High-performance heterometallic photocatalysts afforded by polyoxometalate synthons for efficient H2 production

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 666, P. 496 - 504

Published: April 9, 2024

Language: Английский

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Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Language: Английский

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Donor‐Site‐Acceptor Covalent Organic Frameworks Enable Spontaneous Nitrogen Dissociation for Boosted Photoelectrochemical Ammonia Synthesis

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(24)

Published: Feb. 5, 2024

Abstract Photoelectrochemical (PEC) technology offers new opportunities for pushing the renewable energy‐driven ammonia synthesis toward a practical level, while still facing unsatisfactory efficiency due to obstacle of dissociating inert nitrogen triple‐bonds. Herein, novel donor‐site‐acceptor system is constructed in covalent organic frameworks tackle this challenge highly efficient PEC synthesis. Highly active boron site elaborately embedded between donor and acceptor units, which can be effectively activated with continuous electron flow upon photoexcitation. With assistance solar irradiation, stubborn dissociation successfully changed from passive endothermic reaction spontaneous exothermic process, completely eliminating energy barrier rate‐determining step facilitating overall kinetics. The proof‐of‐concept achieved an excellent NRR performance remarkable Faradaic 91.6%, reaching target set by U.S. Department Energy (90%).

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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Phase-Regulated FeSe₂@(1T-2H)-MoSe₂ Derived from Anderson-Type Polyoxometalate as an Efficient Electrocatalyst for the Nitrogen Reduction Reaction

ACS Sustainable Chemistry & Engineering, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 22, 2025

Language: Английский

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Tunable metal–organic frameworks assist in catalyzing DNAzymes with amplification platforms for biomedical applications

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(21), P. 7549 - 7578

Published: Jan. 1, 2023

Various binding modes of tunable metal organic frameworks (MOFs) and functional DNAzymes (Dzs) synergistically catalyze the emergence abundant nanoplatforms.

Language: Английский

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Boosting Conductive Loss and Magnetic Coupling Based on “Size Modulation Engineering” toward Lower‐Frequency Microwave Absorption

Small, Journal Year: 2023, Volume and Issue: 20(17)

Published: Dec. 2, 2023

Abstract The rational design of absorber size is a promising strategy for obtaining excellent electromagnetic wave (EMW) absorption performance. However, achieving controllable tuning the material through simple methods challenging and associated EMW attenuation mechanisms are still unclear. In this study, sizes metal–organic frameworks (MOFs) successfully tailored by changing growth time molar ratio iron (Fe)/organic ligands. lateral vertical lengths MOFs vary in range 200 nm to 2 µm 100 1 µm, respectively. Both experiments simulations confirm that decrease MOF favors formation more conductive networks, which beneficial improving conductivity loss. Meanwhile, micromagnetic simulation reveals magnetic coupling can be effectively enhanced size, conducive improvement loss, especially low‐frequency range. reflection loss Fe‐based with optimized reaches −46.4 dB at 6.2 GHz an effective bandwidth 3.1 GHz. This work illustrates important role effect dissipation provides enhancing

Language: Английский

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Electronic Perturbation of Isolated Fe Coordination Structure for Enhanced Nitrogen Fixation

ACS Nano, Journal Year: 2023, Volume and Issue: 18(1), P. 288 - 298

Published: Nov. 13, 2023

Modulation of the local electronic structure isolated coordination structures plays a critical role in electrocatalysis yet remains grand challenge. Herein, we have achieved electron perturbation for iron via tuning spin state from high (FeN4) to medium (FeN2B2). The transition polarization facilitates penetration into antibonding π orbitals nitrogen and effectively activates molecules, thereby achieving an ammonia yield 115 μg h–1 mg–1cat. Faradaic efficiency 24.8%. In situ spectroscopic studies theoretical calculations indicate that boron coordinate sites, as acceptors, can regulate adsorption energy NxHy intermediates on Fe center. FeN2B2 sites favor NNH* intermediate formation reduce barrier rate-determining steps, thus accounting excellent fixation performance. Our strategy provides effective approach designing efficient electrocatalysts precise perturbation.

Language: Английский

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Recent advances in polyoxometalate-based materials and their derivatives for electrocatalysis and energy storage

Materials Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 8(3), P. 732 - 768

Published: Nov. 8, 2023

This review highlights the significant roles of POMs in electrocatalysis and energy storage, summarizes recent advances POM-based materials their derivatives water-splitting, CO 2 RR, NRR, SCs, rechargeable batteries.

Language: Английский

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The Electron‐Rich Interface Regulated MBene by S‐Bridge Guided to Enhance Nitrogen Fixation under Environmental Conditions

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

Published: Nov. 15, 2024

Abstract The underutilization of active sites limits the performance enhancement 2D transition metal boride (MBene) in electrocatalytic nitrogen reduction reaction (NRR). Herein, a highly efficient NRR electrocatalyst with S atoms bridging Fe and Mo on surface MBene is successfully constructed by using an site electron optimization strategy, which increases charge density around enhances activation ability catalyst to N 2 molecules. It noteworthy that FeS ‐MBene demonstrates low intrinsic potential for (−0.2 V vs RHE). more favorable adsorption comparison hydrogen atoms, thereby it can effectively inhibit evolution (HER). Under −0.2 versus RHE, ammonia yield rate 37.13 ± 1.31 µg h −1 mg , FE 55.97 2.63%. Density functional theory (DFT) calculations demonstrate serves as . formation heterostructure transfer, resulting becoming electron‐rich state favor subsequent hydrogenation steps. This work offers significant insights into design utilization MBene‐based catalysts NRR.

Language: Английский

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