alternatives to noble‐metal benchmarks, have garnered attention. However, the understanding of relationships between their properties and electrocatalytic activities remains ambiguous. Plenty research articles regarding low‐cost organic started gain momentum in 2010 been flourishing recently though, a review article both entry‐level experienced researchers this field is still lacking. This underscores urgent need elucidate structure–activity relationship design suitable electrode structures, leveraging unique features like controllability compatibility real‐world applications. classified into four groups: small molecules, oligomers, polymers, frameworks, with specific structural physicochemical serving activity indicators. To unlock full potential five strategies discussed: integrated surface property modulation, membrane technologies, electrolyte affinity regulation, addition anticorrosion species, all aimed at enhancing charge efficiency, mass transfer, long‐term stability during reactions. The offers comprehensive overview current state practical applications, bridging gap paving way future developments more efficient

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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CO₂ Cycloaddition under Ambient Conditions over Cu–Fe Bimetallic Metal–Organic Frameworks

Inorganic Chemistry, Journal Year: 2023, Volume and Issue: 62(34), P. 13722 - 13730

Published: Aug. 4, 2023

Carbon dioxide cycloaddition into fine chemicals is prospective technology to solve energy crisis and environmental issues. However, high temperature pressure are usually required in the conventional reactions of CO2 with epoxides. Moreover, metal active sites play a vital role cycloaddition, but it still unclear. Herein, we select isostructural MOF-919-Cu-Fe MOF-919-Cu-Al as models promote performance clarify effects type on cycloaddition. The exposed Fe Cu Lewis acid reaches over 99.9% conversion selectivity at room 1 bar atmosphere, 3.0- 52.6-fold higher than those Al (33.8%) 1H-pyrazole-4-carboxylic acid, Fe, mixed system (1.9%), respectively. proposed mechanism demonstrated that Fe3+ facilitate ring opening epoxide activation boost reaction. This work provides new insight tune catalytic MOFs achieve for fixation.

Language: Английский

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Low‐Coordinated Conductive ZnCu Metal‐Organic Frameworks for Highly Selective H₂O₂ Electrosynthesis

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

Published: May 21, 2024

Direct electrosynthesis of hydrogen peroxide (H

Language: Английский

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Fe-Ce based metal-organic framework as a novel heterogeneous catalyst accelerating redox cycle for efficient degradation of sulfamethoxazole in wide pH ranges

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 353, P. 128356 - 128356

Published: June 13, 2024

Language: Английский

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Ultrafast Charge Transfer on Ru‐Cu Atomic Units for Enhanced Photocatalytic H₂O₂ Production

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

Published: Feb. 18, 2025

Abstract Photosensitizer‐assisted photocatalytic systems offer a solution to overcome the limitations of inherent light harvesting capabilities in catalysts. However, achieving efficient charge transfer between dissociative photosensitizer and catalyst poses significant challenge. Incorporating photosensitive components into reactive centers establish well‐defined channels is expected effectively address this issue. Herein, electrostatic‐driven self‐assembly method utilized integrate photosensitizers metal–organic frameworks, constructing atomically Ru‐Cu bi‐functional units promote local electron migration. Within newly constructed system, [Ru(bpy) 2 ] 2+ component Cu site serve as catalytic active for photocarrier generation H O production, respectively, their integration significantly reduces barriers transfer. Ultrafast spectroscopy situ characterization unveil accelerated directional over units, presenting orders magnitude improvement systems. As result, 37.2‐fold enhancement rate (570.9 µmol g −1 h ) that system (15.3 achieved. This work presents promising strategy integrating atomic‐scale achieve ultrafast enhanced performance.

Language: Английский

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