Comprehensive understanding of the roles of water molecules in aqueous Zn-ion batteries: from electrolytes to electrode materials

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(7), P. 3796 - 3839

Published: Jan. 1, 2021

This review summarizes the influences of water molecules during energy storage process from perspectives electrolyte, Zn anode, and cathode materials, including basic theory, modification methods, practical applications.

Language: Английский

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Metalated covalent organic frameworks: from synthetic strategies to diverse applications

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(15), P. 6307 - 6416

Published: Jan. 1, 2022

This review highlights the recent advances of metalated covalent organic frameworks, including synthetic strategies and applications, discusses current challenges future directions.

Language: Английский

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Bottom-Up Synthesis of 8-Connected Three-Dimensional Covalent Organic Frameworks for Highly Efficient Ethylene/Ethane Separation

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(12), P. 5643 - 5652

Published: March 21, 2022

Developing cost-/energy-efficient separation techniques for purifying ethylene from an ethylene/ethane mixture is highly important but very challenging in the industrial process. Herein, using a bottom-up [8 + 2] construction approach, we rationally designed and synthesized three three-dimensional covalent organic frameworks (COFs) with 8-connected bcu networks, which can selectively remove ethane high efficiency. These COF materials, are fabricated by condensation reaction of customer-designed octatopic aldehyde monomer linear diamino linkers, possess crystallinity, good structural robustness, porosity. Attributed to well-organized micro-sized pores nonpolar/inert pore environment, these COFs display adsorption capacity selectivity over ethylene, making them among best ethane-selective adsorbents purification. Their excellent performance validated dynamic breakthrough experiments high-purity (>99.99%) produced through single The surpasses all reported C2H6-selective even some benchmark metal-organic frameworks. This work provides guidance design new value-added gas

Language: Английский

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Functional Regulation and Stability Engineering of Three-Dimensional Covalent Organic Frameworks

Accounts of Chemical Research, Journal Year: 2022, Volume and Issue: 55(14), P. 1912 - 1927

Published: June 27, 2022

ConspectusAs one of the most attractive members in porous materials family, covalent organic frameworks (COFs) have been reported thousands times since their first discovery 2005, covering design, synthesis, and applications. However, an overwhelming majority these COFs are based on two-dimensional (2D) topologies while three-dimensional (3D) numbered fewer than 100 up to date. In fact, baring enhanced specific surface area, interconnected channels, well-exposed functional moieties, highly adjustable structures, 3D often more competitive various application fields like adsorption, separation, chemical sensing, heterogeneous catalysis compared with 2D counterparts. significant crystallization problems poor stabilities, which might be attributed void absence π-π stacking, raised severe limitations over research COFs. To solve problems, elaborate synthesis regulations or moderate functionalization conditions required. More importantly, strategies for enhancing stabilities vital importance further development practical applications.In this Account, we review design principles, approaches, stability regulation methods toward We begin discussion some essential elements construction COF including topologies, interpenetrations, linkages, synthetic methods. After that, focus several COFs, situ approaches (utilizing generated linkages as active sites), bottom-up (embedding moieties from predesigned building blocks), postsynthesis modification (covalent metalation pristine frameworks). At last, highlight durable amplification is important framework application. This target could achieved through not only introduction extra strengthening force, such hydrophobic effects, coulomb repulsion, steric hindrance but also utilization robust enhance material nature.Due high interpenetrated multifarious functionalities, promising demonstrated excellent performance great potential a wide range adsorption catalysis, energy storage, so on. Although has limited by serious restriction, efforts devoted researchers past decade, mass developed control, regulation, enhancement expect practically utilized future advances preparation, materials.

Language: Английский

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Flexible metal–organic frameworks for gas storage and separation

Dalton Transactions, Journal Year: 2022, Volume and Issue: 51(12), P. 4608 - 4618

Published: Jan. 1, 2022

Flexible metal-organic frameworks (MOFs) have gradually attracted much attention due to their reversible structural changes and flexible responses. The basic research of MOFs is study dynamic responses under different external stimuli translate the into applications. Most studies on focus gas storage separation, but lack a systematic summary. Here, we review development MOFs, transformation effects temperature, pressure, guest molecules, applications in separation. Microporous with structures provide unique opportunities for fine-tuning performance because pore shape size can be controlled by stimuli. characteristics breathing phenomena large specific surface area make suitable candidates Finally, application prospects are reported.

Language: Английский

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Construction of Covalent Organic Frameworks via Multicomponent Reactions

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(3), P. 1475 - 1496

Published: Jan. 16, 2023

Multicomponent reactions (MCRs) combine at least three reactants to afford the desired product in a highly atom-economic way and are therefore viewed as efficient one-pot combinatorial synthesis tools allowing one significantly boost molecular complexity diversity. Nowadays, MCRs no longer confined organic have found applications materials chemistry. In particular, can be used prepare covalent frameworks (COFs), which crystalline porous assembled from monomers exhibit broad range of properties applications. This synthetic approach retains advantages small-molecule MCRs, not only strengthening skeletal robustness COFs, but also providing additional driving forces for their crystallization, has been series robust COFs with diverse The present perspective article provides general background discusses types employed COF date, addresses related critical challenges future perspectives inspire MCR-based design new promote further progress this emerging field.

