Promises of MOF‐Based and MOF‐Derived Materials for Electrocatalytic CO₂ Reduction

Advanced Energy Materials, Год журнала: 2024, Номер 14(39)

Опубликована: Июль 29, 2024

Abstract Electrocatalytic CO 2 reduction (ECR) powered by renewable electricity is a promising technology to mitigate carbon emissions and lessen the dependence on fossil fuels toward carbon‐neutral energy cycle. Metal–organic frameworks (MOFs) their derivatives, due excellent intrinsic activity, have emerged as materials for ECR high‐demand products. However, challenges such unsatisfactory efficiency, selectivity, relatively low production rates hinder industrial scalability. Here, comprehensive critical review presented that summarizes state‐of‐the‐art progress in MOF‐based MOF‐derived electroreduction catalysts from design functionality perspectives. The fundamentals of reaction (CO RR) over heterogeneous catalysts, mechanisms, key faced are described first establish solid foundation forthcoming in‐depth analyses. MOF's building blocks, properties, shortcomings pertinent including conductivity stability, systematically discussed. Moreover, discussions provided design, fabrication, characterization, RR activity pinpoint intricate structure‐property‐performance relationship. Finally, recommendations put forward enhancing MOF electrocatalysts durability. This work may serve guideline developing high‐performance MOF‐related RR, benefiting researchers working this growing potentially game‐changing area.

Язык: Английский

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Enigma of Sustainable CO₂ Conversion to Renewable Fuels and Chemicals Through Photocatalysis, Electrocatalysis, and Photoelectrocatalysis: Design Strategies and Atomic Level Insights

Small, Год журнала: 2025, Номер unknown

Опубликована: Янв. 2, 2025

Growing global population, escalating energy consumption, and climate change threaten future security. Fossil fuel combustion, primarily coal, oil, natural gas, exacerbates the greenhouse effect driving warming through CO

Язык: Английский

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Tailoring CO₂ Adsorption Configuration with Spatial Confinement Switches Electroreduction Product from Formate to Acetate

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Фев. 5, 2025

Multi-proton-coupled electron transfer, multitudinous intermediates, and unavoidable competing hydrogen evolution reaction during CO2 electroreduction make it tricky to control high selectivity for specific products. Here, we present spatial confinement of Fe single atoms (FeN2S2) by adjacent FeS clusters (Fe4S4) orientate the transition adsorption configuration from C,O-side O-end, which triggers a shift activated first-step protonation C–C coupling, thus switching target product HCOOH in Faraday efficiency (FE: 90.6%) on FeN2S2 CH3COOH 82.3%) Fe4S4/FeN2S2. The strength *OCHO upon solitary site is linearly related coordination number Fe–S, with predominantly produced over single-atom (ortho-substituted S atoms). Fe4S4 cluster functions as switch reduction product, can not only optimize electronic structure neighboring but also impel complete hydrocarbon intermediate *CH3, followed coupling CO2* *CH3 via synergistic catalysis This strategy provides new avenue modulate reactant model desirable pathways, potential applications diverse multistep electrochemical processes controlled selectivity.

Язык: Английский

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Enhancing CO2 photoreduction on Au@CdZnS@MnO2 hollow nanospheres via electron configuration modulation

Journal of Material Science and Technology, Год журнала: 2025, Номер unknown

Опубликована: Фев. 1, 2025

Язык: Английский

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Recent advances and future perspectives of metal-organic frameworks as efficient electrocatalysts for CO2 reduction

Science China Materials, Год журнала: 2024, Номер 68(1), С. 21 - 38

Опубликована: Ноя. 8, 2024

Abstract The conversion of carbon dioxide (CO 2 ) to the reduced chemical compounds offers substantial environmental benefits through minimizing emission greenhouse gas and fostering sustainable practices. Recently, unique properties metal-organic frameworks (MOFs) make them attractive candidates for electrocatalytic CO reduction reaction RR), providing many opportunities develop efficient, selective, environmentally processes mitigating emissions utilizing as a valuable raw material synthesis fuels chemicals. Here, recent advances in MOFs efficient catalysts RR are summarized. detailed characteristics, mechanisms, practical approaches improving efficiency, selectivity, durability under realistic conditions also clarified. Furthermore, outlooks on prospects MOF-based electrocatalysts provided.

