Ligands Defect-Induced Structural Self-Reconstruction of Fe–Ni–Co-Hydroxyl Oxides with Crystalline/Amorphous Heterophase from a 2D Metal–Organic Framework for an Efficient Oxygen Evolution Reaction

ACS Catalysis, Год журнала: 2024, Номер 14(3), С. 1553 - 1566

Опубликована: Янв. 16, 2024

The two-dimensional (2D) Fe–Ni–Co-MOF is synthesized using a simple double ligand strategy at room temperature. surface reconstruction process transforms it into crystalline–amorphous heterojunction composed of polycrystalline metal (oxy)hydroxide (MOOH) and amorphous oxides/hydroxides with terephthalic acid (TPA) by coordination covalent bonding. In situ Raman spectroscopy discloses the dynamic structure conversion. Density functional theory (DFT), Fourier transform infrared (FTIR), solid-state nuclear magnetic resonance (SSNMR) reveal induction defects on enhancing effect TPA oxygen evolution reaction (OER) performance through interaction. amorphous–crystalline Fe–Ni–CoOOH-TPA has numerous structural high electrical conductivity, resulting in an efficient stable OER overpotentials 236 mV 10 mA cm–2. It also been observed that catalyst processes self-healing idle state, arising from reversible conversion MOOH to M(OH)2. This work reveals compositional transformation 2D during reconstruction, elucidating relationship between electrocatalytic water-splitting metal–organic framework (MOF)-based catalysts. proven appropriate interactions enhance electrocatalysts.

Язык: Английский

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Synthesis, properties, and applications of high-entropy oxide ceramics: Current progress and future perspectives

Journal of Alloys and Compounds, Год журнала: 2023, Номер 960, С. 170690 - 170690

Опубликована: Май 23, 2023

Язык: Английский

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High Entropy Sulfide Nanoparticles as Lithium Polysulfide Redox Catalysts

ACS Nano, Год журнала: 2023, Номер 17(18), С. 18402 - 18410

Опубликована: Сен. 17, 2023

The polysulfide shuttle contributes to capacity loss in lithium-sulfur batteries, which limits their practical utilization. Materials that catalyze the complex redox reactions responsible for are emerging, but foundational knowledge enables catalyst development remains limited with only a small number of catalysts identified. Here, we employ rigorous electrochemical approach show quantitatively lithium reaction is catalyzed by nanoparticles high entropy sulfide material, Zn0.30Co0.31Cu0.19In0.13Ga0.06S. When 2% weight added sulfur cathode composite, and Coulombic efficiency resulting battery improved at both moderate (0.2 C) (1 charge/discharge rates. Surface analysis using X-ray photoelectron spectroscopy provides important insights into how material evolves during cycling process. Zn0.30Co0.31Cu0.19In0.13Ga0.06S nanoparticle outperformed constituent metal sulfides, pointing role high-entropy "cocktail effect" can play advanced electrocatalytic materials performance.

Язык: Английский

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High‐Entropy Photothermal Materials

Advanced Materials, Год журнала: 2024, Номер 36(24)

Опубликована: Март 4, 2024

Abstract High‐entropy (HE) materials, celebrated for their extraordinary chemical and physical properties, have garnered increasing attention broad applications across diverse disciplines. The expansive compositional range of these materials allows nuanced tuning properties innovative structural designs. Recent advances been centered on versatile photothermal conversion capabilities, effective the full solar spectrum (300–2500 nm). HE effect, coupled with hysteresis diffusion, imparts desirable thermal stability. These attributes position as a revolutionary alternative to traditional signifying transformative shift in technology. This review delivers comprehensive summary current state knowledge regarding emphasizing intricate relationship between compositions, structures, light‐absorbing mechanisms, optical properties. Furthermore, outlines notable contributions areas, such water evaporation, personal management, thermoelectric generation, catalysis, biomedical applications. culminates presenting roadmap that prospective directions future research this burgeoning field, also fruitful ways develop advanced expand promising

Язык: Английский

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Ultrathin High‐Entropy Fe‐Based Spinel Oxide Nanosheets with Metalloid Band Structures for Efficient Nitrate Reduction toward Ammonia

Advanced Materials, Год журнала: 2024, Номер 36(27)

