High‐Entropy Engineering Reinforced Surface Electronic States and Structural Defects of Hierarchical Metal Oxides@Graphene Fibers toward High‐Performance Wearable Supercapacitors

Advanced Materials, Год журнала: 2024, Номер 36(35)

Опубликована: Июнь 20, 2024

Abstract Construction advanced fibers with high Faradic activity and conductivity are effective to realize energy density sufficient redox reactions for fiber‐based electrochemical supercapacitors (FESCs), yet it is generally at the sacrifice of kinetics structural stability. Here, a high‐entropy doping strategy proposed develop high‐energy‐density FESCs based on doped metal oxide@graphene fiber composite (HE‐MO@GF). Due synergistic participation multi‐metal elements via doping, HE‐MO@GF features abundant oxygen vacancies from introducing various low‐valence ions, lattice distortions, optimized electronic structure. Consequently, maintains active sites, low diffusion barrier, fast adsorption kinetics, improved conductivity, enhanced stability, Faradaic reversibility. Thereinto, presents ultra‐large areal capacitance (3673.74 mF cm −2 ) excellent rate performance (1446.78 30 mA in 6 M KOH electrolyte. The HE‐MO@GF‐based solid‐state also deliver (132.85 µWh ), good cycle (81.05% capacity retention after 10,000 cycles), robust tolerance sweat erosion multiple washing, which woven into textile power wearable devices (e.g., watch, badge luminous glasses). This provides significant guidance designing innovative materials highlights development next‐generation devices.

Язык: Английский

---

3D-Printed MOF Monoliths: Fabrication Strategies and Environmental Applications

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Авг. 15, 2024

Metal-organic frameworks (MOFs) have been extensively considered as one of the most promising types porous and crystalline organic-inorganic materials, thanks to their large specific surface area, high porosity, tailorable structures compositions, diverse functionalities, well-controlled pore/size distribution. However, developed MOFs are in powder forms, which still some technical challenges, including abrasion, dustiness, low packing densities, clogging, mass/heat transfer limitation, environmental pollution, mechanical instability during process, that restrict applicability industrial applications. Therefore, recent years, attention has focused on techniques convert MOF powders into macroscopic materials like beads, membranes, monoliths, gel/sponges, nanofibers overcome these challenges.Three-dimensional (3D) printing technology achieved much interest because it can produce many high-resolution with complex shapes geometries from digital models. this review summarizes combination different 3D strategies MOF-based for fabricating 3D-printed monoliths applications, emphasizing water treatment gas adsorption/separation Herein, various fabrication such direct ink writing, seed-assisted in-situ growth, coordination replication solid precursors, matrix incorporation, selective laser sintering, light processing, described relevant examples. Finally, future directions challenges also presented better plan trajectories shaping improved control over structure, composition, textural properties monoliths.

Язык: Английский

---

High Fire‐Safety and Multifunctional Eutectogel for Flexible Quasi‐Solid‐State Supercapacitors

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 10, 2024

Abstract The preparation of high‐performance and fire‐safe electrolytes for flexible quasi‐solid‐state supercapacitors is challenging. In this work, a novel multifunctional deep eutectic solvent gel (DESG) fabricated using acrylic acid urea as hydrogen bond donors choline chloride acceptor. DESG shows high ionic conductivity (0.552 S m −1 ), good electrochemical performance (specific capacitance: 106.8 F g wide operating temperature range (−20–90 °C), being promising candidate solid‐state supercapacitors. Furthermore, it exhibits thermoelectric conversion capability (Seebeck coefficient: 1.56 mV K ideal capacitors fire‐warning sensors. prepared rapidly self‐extinguishes after removal from fire, reaching limiting oxygen index value 38.0% demonstrating its excellent flame retardancy. addition, has self‐healing (healing efficiency 84.3%). work provides new insights into the application fire‐safety eutectogels

Язык: Английский

---

Ion Exchange‐Mediated 3D Cross‐Linked ZIF‐L Superstructure for Flexible Electrochemical Energy Storage

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(36)

Опубликована: Июнь 17, 2024

Metal-organic frameworks (MOFs) are considered as a promising candidate for advancing energy storage owing to their intrinsic multi-channel architecture, high theoretical capacity, and precise adjustability. However, the low conductivity poor structural stability lead unsatisfactory rate cycling performance, greatly hindering practical application. Herein, we propose sea urchin-like Co-ZIF-L superstructure using molecular template induce self-assembly followed by ion exchange method, which shows improved conductivity, successive channels, stability. The can gradually etch superstructure, leading reconstruction of with three-dimensional (3D) cross-linked ultrathin porous nanosheets. Moreover, control Co Ni ratios construct effective micro-electric field synergistically enhance rapid transfer electrons electrolyte ions, improving CoNi-ZIF-L.