Язык: Английский

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Comprehensive Insight Into Electronic Modulation of Rare‐Earth Elements for Enhancing Electrocatalytic Performance of Atomically Dispersed Materials

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 2, 2025

Abstract Atomically dispersed materials have been a thriving research field due to their maximum atomic utilization and remarkable performance in energy conversion storage systems. Owing the large radius, strong oxophilicity, unique electronic properties, rare‐earth (RE) elements widely investigated as oxide carriers promoters atomically manipulate regulate structure of active species. Single‐atom state with an adjustable coordination environment on N‐doped carbon endows RE metals special states outstanding catalytic performances. A thorough comprehension modulation mechanism paves way for construction advanced RE‐based electrocatalysts high activity, stability, selectivity. This review provides widespread insight into roles modulating properties combined structure–performance relationship electrocatalysis processes. The characteristic physical chemical are highlighted, synthetic strategy is discussed. Finally, summary perspectives rational design development highly efficient catalysts proposed. aims provide guideline promoting effective functional materials.

Язык: Английский

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Solvent Mediated Interfacial Microenvironment Design for High‐Performance Electrochemical CO₂ Reduction to C₂₊ Products

Small, Год журнала: 2025, Номер unknown

Опубликована: Янв. 16, 2025

Electrochemical CO2 reduction (CO2RR) in membrane electrode assembly (MEA) represents a viable strategy for converting into value-added multi-carbon (C2+) compounds. Therefore, the microstructure of catalyst layer (CL) affects local gas transport, charge conduction, and proton supply at three-phase interfaces, which is significantly determined by solvent environment. However, microenvironment CLs mechanism effect on C2+ selectivity remains elusive. Herein, tailored interfacial structure designed introducing solvent-mediated catalyst-ionomer-solvent microenvironment. The acetone surface promotion beneficial unfolded ionomers to uniformly coat catalysts, contributes enhancing hydrophobicity inhibiting hydrogen evolution. Furthermore, molecular dynamics (MD) simulation situ ATR-SEIRAS are employed elucidate appropriate network with balanced distribution H2O. uniform continuous advantageous CO2-to-C2+. optimized favors production products Cu-based MEA, exhibiting high faradaic efficiency (FE) 80.27% 400 mA cm-2.

Язык: Английский

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Recent Breakthroughs in Electrocatalytic Reduction of Nitrogen-Oxyanions for Environmentally Benign Ammonia Synthesis

Nano Energy, Год журнала: 2025, Номер unknown, С. 110683 - 110683

Опубликована: Янв. 1, 2025

Язык: Английский

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Construction of electron-rich nickel single atom catalyst by heteroatom doping for enhanced CO2 electroreduction

Journal of Catalysis, Год журнала: 2025, Номер unknown, С. 116020 - 116020

Опубликована: Фев. 1, 2025

Язык: Английский

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Hydrophobic Ionic Liquid Engineering for Reversing CO Intermediate Configuration toward Ampere-Level CO₂ Electroreduction to C₂₊ Products

Journal of the American Chemical Society, Год журнала: 2025, Номер 147(9), С. 7921 - 7931

Опубликована: Фев. 24, 2025

Hydrophobic ionic liquid (HIL) engineering on the catalyst surface represents a simple yet potent direction for optimizing CO2 electroreduction performance. However, pivotal role of HIL at an industrial current density is still ambiguous due to limited and conflicting research findings. Herein, HIL-engineered oxide-derived Cu porous nanoparticles with electron-delocalized groups specific ultramicropore structure are first constructed facilitate CO2-to-C2+ ampere-level densities. The uniformly decorated innovatively demonstrated by positron annihilation lifetime spectroscopy, which offers unparalleled advantages in characterization. Bader charge-dependent performance analyses theoretical calculations disclose that N atoms lower adsorption energy CO atop site from -0.38 -1.42 eV through electron donation, inverts most stable favors energy-efficient dimerization atop-bound CO. Operando Raman spectra situ attenuated total reflection-surface enhanced infrared absorption spectroscopy indicate adhered increases *CO coverage alters configuration state abundant high-frequency band. Furthermore, staircase potential electrochemical impedance unravels arrangement enlarges charge about 1.5 times, thereby accelerating electroreduction. As result, achieve prominent C2+ productivity Faradaic efficiency 85.1% formation rate up 2512 μmol h-1 cm-2, outperforming reported Cu-based electrocatalysts.

Язык: Английский

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