Conjugated Coordination Polymer Aerogels with Increased Accessibility of Well‐Defined Single‐Atom Metal Sites as a New Paradigm of Electrocatalysts

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 24, 2025

Developing high-performance single-atom catalysts (SACs) with maximum metal utilization efficiency is of significance, which presents enormous potentials to be extensively applied. It desired yet challenging elaborately tailor the coordination structures active sites in SACs and simultaneously enable sufficient accessibility these reactants. Here, a facile general strategy prepare conjugated polymer aerogels (CCPA) porous architectures that can markedly increase their elaborately-tailored sites, as new electrocatalyst paradigm fully present both structural advantages aerogel materials, reported. Taking nickel (Ni) an example, Ni-based CCPA (Ni-CCPA) its counterpart Ni-CCP non-aerogel feature are studied proof-of-concept case. Electrochemical measurements show that, relative Ni-CCP, Ni-CCPA exhibits appreciably higher performance toward alkaline oxygen evolution reaction (OER). Both experimental results theoretical simulations unravel improved OER arises from accelerated OH- diffusion within architecture enhanced concentration near highly exposed at high-curvature surfaces localized electric fields. Importantly, evidenced by Cu-CCPA Zn-CCPA examples, such promisingly applied targeted various catalytic reactions beyond.

Language: Английский

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Phase‐Controlled Pd─S Nanosheet Aerogels for Electrocatalytic Upgrading of Waste Plastics

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 23, 2025

Abstract Phase engineering of metal sulfides offers a promising strategy to enhance the catalytic performance by adjusting their atomic arrangement and electronic structure. However, achieving continuous phase‐controlled elucidating structure‐performance relationship remains significant challenge. Herein, for first time, novel class palladium‐sulphur nanosheet aerogels (Pd─S NAs) aimed at enhancing electrocatalytic waste polymer‐derived ethylene glycol oxidation reaction (EGOR) is introduced. Remarkably, benefiting from ordered arrangement, Pd 3 S NAs with 4 phase deliver superior toward EGOR, surpassing both S‐doped (Pd 9 amorphous 1 NAs. Density functional theory calculations reveal that different vital structural descriptor performance, where structure intrinsic contribution excellent Compared other Pd─S NAs, have regular arrangements, which promote carbon monoxide intermediate ( * CO), cause optimal adsorption CH₂OHCOO key intermediates during facilitate selective EG glycolic acid, lower barrier in potential determining step reaction, thus presenting EGOR performance. This study advances synthesis Pd‐based nanomaterials highlights importance phase‐dependent properties electrocatalysis.

Language: Английский

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Nitrogen-Doped Two-Dimensional Carbon Nanosheets for High-Sulfur-Loading Lithium–Sulfur Batteries via a Lignin-Based High-Internal-Phase Pickering Emulsion Strategy

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 16, 2025

Attributable to sulfur's significant theoretical energy density, its affordability, and environmentally friendly nature, lithium–sulfur batteries (LSBs) are recognized as advanced storage technologies with considerable potential. Nonetheless, the solubility migration of polysulfides within electrolyte substantially hinder their practical implementation. To address this issue, we developed a nitrogen-doped two-dimensional (2D) wavy carbon nanosheet material (NCN) by using Pickering emulsion templating method. Nitrogen doping enhances surface polarity material, promoting penetration providing strong chemical adsorption polysulfides. The distinctive structure lithium-ion transport regulates polysulfide dissolution diffusion throughout electrochemical cycle, resulting in an enhanced performance. Therefore, S@NCN cathode shows discharge specific capacity, reaching 936 mAh g–1 at 1 C. Despite sulfur load 7.2 mg cm–2, achieves capacity 823 g–1. These findings indicate that NCN is high-performance 2D for cathodes, effectively improving stability LSBs showing great potential future applications LSBs.