Язык: Английский

---

High‐Entropy Ag‐Ru‐based Electrocatalysts with Dual‐Active‐Center for Highly Stable Ultra‐Low‐Temperature Zinc‐Air Batteries

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Окт. 7, 2024

Abstract The development of advanced bifunctional catalysts for oxygen evolution reaction (OER) and reduction (ORR) is significant rechargeable zinc‐air batteries (ZABs). Herein, a unique dual active center alloying strategy proposed to achieve the efficient catalysis, high entropy effect further exploited modulate structure performance catalysts. MOF‐assisted pyrolysis‐replacement‐alloying method was employed construct CoCuFeAgRu high‐entropy alloy (HEA), which are uniformly anchored in porous nitrogen‐doped carbon nanosheets. Notably, obtained HEA catalyst exhibits excellent catalytic both ORR OER, peak power density 136. 53 mW cm −2 an energy 987.9 mAh g Zn −1 , surpassing most previously reported electrocatalysts. Moreover, assembled flexible ZAB enables even at ultralow temperature −40 °C, with 601.6 remarkable cycling stability up 1,650 hours. Combined experimental theoretical calculation results reveal that activity originated from synergistic Ag Ru centers, optimization electronic by effect.

Язык: Английский

---

Core–Shell Co‐Co_xP Nanoparticle‐Embedded N‐Doped Carbon Nanowhiskers Hollow Sphere for Efficient Oxygen Evolution Electrocatalysis

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Июль 26, 2024

Abstract The development of efficient oxygen evolution reaction (OER) electrocatalysts is critical to overcome the efficiency bottleneck in hydrogen generation via water electrolysis. Hollow nanostructured materials have emerged as a hot topic for electrocatalysis research because their advantages, including abundant active sites, large contact area between catalyst and electrolyte, short transmission path. As highly stable OER electrocatalysts, cobalt‐based attracted more attention. In this work, cobalt metal/cobalt phosphides/nitrogen‐doped carbon composites (Co‐Co x P/NC) with hierarchical hollow structure are designed by using ZIF‐67 microspheres precursors. By coating ZIF‐8 on surface further carbonizing, nanowhiskers successfully formed spheres under catalytic effect Co nanoparticles at high temperature. subsequent phosphating process, solid nanocrystalline particles transformed into core–shell CoP 2 P account Kirkendall effect. Through optimization microstructure material synergistic transition metal, metal phosphide, nitrogen doping, overpotential optimal only 287 mV 10 mA cm −2 current density 1 m KOH.