Опубликована: Апрель 19, 2024

Abstract Spinel oxides with tunable chemical compositions have emerged as versatile electrocatalysts, however their performance is greatly limited by small surface area and low electron conductivity. Here, ultrathin high‐entropy Fe‐based spinel nanosheets are rationally designed (i.e., (Co 0.2 Ni Zn Mg Cu )Fe 2 O 4 ; denotes A 5 Fe ) in thickness of ≈4.3 nm large highly exposed active sites via a modified sol–gel method. Theoretic experimental results confirm that the bandgap significantly smaller than ordinary oxides, realizing transformation binary oxide from semiconductors to metalloids. As result, such manifest excellent for nitrate reduction reaction (NO 3 − RR) ammonia (NH ), NH yield rate ≈2.1 mmol h −1 cm −2 at −0.5 V versus Reversible hydrogen electrode, outperforming other spinel‐based electrocatalysts. Systematic mechanism investigations reveal NO RR mainly occurred on sites, introducing tetrahedral regulates adsorption strength N O‐related intermediates boosting RR. The above findings offer platform regulate enhance electrocatalytic oxides.

Язык: 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, Год журнала: 2024, Номер 11(33)

Опубликована: Июль 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.

Язык: Английский

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High-entropy oxides for energy-related electrocatalysis

Materials Today Catalysis, Год журнала: 2024, Номер 4, С. 100039 - 100039

Опубликована: Янв. 17, 2024

Electrocatalysis plays a crucial role in the conversion and storage of renewable energy, offering significant potential for addressing energy crisis environmental concerns. High-entropy oxides (HEOs), class emerging functional materials, have gained increasing attention electrocatalysis due to their stable crystal structure, exceptional geometric compatibility, unique electronic balance factors, abundant active sites. In this comprehensive review, we present recent advancements utilizing HEOs as catalysts various energy-based electrocatalytic reactions. We begin with an overview that includes definitions, fundamental properties, theoretical investigations. Subsequently, describe different synthetic methods while highlighting two newly-developed techniques. Furthermore, extensively discuss developments HEO-based electrocatalysts diverse structures such rock-salt-type, rutile-type, spinel-type, perovskite-type, other specially-structured HEOs. Special emphasis is placed on designed strategies aimed at enhancing performance exploring correlations between structure/ composition performance. Finally, provide concluding remarks along perspectives future opportunities exciting field.

Язык: Английский

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Designing with A-site cation defects in LaFeO3: Removal of tetracycline hydrochloride in complex environments using photo-Fenton synergy

Chemical Engineering Journal, Год журнала: 2024, Номер 484, С. 149613 - 149613

Опубликована: Фев. 15, 2024

Язык: Английский

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Two-Dimensional High-Entropy Selenides for Boosting Visible-Light-Driven Photocatalytic Performance

ACS Nano, Год журнала: 2024, Номер 18(31), С. 20740 - 20750

Опубликована: Июль 23, 2024

High-entropy materials (HEMs) have garnered extensive attention owing to their diverse and captivating physicochemical properties. Yet, fine-tuning morphological properties of HEMs remains a formidable challenge, constraining potential applications. To address this, we present rapid, low-energy consumption diethylenetriamine (DETA)-assisted microwave hydrothermal method for synthesizing series two-dimensional high-entropy selenides (HESes). Subsequently, the obtained HESes are harnessed photocatalytic water splitting. Noteworthy is optimized HESes, Cd

Язык: Английский

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Constructing High‐Performance Cobalt‐Based Environmental Catalysts from Spent Lithium‐Ion Batteries: Unveiling Overlooked Roles of Copper and Aluminum from Current Collectors

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(32)

Опубликована: Май 15, 2024

Abstract Converting spent lithium‐ion batteries (LIBs) cathode materials into environmental catalysts has drawn more and attention. Herein, we fabricated a Co 3 O 4 ‐based catalyst from LiCoO 2 LIBs (Co ‐LIBs) found that the role of Al Cu current collectors on its performance is nonnegligible. The density functional theory calculations confirmed doping and/or upshifts d‐band center Co. A Fenton‐like reaction based peroxymonosulfate (PMS) activation was adopted to evaluate activity. Interestingly, strengthened chemisorption for PMS (from −2.615 eV −2.623 eV) shortened Co−O bond length 2.540 Å 2.344 Å) between them, whereas reduced interfacial charge‐transfer resistance 28.347 kΩ 6.689 kΩ) excepting enhancement above characteristics. As expected, degradation activity toward bisphenol ‐LIBs (0.523 min −1 ) superior prepared commercial CoC (0.287 ). Simultaneously, reasons improved were further verified by comparing with doped . This work reveals elements LIBs, which beneficial sustainable utilization LIBs.

Язык: Английский

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