Constructing Cooperative Interface via Bi‐Functional COF for Facilitating the Sulfur Conversion and Li+ Dynamics DOI
Qi An, Li-Lian Wang,

Genfu Zhao

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(4)

Published: Sept. 1, 2023

Abstract Lithium–sulfur (Li–S) batteries stand out for their high theoretical specific capacity and cost‐effectiveness. However, the practical implementation of Li–S is hindered by issues such as shuttle effect, tardy redox kinetics, dendrite growth. Herein, an appealingly designed covalent organic framework (COF) with bi‐functional active sites cyanide groups polysulfide chains (COF‐CN‐S) developed cooperative functional promoters to simultaneously address dendrites effect issues. Combining in situ techniques calculations, it can be demonstrated that unique chemical architecture COF‐CN‐S capable performing following functions: 1) The delivers significantly enhanced Li + transport capability due abundant ion‐hopping (cyano‐groups); 2) functions a selective ion sieve regulating dynamic behavior anions , thus inhibiting growth; 3) acting mediator, effectively control electrochemical polysulfides enhance conversion kinetics. Based on above advantages, endows excellent performance. This study highlights significance interface modification offers novel insights into rational design materials realm.

Language: Английский

An ultrathin and crack‐free metal‐organic framework film for effective polysulfide inhibition in lithium–sulfur batteries DOI Creative Commons
Cheng Zhou, Chenxu Dong, Weixiao Wang

et al.

Interdisciplinary materials, Journal Year: 2024, Volume and Issue: 3(2), P. 306 - 315

Published: Feb. 5, 2024

Abstract Due to their extensive microporous structure, metal‐organic frameworks (MOFs) find widespread application in constructing modification layers, functioning as ion sieves. However, the layers prepared by existing methods feature gaps between MOFs that are noticeably larger than inherent MOF pore dimensions. Polysulfides and lithium ions unavoidably permeate through these gaps, hindering full exploitation of structural advantages. Herein, an ultrathin (20 nm) crack‐free film is formed on separator atomic layer deposition for first time. Based separator, mechanism different has been verified phase field simulation situ Raman spectroscopy. The results accurately prove particle can relieve shuttle polysulfides, but it does not have effect homogenizing ions. Only with proper size act sieve both polysulfides As a result, under test condition 2 mA cm −2 –2 mAh , overpotential Li/Li symmetric battery only 18 mV after 2500 h. capacity retention rate lithium–sulfur 95.6% 500 cycles 80% 1000 at C.

Language: Английский

Citations

65
Tuning the structure characteristic of the flexible covalent organic framework (COF) meets a high performance for lithium-sulfur batteries DOI

Yunchen Ge,

Jianming Li, Yan Meng

et al.

Nano Energy, Journal Year: 2023, Volume and Issue: 109, P. 108297 - 108297

Published: Feb. 22, 2023

Language: Английский

Citations

54
Enhanced Electron Delocalization within Coherent Nano‐Heterocrystal Ensembles for Optimizing Polysulfide Conversion in High‐Energy‐Density Li‐S Batteries DOI
Zhiqiang Zhao,

Yukun Pan,

Shan Yi

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(13)

Published: Dec. 25, 2023

Abstract Commercialization of high energy density Lithium‐Sulfur (Li‐S) batteries is impeded by challenges such as polysulfide shuttling, sluggish reaction kinetics, and limited Li + transport. Herein, a jigsaw‐inspired catalyst design strategy that involves in situ assembly coherent nano‐heterocrystal ensembles (CNEs) to stabilize high‐activity crystal facets, enhance electron delocalization, reduce associated barriers proposed. On the surface, stabilized facets induce aggregation. Simultaneously, surrounded surface with enhanced activity promote 2 S deposition diffusion, synergistically facilitating continuous efficient sulfur redox. Experimental DFT computations results reveal dual‐component hetero‐facet alters coordination Nb atoms, enabling redistribution 3D orbital electrons at center promoting d‐p hybridization sulfur. The CNE, based on level gradient lattice matching, endows maximum transfer catalysts establishes smooth pathways for ion diffusion. Encouragingly, NbN‐NbC‐based pouch battery delivers Weight 357 Wh kg −1 , thereby demonstrating practical application value CNEs. This work unveils novel paradigm designing high‐performance catalysts, which has potential shape future research electrocatalysts storage applications.

Language: Английский

Citations

53
Latest advances in layered covalent organic frameworks for water and wastewater treatment DOI
Changlei Xia, Sang‐Woo Joo, Akbar Hojjati‐Najafabadi

et al.