Язык: Английский

---

Rational Design and Controlled Synthesis of MOF-Derived Single-Atom Catalysts

Accounts of Materials Research, Год журнала: 2025, Номер unknown

Опубликована: Янв. 4, 2025

ConspectusSingle-atom catalysts (SACs) represent a transformative advancement in heterogeneous catalysis, offering unparalleled opportunities for maximizing atomic efficiency and enhancing performance. SACs are characterized by isolated metal atoms uniformly dispersed on suitable supports, ensuring each atom serves as an independent catalytic site. This dispersion mitigates aggregation, common issue conventional nanocatalysts, thus enabling superior activity, selectivity, stability. Metal–organic frameworks (MOFs) have emerged ideal platform SAC synthesis due to their structural diversity, tunable coordination environments, high surface areas. MOFs provide well-defined sites that facilitate the precise stabilization of single atoms, presenting significant advantages over traditional supports like oxides materials. Carbonization yields MOF-derived carbon materials retain key characteristics while enhanced electrical conductivity stability, making them various applications.Recent advances rational design controlled significantly improved performance electrocatalytic processes such oxygen reduction reaction (ORR) dioxide (CO2RR). However, challenges remain, including maintaining integrity during high-temperature carbonization, mass electron transport stability under conditions. To address these challenges, strategies using structure-directing agents stabilize MOF frameworks, forming high-energy porous networks, optimizing support morphologies been developed maximize active site exposure accessibility. On other hand, interplay between environments is crucial determining activity selectivity SACs. Advanced computational modeling, coupled with experimental validation, has provided insights into electronic structure interactions supports. These enabled researchers fine-tune local coordination, leading enhancements For instance, modifying environment optimizes binding strength intermediates, thereby improving both selectivity. account highlights our group's contributions SACs, focusing innovative design, functionalization, approaches enhance activity. Notable include maintain pore connectivity preserving areas, transport. We also discuss networks continuous improve interaction reactants, ultimately boosting efficiency. Techniques electrospinning employed create hierarchical structures one-dimensional nanofibers, transfer. The requires comprehensive understanding microenvironment surrounding sites, leveraging tools, can precisely control microenvironments achieve desired outcomes.MOF-derived hold substantial promise energy conversion chemical synthesis. Continued research essential optimize scalability, explore new applications, advancing sustainable catalysis. provides overview latest advancements highlighting potential next-generation electrocatalysts role technologies.

Язык: Английский

---

Metal Organic Framework Derived Heterogeneous CoNiP@CoNiSe for High Performance Asymmetric Supercapacitor

Industrial & Engineering Chemistry Research, Год журнала: 2025, Номер unknown

Опубликована: Фев. 25, 2025

Язык: Английский

---

Electronic Structure Regulation by Fe Doped Ni‐Phosphides for Long‐term Overall Water Splitting at Large Current Density

Small, Год журнала: 2024, Номер 20(46)

Опубликована: Авг. 13, 2024

Abstract Acquiring a highly efficient electrocatalyst capable of sustaining prolonged operation under high current density is paramount importance for the process electrocatalytic water splitting. Herein, Fe‐doped phosphide (Fe‐Ni 5 P 4 ) derived from NiFc metal−organic framework (NiFc‐MOF) (Fc: 1,1′‐ferrocene dicarboxylate) shows catalytic activity overall splitting (OWS). Fe‐Ni ||Fe‐Ni exhibits low voltage 1.72 V OWS at 0.5 A cm −2 and permits stable 2700 h in 1.0 m KOH. Remarkably, can sustain robust an extra‐large 1 1170 even alkaline seawater. Theoretical calculations confirm that Fe doping simultaneously reduces reaction barriers coupling desorption (O * →OOH , OOH →O 2 oxygen evolution (OER) regulates adsorption strength intermediates (H O H hydrogen (HER), enabling to possess excellent dual functional activity. This study offers valuable reference advancement durable electrocatalysts through regulation coordination frameworks, with significant implications industrial applications energy conversion technologies.

Язык: Английский

---

Frontiers in metal–organic frameworks: innovative nanomaterials for next-generation supercapacitors

Advanced Composites and Hybrid Materials, Год журнала: 2024, Номер 7(6)

Опубликована: Окт. 30, 2024

Abstract Metal–organic frameworks (MOFs) have emerged as a versatile class of porous materials with tremendous potential for various applications, including energy storage devices. This review provides comprehensive analysis recent advancements and applications MOFs in the field brief overview fundamental aspects MOFs, their synthesis, structural diversity, tuneable properties. been extensively investigated advanced systems supercapacitors. can be employed electrode materials, separators, catalysts, offering enhanced electrochemical performance, improved charge/discharge rates, prolonged cycling stability. The unique tunability allows rational design tailored desired properties, such high specific capacity, excellent conductivity, superior developments MOF-based capacitors, particularly significant progress reported achieving power densities, are noteworthy. exceptional charge capacity combined facile synthesis scalability, makes them promising candidates next-generation technologies. sheds light on challenges opportunities practical implementation devices discusses strategies enhancing stability different environments, improving electrical developing scalable methods. We briefly discuss perspectives future directions, particular focus research development use applications.

Язык: Английский

---