Metal‐Organic Frameworks: Direct Synthesis by Organic Acid‐Etching and Reconstruction Disclosure as Oxygen Evolution Electrocatalysts

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(11)

Published: Jan. 22, 2024

Abstract Metal‐organic frameworks (MOFs) have emerged as promising oxygen evolution reaction (OER) electrocatalysts. Chemically bonded MOFs on supports are desirable yet lacking in routine synthesis, they may allow variable structural and the underlying structure‐activity relationship to be disclosed. Herein, direct MOF synthesis is achieved by an organic acid‐etching strategy (AES). Using π‐conjugated ferrocene (Fc) dicarboxylic acid etching agent ligand, a series of MFc‐MOF (M=Ni, Co, Fe, Zn) nanosheets synthesized metal supports. The crystal structure studied using X‐ray diffraction low‐dose transmission electron microscopy, which quasi ‐lattice‐matched with that metal, enabling situ growth. Operando Raman attenuated total reflectance Fourier transform infrared spectroscopy disclose NiFc‐MOF features dynamic rebuilding during OER. reconstructed one showing optimized electronic structures upshifted d ‐band center, high M−O bonding state occupancy, localized electrons adsorbates indicated density functional theory calculations, exhibits outstanding OER performance fairly low overpotential (130 mV at 10 mA cm −2 ) good stability (144 h). newly established approach for reconstruction disclosure stimulate development more prudent catalysts advancing

Language: Английский

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Boosting oxygen evolution reaction by FeNi hydroxide-organic framework electrocatalyst toward alkaline water electrolyzer

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Aug. 23, 2024

The oxygen evolution reaction plays a vital role in modern energy conversion and storage, developing cost-efficient catalysts with industrially relevant activity durability is highly desired but still challenging. Here, we report an efficient durable FeNi hydroxide organic framework nanosheet array catalyst that competently affords long-term at industrial-grade current densities alkaline electrolyte. desirable high-intensity performance attributed to three aspects as follows. First, two-dimensional porous arrays maximum specific surface facilitate mass/charge transfer accommodate high-current-density catalysis. Second, situ derived motifs offer bimetallic synergistic catalysis centers high intrinsic activity. Third, carboxyl ligands alleviate metal oxidation favorable for charge tolerability against peroxidation dissolution under strong polarization. As result, this requires overpotential of only 280 mV deliver density up 1 A/cm2 long over 1000 h. Moreover, water electrolyzer alternative demonstrates increased economic effectiveness compared commercial levels present. Developing crucial various technologies. Here the authors NiFe

Language: Английский

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Tailoring the Electrochemical Responses of MOF‐74 Via Dual‐Defect Engineering for Superior Energy Storage

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(31)

Published: May 23, 2024

Rationally designed defects in a crystal can confer unique properties. This study showcases novel dual-defects engineering strategy to tailor the electrochemical response of metal-organic framework (MOF) materials used for energy storage. Salicylic acid (SA) is identified as an effective modulator control MOF-74 growth and induce structural defects, cobalt cation doping adopted introducing second type defect. The resulting engineered bimetallic MOF exhibits discharging capacity 218.6 mAh g

Language: Английский

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Interfacial Electronic Interactions Between Ultrathin NiFe‐MOF Nanosheets and Ir Nanoparticles Heterojunctions Leading to Efficient Overall Water Splitting

Advanced Science, Journal Year: 2024, Volume and Issue: 11(28)

Published: April 26, 2024

Abstract Creating specific noble metal/metal‐organic framework (MOF) heterojunction nanostructures represents an effective strategy to promote water electrolysis but remains rather challenging. Herein, a electrocatalyst is developed by growing Ir nanoparticles on ultrathin NiFe‐MOF nanosheets supported nickel foam (NF) via readily accessible solvothermal approach and subsequent redox strategy. Because of the electronic interactions between nanosheets, optimized Ir@NiFe‐MOF/NF catalyst exhibits exceptional bifunctional performance for hydrogen evolution reaction (HER) ( η 10 = 15 mV, denotes overpotential) oxygen (OER) 213 mV) in 1.0 m KOH solution, superior commercial recently reported electrocatalysts. Density functional theory calculations are used further investigate shedding light mechanisms behind enhanced HER OER performance. This work details promising design development efficient electrocatalysts overall splitting.

Language: Английский

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Design and regulation of defective electrocatalysts

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

This review focuses on the synthesis and characterization of defective electrocatalysts, internal correlation between defects catalytic activity, development application electrocatalysts in various fields.

Language: Английский

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Electric Field Redistribution Triggered Surface Adsorption and Mass Transfer to Boost Electrocatalytic Glycerol Upgrading Coupled with Hydrogen Evolution

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(29)

Published: May 5, 2024

Abstract Electrocatalytic glycerol oxidation reaction (GOR) stands out as an economical and prospective technology to replace oxygen evolution for co‐producing high‐valued chemicals hydrogen (H 2 ). Regulating the adsorption of (GLY) hydroxyl (OH) species is great significance improving GOR performance. Herein, a hierarchical p–n heterojunction by combining Co‐metal organic framework (MOF) nanosheets with CuO nanorod arrays (CuO@Co‐MOF) developed realize optimization on GOR. Specifically, CuO@Co‐MOF electrode exhibits superior performance conversion 98.4%, formic acid (FA) selectivity 87.3%, Faradaic efficiency (FE) 98.9%. The flow‐cell system bifunctional pairing (HER) reveals better energy efficiency. Experimental results theoretical calculations unravel redistributed electric field introducing Co‐containing that contribute improved performance, which not only enhances OH but also modulates excessive GLY CuO, thus reducing barriers FA desorption. Simultaneously, finite element analysis novelty structure can increase concentration − facilitate mass transfer in solution.

Language: Английский

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Structure–Activity Relationships in Oxygen Electrocatalysis

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

Published: Sept. 30, 2024

Abstract Oxygen electrocatalysis, as the pivotal circle of many green energy technologies, sets off a worldwide research boom in full swing, while its large kinetic obstacles require remarkable catalysts to break through. Here, based on summarizing reaction mechanisms and situ characterizations, structure–activity relationships oxygen electrocatalysts are emphatically overviewed, including influence geometric morphology chemical structures electrocatalytic performances. Subsequently, experimental/theoretical is combined with device applications comprehensively summarize cutting‐edge according various material categories. Finally, future challenges forecasted from perspective catalyst development applications, favoring researchers promote industrialization electrocatalysis at an early date.

Language: Английский

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Construction of 2D CoFe-MOF derived from LDH electrocatalyst for efficient oxygen and urea evolution

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 684, P. 243 - 250

Published: Jan. 15, 2025

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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Diffusion-programmed catalysis in nanoporous material

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Feb. 3, 2025

Abstract In the realm of heterogeneous catalysis, diffusion reactants into catalytically active sites stands as a pivotal determinant influencing both turnover frequency and geometric selectivity in product formation. While accelerated can elevate reaction rates, it often entails compromise selectivity. Porous catalysts, including metal-organic covalent organic frameworks, confront formidable obstacles regulating reactant rates. Consequently, chemical functionality catalysts typically governs This study presents an approach harnessing length to achieve improved manipulation reactant-active site residence time at augment kinetics. Through deployment thin film composed porous framework catalyst, we illustrate how programming within cross-flow microfluidic catalytic reactor concurrently amplify (exceeding 1000-fold) enhance ( ~ 2-fold) relative conventional nano/microcrystals catalyst one-pot reactor. diffusion-programed strategy represents robust solution surmount constraints imposed by bulk marking advancement design catalyst-driven reactions.

Language: Английский

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