Language: Английский

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3D Covalent Organic Frameworks with Interpenetrated pcb Topology Based on 8-Connected Cubic Nodes

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(13), P. 5728 - 5733

Published: March 23, 2022

The connectivity of building units for 3D covalent organic frameworks (COFs) has long been primarily 4 and 6, which have severely curtailed the structural diversity COFs. Here we demonstrate successful design synthesis a porphyrin based, 8-connected block with cubic configuration, could be further reticulated into an unprecedented interpenetrated pcb topology by imine condensation linear amine monomers. This study presents first case high-connectivity bearing nodes, thus greatly enriching topological possibilities

Language: Английский

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Conjugated Three-Dimensional High-Connected Covalent Organic Frameworks for Lithium–Sulfur Batteries

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(37), P. 17209 - 17218

Published: Sept. 9, 2022

Developing conjugated three-dimensional (3D) covalent organic frameworks (COFs) still remains an extremely difficult task due to the lack of enough 3D building blocks. Herein, condensation between 8-connected pentiptycene-based D2h block (DMOPTP) and 4-connected square-planar linkers affords two COFs (named 3D-scu-COF-1 3D-scu-COF-2). A combination homoaromatic structure former with 2D latter linking units enables π-electron delocalization over whole both COFs, endowing them excellent conductivities 3.2-3.5 × 10-5 S cm-1. In particular, rigid quadrangular prism shape DMOPTP guides formation a twofold interpenetrated scu topology high-connected permanent porosity large Brunauer-Emmett-Teller (BET) surface area 2340 1602 m2 g-1 for 3D-scu-COF-2, respectively, ensuring effective small molecule storage mass transport characteristics. This, in their good charge properties, renders promising sulfur host materials lithium-sulfur batteries (LSBs) high capacities (1035-1155 mA h at 0.2 C, 1 C = 1675 g-1), rate capabilities (713-757 5.0 C), superior cycling stability (71-83% capacity retention 2.0 after 500 cycles), surpassing most LSB cathodes reported thus far.

Language: Английский

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Highly Connected Three-Dimensional Covalent Organic Framework with Flu Topology for High-Performance Li-S Batteries

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(14), P. 8141 - 8149

Published: March 29, 2023

Lithium-sulfur batteries (LSBs) have been considered as a promising candidate for next-generation energy storage devices, which however still suffer from the shuttle effect of intermediate lithium polysulfides (LiPSs). Covalent-organic frameworks (COFs) exhibited great potential sulfur hosts LSBs to solve such problem. Herein, pentiptycene-based D2h symmetrical octatopic polyaldehyde, 6,13-dimethoxy-2,3,9,10,18,19,24,25-octa(4'-formylphenyl)pentiptycene (DMOPTP), was prepared and utilized building block toward preparing COFs. Condensation DMOPTP with 4-connected tetrakis(4-aminophenyl)methane affords an expanded [8 + 4] connected network 3D-flu-COF, flu topology. The non-interpenetrated nature topology endows 3D-flu-COF high Brunauer-Emmett-Teller surface area 2860 m2 g-1, large octahedral cavities, cross-linked tunnels in framework, enabling loading capacity (∼70 wt %), strong LiPS adsorption capability, facile ion diffusion. Remarkably, when used host LSBs, delivers 1249 mA h g-1 at 0.2 C (1.0 = 1675 g-1), outstanding rate capability (764 5.0 C), excellent stability, representing one best results among thus far reported COF-based materials being competitive state-of-the-art inorganic materials.

Language: Английский

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Three-Dimensional Covalent Organic Frameworks with she Topology

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(40), P. 18511 - 18517

Published: Sept. 28, 2022

Reticular chemistry allows the control of crystalline frameworks at atomic precision according to predesigned topological structures. However, only a limited number structures three-dimensional (3D) covalent organic (COFs) have been established. In this work, we developed series 3D COFs with an unprecedented she topology, which were constructed D3d- and D4h-symmetric building blocks. The resulting crystallize in space group Im3̅m, each D3d unit connects six D4h units form noninterpenetrated network uniform pore size 2.0 nm. addition, these exhibited high crystallinity, excellent porosity, good chemical thermal stability. structures, composition, physicochemical properties networks unambiguously characterized. Notably, inbuilt porphyrin render as efficient catalysts for photoredox C-C bond forming photocatalytic carbon dioxide reduction reactions. Thus, work constitutes new approach construction she-net also enhances structural diversity complexity COFs.

Language: Английский

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