Nature Chemistry, Год журнала: 2023, Номер 16(1), С. 114 - 121
Опубликована: Сен. 18, 2023
Язык: Английский
Nature Reviews Methods Primers, Год журнала: 2023, Номер 3(1)
Опубликована: Янв. 12, 2023
Язык: Английский
Процитировано
397
Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(45), С. 23946 - 23974
Опубликована: Март 30, 2021
At its core, reticular chemistry has translated the precision and expertise of organic inorganic synthesis to solid state. While initial excitement over metal-organic frameworks (MOFs) covalent (COFs) was undoubtedly fueled by their unprecedented porosity surface areas, most profound scientific innovation field been elaboration design strategies for extended crystalline solids through strong directional bonds. In this contribution we highlight different classes materials that have developed, how these can be functionalized, complexity introduced into backbones. Finally, show structural control is being from molecular scale crystal morphology shape on nanoscale, all way shaping bulk scale.
Язык: Английский
Процитировано
322
Matter, Год журнала: 2021, Номер 4(7), С. 2230 - 2265
Опубликована: Июль 1, 2021
Язык: Английский
Процитировано
265
Nature Communications, Год журнала: 2023, Номер 14(1)
Опубликована: Май 29, 2023
The strong excitonic effects widely exist in polymer-semiconductors and the large exciton binding energy (Eb) seriously limits their photocatalysis. Herein, density functional theory (DFT) calculations are conducted to assess band alignment charge transfer feature of potential donor-acceptor (D-A) covalent organic frameworks (COFs), using 1,3,5-tris(4-aminophenyl)triazine (TAPT) or 1,3,5-tris(4-aminophenyl)benzene (TAPB) as acceptors tereph-thaldehydes functionalized diverse groups donors. Given discernable D-A interaction strengths pairs, Eb can be systematically regulated with minimum TAPT-OMe. Guided by these results, corresponding COFs synthesized, where TAPT-OMe-COF possesses best activity photocatalytic H2 production trend other is associated that calculated for pairs. In addition, further alkyne cycloaddition imine linkage greatly improves stability resulting TAPT-OMe-alkyne-COF a substantially smaller exhibits ~20 times higher than parent COF.
Язык: Английский
Процитировано
224
Journal of the American Chemical Society, Год журнала: 2022, Номер 144(12), С. 5643 - 5652
Опубликована: Март 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
Язык: Английский
Процитировано
209
Nature Reviews Chemistry, Год журнала: 2022, Номер 6(12), С. 881 - 898
Опубликована: Ноя. 11, 2022
Язык: Английский
Процитировано
200
Journal of the American Chemical Society, Год журнала: 2022, Номер 144(26), С. 11482 - 11498
Опубликована: Июнь 27, 2022
The practical utilization of covalent organic frameworks (COFs) with manipulation at the atomic and molecular scale often demands their assembly on nano-, meso-, macroscale precise control. Consequently, synthetic approaches that establish ability to control nucleation growth COF crystallites self-assembly desired nanomorphologies have drawn substantial attention from researchers. On basis dimensionality morphologies, we can categorize them into zero- (0-D), one- (1-D), two- (2-D), three-dimensional (3-D) nanomorphologies. In this perspective, summarize reported strategies enable nanomorphologies' size, shape, reveal impact dimensionalities in physicochemical properties applications. aim is a synergistic optimization morphological while keeping micro- or mesoporosity, crystallinity, chemical functionalities COFs perspective. A detailed knowledge along way should help us enrich performance variety applications like catalysis, separation, sensing, drug delivery, energy storage, etc. We discussed interlinking between via transmutation dimensionalities. Such could lead variation during transition. Finally, concept constructing superstructures through combination two more has been explored, it bring up opportunities for developing next-generation innovative materials multidisciplinary
Язык: Английский
Процитировано
193
ACS Nano, Год журнала: 2023, Номер 17(3), С. 1879 - 1905
Опубликована: Янв. 30, 2023
Covalent organic frameworks (COFs) are a type of crystalline porous material with specific features and interesting structures, including porosity, large surface area, biocompatibility. These enable COFs to be considered as excellent candidates for applications in various fields. Recently, have been widely demonstrated promising materials biomedical because their physicochemical properties ultrathin structures. In this review, we cover the recent progress COF photodynamic therapy, gene delivery, photothermal drug bioimaging, biosensing, combined therapies. Moreover, critical challenges further perspectives regards future biology-facing also discussed.
Язык: Английский
Процитировано
185
Journal of the American Chemical Society, Год журнала: 2023, Номер 145(11), С. 6057 - 6066
Опубликована: Март 8, 2023
The development of efficient photocatalysts for N2 fixation to produce NH3 under ambient conditions remains a great challenge. Since covalent organic frameworks (COFs) possess predesignable chemical structures, good crystallinity, and high porosity, it is highly significant explore their potential photocatalytic nitrogen conversion. Herein, we report series isostructural porphyrin-based COFs loaded with Au single atoms (COFX-Au, X = 1-5) fixation. porphyrin building blocks act as the docking sites immobilize well light-harvesting antennae. microenvironment catalytic center precisely tuned by controlling functional groups at proximal distal positions units. As result, COF1-Au decorated strong electron-withdrawing exhibits activity toward production rates 333.0 ± 22.4 μmol g-1 h-1 37.0 2.5 mmol gAu-1 h-1, which are 2.8- 171-fold higher than that COF4-Au electron-donating porphyrin-Au molecular catalyst, respectively. could be further increased 427.9 18.7 61.1 2.7 catalysis COF5-Au featuring two different kinds groups. structure-activity relationship analysis reveals introduction facilitates separation transportation photogenerated electrons within entire framework. This work manifests structures optoelectronic properties COF-based can finely through rational predesign level, thus leading superior evolution.
Язык: Английский
Процитировано
172
Advanced Materials, Год журнала: 2022, Номер 34(16)
Опубликована: Фев. 16, 2022
Microsized silicon particles are desirable Si anodes because of their low price and abundant sources. However, it is challenging to achieve stable electrochemical performances using a traditional microsized anode due the poor electrical conductivity, serious volume expansion, unstable solid electrolyte interface. Herein, composite designed synthesized by constructing unique polymer, poly(hexaazatrinaphthalene) (PHATN), at Si/C surface (PCSi). The Li+ transport mechanism PCSi elucidated in situ characterization theoretical simulation. During lithiation anode, CN groups with high electron density PHATN first coordinate form CNLi bonds on both sides molecule plane. Consequently, original benzene rings become active centers accept lithium Li-rich coatings. molecules expand change molecular configuration during consecutive process, which provides controllable space for expansion particles. exhibits specific capacity 1129.6 mAh g-1 after 500 cycles 1 A , compelling rate performance, maintaining 417.9 16.5 .
Язык: Английский
Процитировано
161