Language: Английский

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Highly Distorted High-Entropy Alloy Aerogels for High-Efficiency Hydrogen Oxidation Reaction

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

The development of efficient electrocatalysts for alkaline hydrogen oxidation reaction (HOR) is essential anion exchange membrane fuel cells and advancing the economy. Herein, we demonstrated PtRuRhPdIr high-entropy alloy aerogels (HEAAs) with highly distorted structure as HOR realized effective control PtRu-based metallic (MAs) elemental components ranging from two to seven. Specially, HEAAs on carbon (PtRuRhPdIr HEAAs/C) exhibit excellent activity, Pt group metal (PGM)-normalized mass activity (5.75 A mgPGM–1) at 50 mV current density normalized by electrochemical surface area (0.69 mA cm–2), approximately 16.9 4.1 times that commercial Pt/C (0.34 mgPGM–1, 0.17 respectively. mechanism study shows provide abundant unsaturated sites HOR, synergistic effect multiple-active balances adsorption H* *OH, boosting performance.

Language: Английский

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In situ construction of a crystalline/amorphous interface in SnO₂/Bi nanobelts for efficient CO₂ electroreduction

Journal of Materials Chemistry A, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Crystalline/amorphous SnO 2 /Bi nanobelts (C/A-SnO NBs) were prepared via an in situ electrochemical dynamic reconstruction strategy for efficient CO electroreduction.

Language: Английский

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Carbon Nanofiber Host with Directed Gradient Pore Size for Dendrite-Free Lithium Metal Anodes

ACS Applied Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 23, 2025

Language: Английский

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Recent Developments and Prospects on Functional Graphene‐Based Nanocomposites as Potential Sulfur Hosts for Next‐Generation Lithium‐Sulfur Batteries

Energy & environment materials, Journal Year: 2025, Volume and Issue: unknown

Published: May 11, 2025

Lithium‐sulfur batteries have been developing in recent years and appear to offer an alternative existing commercial that can potentially replace them the future. With their exceptional theoretical energy density, lower production costs, affordable environmentally friendly abundant raw materials, lithium‐sulfur shown ability defeat counterparts race for rechargeable devices currently being developed. The display extraordinary features, but they suffer from sulfur's non‐conductivity, shuttle effect results polysulfide dissolution, volumetric sulfur changes during charging, dendrites at anode, resulting a decline capacity short battery life. As result of rigorous innovative engineering designs, developed overcome drawbacks utilize entire potential past decade. This review will pay particular attention porous carbon‐based matrix especially graphene‐based nanocomposites are most commonly used producing cathodes. We provide in‐depth perspective on structural merits graphene detailed mechanism by which interact with sulfur, essential strategies designing high‐performance cathodes batteries. Finally, we discuss significant challenges prospects high density long cycle lives next‐generation electric vehicles.

Language: Английский

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A Self‐Constructed Mg²⁺/K⁺ Co‐Doped Prussian Blue with Superior Cycling Stability Enabled by Enhanced Coulombic Attraction

Advanced Science, Journal Year: 2024, Volume and Issue: 11(42)

Published: Sept. 20, 2024

Abstract Prussian blue (PB) is regarded as a promising cathode for sodium‐ion batteries because of its sustainable precursor elements (e.g., Mn, Fe), easy preparation, and unique framework structure. However, the unstable structure inherent crystal H 2 O restrain practical application. For this purpose, self‐constructed trace Mg 2+ /K + co‐doped PB prepared via sea‐water‐mediated method proposed to address problem. The co‐doping in Na sites permitted by both thermodynamics kinetics factors when synthesized sea water. results reveal that introduced K are immovable lattices can form stronger K‒N Mg‒N Coulombic attraction relieve phase transition element dissolution. Besides, reduce defect contents. As result, water exhibits an extremely long cycle life (80.1% retention after 2400 cycles) superior rate capability (90.4% capacity at 20 C relative 0.1 C). To applications, sodium salts recycling strategy greatly production cost. This work provides high‐performance low preparation cost sustainable, large‐scale energy storage.

Language: Английский

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Hollow Urchin-like Ni–Co MOF and RGO Synergistically Functionalizing the Separators for High-Performance Li–S Batteries

Industrial & Engineering Chemistry Research, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 12, 2024

Language: Английский

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Ion-selective gel polymer electrolyte and cathode binder derived from a shared polyether to synergistically mitigate polysulfides shuttling in lithium sulfur batteries

Energy storage materials, Journal Year: 2024, Volume and Issue: unknown, P. 103870 - 103870

Published: Oct. 1, 2024

Language: Английский

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