Stimuli-Responsive Crystalline Smart Materials: From Rational Design and Fabrication to Applications DOI
Yan Dong, Zhifang Wang, Zhenjie Zhang

et al.

Accounts of Chemical Research, Journal Year: 2022, Volume and Issue: 55(7), P. 1047 - 1058

Published: March 16, 2022

Stimuli-responsive smart materials that can undergo reversible chemical/physical changes under external stimuli such as mechanical stress, heat, light, gas, electricity, and pH, are currently attracting increasing attention in the fields of sensors, actuators, optoelectronic devices, information storage, medical applications, so forth. The current mostly concentrate on polymers, carbon materials, crystalline liquids, hydrogels, which have no or low structural order (i.e., responsive groups/moieties disorderly structures), inevitably introducing deficiencies a relatively response speeds, energy transformation inefficiencies, unclear structure-property relationships. Consequently, with well-defined regular molecular arrays offer new opportunity to create novel improved stimuli-responsive performance. Crystalline include framework (e.g., metal-organic frameworks, MOFs; covalent organic COFs) crystals molecules cages), obvious advantages compared amorphous materials. For example, be uniformly installed skeleton crystal form ordered arrays, making transfer between external-stimulus signals sites much faster more efficiently. Besides that, structures facilitate situ characterization their at level by means various techniques high-tech equipment spectra single-crystal/powder X-ray diffraction, thus benefiting investigation understanding mechanism behind behaviors Nevertheless, some unsolved challenges remain for (CSMs), hampering fabrication material systems practical applications. instance, materials' crystallinity increases, processability properties usually decrease, unavoidably hindering application. Moreover, exist micro/nanosized powders, difficult make macroscale. Thus, developing strategies balance establishing macroscale great significance applications.In this Account, we mainly summarize recent research progress achieved our groups, including (i) rational design an in-depth relationship (ii) creating modification improve Overall, Account summarizes state-of-the-art points out existing future development directions field.

Language: Английский

Optoelectronic processes in covalent organic frameworks DOI Open Access
Niklas Keller, Thomas Bein

Chemical Society Reviews, Journal Year: 2020, Volume and Issue: 50(3), P. 1813 - 1845

Published: Dec. 17, 2020

Covalent organic frameworks (COFs) are crystalline porous materials constructed from molecular building blocks using diverse linkage chemistries. Their modular construction system allows not only for tailor-made design but also an immense variety of blocks, opening the door to numerous different functionalities and potential applications. As a consequence, large number that can act as light-harvesters, semiconductors, ligands, binding sites or redox centers have recently been integrated into scaffolds COFs. This unique combination reticular chemistry with control intrinsic properties paves way towards new semiconducting (opto-)electronic applications such sensors, photocatalysts -electrodes, supercapacitor battery materials, solar-harvesting devices light emitting diodes. With developments regarding motif, highly stable still tunable COFs developed even under harsh conditions. Further, stacking modes distances in investigated powerful means optical electrical characteristics these self-assembled frameworks. Advanced understanding optoelectronic processes has enabled their implementation promising real-world review highlights key concepts synthesis electro- photoactive well our frameworks, hence establishing paradigm rational well-defined novel devices.

Language: Английский

Citations

401
Covalent organic frameworks DOI
Ke Tian Tan, Samrat Ghosh, Zhiyong Wang

et al.

Nature Reviews Methods Primers, Journal Year: 2023, Volume and Issue: 3(1)

Published: Jan. 12, 2023

Language: Английский

Citations

401
Regenerable Covalent Organic Frameworks for Photo‐enhanced Uranium Adsorption from Seawater DOI
Wei‐Rong Cui, Fangfang Li,

Rui‐Han Xu

et al.

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 59(40), P. 17684 - 17690

Published: June 25, 2020

Abstract Uranium is a key resource for the development of nuclear industry, and extracting uranium from natural seawater one most promising ways to address shortage resources. Herein, semiconducting covalent organic framework (named NDA‐TN‐AO) with excellent photocatalytic photoelectric activities was synthesized. The effect endowed NDA‐TN‐AO high anti‐biofouling activity by generating biotoxic reactive oxygen species promoting photoelectrons reduce adsorbed U VI insoluble IV , thereby increasing extraction capacity. Owing photoinduced effect, adsorption capacity in reaches 6.07 mg g −1 which 1.33 times that dark. enhanced material seawater.

Language: Английский

Citations

353
Amidoxime-based materials for uranium recovery and removal DOI
Ning Tang, Jie Liang, Cheng‐Gang Niu

et al.

Journal of Materials Chemistry A, Journal Year: 2020, Volume and Issue: 8(16), P. 7588 - 7625

Published: Jan. 1, 2020

This review provides a comprehensive overview of amidoxime-based materials for uranium recovery and removal from the perspectives synthesis, characterizations, types, influence factors, binding mechanisms, cost evaluation.

Language: Английский

Citations

343
Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance DOI Creative Commons
Zhongshan Chen, Jingyi Wang, Mengjie Hao

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Feb. 27, 2023

Covalent organic frameworks (COFs) represent an emerging class of photocatalysts. However, their complicated structures lead to indeterminacy about photocatalytic active sites and reaction mechanisms. Herein, we use reticular chemistry construct a family isoreticular crystalline hydrazide-based COF photocatalysts, with the optoelectronic properties local pore characteristics COFs modulated using different linkers. The excited state electronic distribution transport pathways in are probed host experimental methods theoretical calculations at molecular level. One our developed (denoted as COF-4) exhibits remarkable electron utilization efficiency charge transfer properties, achieving record-high uranium extraction performance ~6.84 mg/g/day natural seawater among all techniques reported so far. This study brings new understanding operation COF-based guiding design improved photocatalysts for many applications.