Chemosphere, Journal Year: 2023, Volume and Issue: 329, P. 138580 - 138580

Published: April 3, 2023

Language: Английский

Citations

51
Made to Measure Squaramide COF Cathode for Zinc Dual‐Ion Battery with Enriched Storage via Redox Electrolyte DOI Creative Commons
Rinku Kushwaha, Chitvan Jain, Pragalbh Shekhar

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(34)

Published: July 27, 2023

Abstract Aqueous rechargeable batteries are promising grid‐scale energy storage devices because of their affordability, operational safety, and environmental benignity. Among these, Zn‐ion (ZIBs) have unfolded new horizons. Designing superior cathodes for ZIBs is crucial. Covalent organic frameworks (COFs) can be made redox active with a high surface. Here, the first time, chelating COF redox‐active ZnI 2 in ZnSO 4 (aq) electrolyte combined. Including iodide harvests an approximately threefold enhancement capacity from 208 to 690 mAh g −1 at 1.5 A , highest among all COF‐derived ZIBs. Remarkably, charge–discharge curve 1.3 V exhibits very limited dropout voltage super‐flat platform, remarkable 600 5 stable up 6000 cycles, confirming that polyiodide generation sustainable. The COF's dual‐ion (Zn 2+ polyidode) delivers ZIB density. Spectro‐electrochemical measurements coupled X‐ray photoelectron spectroscopy unambiguously unveil existence multiple species, I 3 − IO ions as prominent species. latter gets reduced electrode under applied potential, leaving major species stored on COF. prospect COF‐polyiodide windfall metal‐ion batteries.

Language: Английский

Citations

44
All-solid-state lithium–sulfur batteries through a reaction engineering lens DOI
Jung Tae Kim, Han Su, Yu Lin Zhong

et al.

Nature Chemical Engineering, Journal Year: 2024, Volume and Issue: 1(6), P. 400 - 410

Published: June 25, 2024

Language: Английский

Citations

35
Covalent Organic Frameworks for Photocatalytic Reduction of Carbon Dioxide: A Review DOI
Jinglun Yang, Zihao Chen, Lei Zhang

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(33), P. 21804 - 21835

Published: Aug. 8, 2024

Covalent organic frameworks (COFs) are crystalline networks with extended backbones cross-linked by covalent bonds. Due to the semiconductive properties and variable metal coordinating sites, along rapid development in linkage chemistry, utilization of COFs photocatalytic CO2RR has attracted many scientists' interests. In this Review, we summarize latest research progress on for CO2 reduction. first part, present COF linkages that have been used CO2RR, discuss four mechanisms including as intrinsic photocatalysts, photosensitive motifs metalated semiconductors heterojunction photocatalysts. Then, principles structural designs functional building units stacking mode exchange. Finally, outlook challenges provided. This Review is intended give some guidance design synthesis diverse different linkages, various structures, divergent modes efficient photoreduction CO2.

Language: Английский

Citations

34
Advanced Polymers in Cathodes and Electrolytes for Lithium–Sulfur Batteries: Progress and Prospects DOI
Zihui Song,

Wanyuan Jiang,

Borui Li

et al.

Small, Journal Year: 2024, Volume and Issue: 20(19)

Published: Jan. 28, 2024

Abstract Lithium–sulfur (Li–S) batteries, which store energy through reversible redox reactions with multiple electron transfers, are seen as one of the promising storage systems future due to their outstanding advantages. However, shuttle effect, volume expansion, low conductivity sulfur cathodes, and uncontrollable dendrite phenomenon lithium anodes have hindered further application Li–S batteries. In order solve problems clarify electrochemical reaction mechanism, various types materials, such metal compounds carbon used in Polymers, a class inexpensive, lightweight, electrochemically stable enable construction low‐cost, high‐specific capacity Moreover, polymers can be multifunctionalized by obtaining rich structures molecular design, allowing them applied not only but also binders solid‐state electrolytes optimize performance from perspectives. The most widely areas related polymer applications including cathodes electrolytes, selected for comprehensive overview, relevant mechanisms action different components discussed. Finally, prospects practical batteries presented terms advanced characterization mechanistic analysis.

Language: Английский

Citations

29
The development of catalysts and auxiliaries for the synthesis of covalent organic frameworks DOI
Wei Zhao, Qiang Zhu, Xiaofeng Wu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(14), P. 7531 - 7565

Published: Jan. 1, 2024

Covalent organic frameworks (COFs) have recently seen significant advancements. Large quantities of structurally & functionally oriented COFs with a wide range applications, such as gas adsorption, catalysis, separation, and drug delivery, been explored. Recent achievements in this field are primarily focused on advancing synthetic methodologies, catalysts playing crucial role achieving highly crystalline COF materials, particularly those featuring novel linkages chemistry. A series reviews already published over the last decade, covering fundamentals, synthesis, applications COFs. However, despite pivotal that auxiliaries play forming materials adjusting their properties (

Language: Английский

Citations

25
Functionality Modulation Toward Thianthrene‐based Metal‐Free Electrocatalysts for Water Splitting DOI

Arnab Sadhukhan,

Arun Karmakar, Kalipada Koner

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(18)

Published: Jan. 21, 2024

The development of metal-free bifunctional electrocatalysts for hydrogen and oxygen evolution reactions (HER OER) is significant but rarely demonstrated. Porous organic polymers (POPs) with well-defined electroactive functionalities show superior performance in reaction (HER) (OER). Precise control the active sites' local environment requires careful modulation linkers through judicious selection building units. Here, a systematic strategy introduced modulating functionality to design synthesize series thianthrene-based sp

Language: Английский

Citations

22