Language: Английский

Citations

292
Fully Conjugated Donor–Acceptor Covalent Organic Frameworks for Photocatalytic Oxidative Amine Coupling and Thioamide Cyclization DOI
Shuai Li, Li Li, Yijun Li

et al.

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(15), P. 8717 - 8726

Published: July 10, 2020

Covalent organic frameworks (COFs) are promising candidates as heterogeneous photocatalysts because of their porosity and tunable light absorption. The photostability charge separation COFs highly important to improve the efficiency photocatalytic transformation. In this work, a fully conjugated donor–acceptor COF is constructed with benzothiadiazole unit, which exhibits high stability enhanced separation. prepared can efficaciously produce superoxide radical anions under air visible light, mediate oxidative amine coupling cyclization thioamide 1,2,4-thiadiazole in moderate yield recyclability (18 examples). This study demonstrates great capacity D–A structure for light-driven synthesis.

Language: Английский

Citations

288
Covalent Organic Polymers and Frameworks for Fluorescence-Based Sensors DOI Creative Commons
Tina Škorjanc, Dinesh Shetty, Matjaž Valant

et al.

ACS Sensors, Journal Year: 2021, Volume and Issue: 6(4), P. 1461 - 1481

Published: April 7, 2021

Following the advancements and diversification in synthetic strategies for porous covalent materials literature, science community started to investigate performance of organic polymers (COPs) frameworks (COFs) applications that require large surface areas interaction with other molecules, chemical stability, insolubility. Sensorics is an area where COPs COFs have demonstrated immense potential achieved high levels sensitivity selectivity on account their tunable structures. In this review, we focus those polymeric systems use fluorescence spectroscopy as a method detection. After briefly reviewing physical basis fluorescence-based sensors, delve into various kinds analytes been explored COFs, namely, heavy metal ions, explosives, biological amines, pH, volatile compounds solvents, iodine, enantiomers, gases, anions. Throughout work, discuss mechanisms involved each sensing application aim quantify potency discussed sensors by providing limits detection quenching constants when available. This review concludes summary surveyed literature raises few concerns should be addressed future development COP COF sensors.

Language: Английский

Citations

288
Functionalized Iron–Nitrogen–Carbon Electrocatalyst Provides a Reversible Electron Transfer Platform for Efficient Uranium Extraction from Seawater DOI
Hui Yang, Xiaolu Liu, Mengjie Hao

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(51)

Published: Oct. 4, 2021

Uranium extraction from seawater provides an opportunity for sustainable fuel supply to nuclear power plants. Herein, adsorption-electrocatalysis strategy is demonstrated efficient uranium using a functionalized iron-nitrogen-carbon (Fe-Nx -C-R) catalyst, comprising N-doped carbon capsules supporting FeNx single-atom sites and surface chelating amidoxime groups (R). The bring hydrophilicity the adsorbent offer surface-specific binding UO22+ capture. site-isolated centres reduce adsorbed UO2+ . Subsequently, through electrochemical reduction of sites, unstable U(V) ions are reoxidized U(VI) in presence Na+ resulting generation solid Na2 O(UO3 ·H2 O)x , which can easily be collected. Fe-Nx -C-R reduced concentration ≈3.5 ppb below 0.5 with calculated capacity ≈1.2 mg g-1 within 24 h. To best knowledge, developed system first use adsorption uranyl electrodeposition .H2 seawater. important discoveries guide technology development

Language: Английский

Citations

285
Vinylene‐Linked Covalent Organic Frameworks (COFs) with Symmetry‐Tuned Polarity and Photocatalytic Activity DOI

Junsong Xu,

Can Yang, Shuai Bi

et al.

Angewandte Chemie International Edition, Journal Year: 2020, Volume and Issue: 59(52), P. 23845 - 23853

Published: Sept. 21, 2020

Abstract The polarity of a semiconducting molecule affects its intrinsic photophysical properties, which can be tuned by varying the molecular geometry. Herein, we developed D 3 h ‐symmetric tricyanomesitylene as new monomer could reticulated into vinylene‐linked covalent organic framework (g‐C 54 N 6 ‐COF) via Knoevenagel condensation with another 2,4,6‐tris(4′‐formyl‐biphenyl‐4‐yl)‐1,3,5‐triazine. Replacing C 2 v 3,5‐dicyano‐2,4,6‐trimethylpyridine gave less‐symmetric COF 52 ‐COF). octupolar conjugated characters g‐C ‐COF were reflected in scarce solvatochromic effects either ground or excited states, and endowed it more promising behavior compared ‐COF, such enhanced light‐harvesting excellent photo‐induced charge generation separation. Along matched energy level, enabled two‐half reactions photocatalytic water splitting an average O evolution rate 51.0 μmol −1 g H 2518.9 . Such values are among highest state‐of‐the‐art photocatalysts.

Language: Английский

Citations

264
Extremely stable amidoxime functionalized covalent organic frameworks for uranium extraction from seawater with high efficiency and selectivity DOI
Gong Cheng,

Anrui Zhang,

Zhiwei Zhao

et al.

Science Bulletin, Journal Year: 2021, Volume and Issue: 66(19), P. 1994 - 2001

Published: May 16, 2021

Language: Английский

Citations

252