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

Chemically Stable Guanidinium Covalent Organic Framework for the Efficient Capture of Low-Concentration Iodine at High Temperatures DOI
Zhiyuan Zhang, Xinglong Dong, Jun Yin

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(15), P. 6821 - 6829

Published: April 5, 2022

The capture of radioactive I2 vapor from nuclear waste under industrial operating conditions remains a challenging task, as the practical high temperature (≥150 °C) and low concentration (∼150 ppmv) are unfavorable for adsorption. We report novel guanidinium-based covalent organic framework (COF), termed TGDM, which can efficiently conditions. At 150 °C ppmv I2, TGDM exhibits an uptake ∼30 wt %, is significantly higher than that silver-based adsorbents such Ag@MOR (17 %) currently used in fuel reprocessing industry. Characterization theoretical calculations indicate among multiple types adsorption sites only ionic bond to through strong Coulomb interactions harsh abundant groups account its superior performance compared various benchmark adsorbents. In addition, exceptionally chemical thermal stabilities fully meet requirements (high-temperature, humid, acidic environment) differentiate it other COFs. Furthermore, has excellent recyclability cost, unavailable current These advantages make promising candidate capturing during reprocessing. This strategy incorporating chemically stable guanidine moieties COF would stimulate development new related applications.

Language: Английский

Citations

175
Advanced porous adsorbents for radionuclides elimination DOI
Mengjie Hao, Yanfang Liu,

Weijin Wu

et al.

EnergyChem, Journal Year: 2023, Volume and Issue: 5(4), P. 100101 - 100101

Published: Feb. 14, 2023

Language: Английский

Citations

156
Precise recognition of palladium through interlaminar chelation in a covalent organic framework DOI Creative Commons

Yaoyao Bai,

Long Chen, Linwei He

et al.

Chem, Journal Year: 2022, Volume and Issue: 8(5), P. 1442 - 1459

Published: March 16, 2022

Language: Английский

Citations

91
Redox-Active Covalent Organic Frameworks with Nickel–Bis(dithiolene) Units as Guiding Layers for High-Performance Lithium Metal Batteries DOI
Si‐Wen Ke,

Yaoda Wang,

Jian Su

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(18), P. 8267 - 8277

Published: April 28, 2022

Combining the chemistry of metal-organic frameworks (MOFs) and covalent organic (COFs) can bring new opportunities for design advanced materials with enhanced tunability functionality. Herein, we constructed two COFs based on Ni-bis(dithiolene) units imine bonds, representing a bridge between traditional MOFs COFs. The Ni-bis(dithiolene)tetrabenzaldehyde as 4-connected linker was initially synthesized, which further linked by tetra(aminophenyl)pyrene (TAP) or 3-connected tris(aminophenyl)amine (TAA) linkers into COFs, namely, Ni-TAP Ni-TAA. shows two-dimensional sql network, while TAA is twofold interpenetrated framework an ffc topology. They both exhibit high Brunauer-Emmett-Teller surface area (324 689 m2 g-1 Ni-TAA, respectively), fairly good conductivity (1.57 × 10-6 9.75 10-5 S m-1 chemical stability (a stable pH window 1-14 Ni-TAA). When applied in lithium metal batteries intermediate layer guiding uniform Li electrodeposition, Ni-TAA displayed impressive lithiophilicity Li-ion conductivity, enabling achievement smooth dense deposition clear columnar morphology plating/stripping behaviors utilization, anticipated to pave way upgrade anodes application high-energy-density battery systems.

Language: Английский

Citations

80
Effective Iodine Adsorption by Nitrogen-Rich Nanoporous Covalent Organic Frameworks DOI
Hailian Li, De-Shan Zhang, Ke Cheng

et al.

ACS Applied Nano Materials, Journal Year: 2023, Volume and Issue: 6(2), P. 1295 - 1302

Published: Jan. 11, 2023

With the rapid development of nuclear industry, effective treatment radioactive iodine has currently become an urgent but challenging task. Herein, two covalent organic frameworks (COFs), TFBT-1 and TFBT-2, were successfully synthesized for adsorption. Structure analysis revealed that they are both nanoporous materials with one-dimensional channels derived from packing related two-dimensional frameworks. Iodine adsorption experiments demonstrated COF exhibit performance adsorption, a maximum amount upto 3.15 g g–1 2.60 TFBT-2. The results experimental analyses Fourier-transform infrared spectroscopy, X-ray photoelectron Raman spectroscopy clearly their high is attributed to strong interactions between adsorbed uniformly located abundant nitrogen sites in pores materials, which pre-introduced acylamides situ-generated Schiff base imine groups. present work by introducing nitrogen-rich into adsorbents can be achieved.

Language: Английский

Citations

80
From Supramolecular Organic Cages to Porous Covalent Organic Frameworks for Enhancing Iodine Adsorption Capability by Fully Exposed Nitrogen‐Rich Sites DOI
Ke Cheng, Hailian Li, Jiarui Wang

et al.

Small, Journal Year: 2023, Volume and Issue: 19(34)

Published: May 10, 2023

In order to overcome the limitations of supramolecular organic cages for their incomplete accessibility active sites in solid state and uneasy recyclability liquid solution, herein a nitrogen-rich cage is rationally linked into framework systems four isoreticular covalent frameworks (COFs), that is, Cage-TFB-COF, Cage-NTBA-COF, Cage-TFPB-COF, Cage-TFPT-COF, are successfully synthesized. Structure determination reveals they all high-quality crystalline materials derived from eclipsed packing related two-dimensional frameworks. Since usually have high affinity toward iodine species, adsorption investigations carried out results show them display an enhancement capacities. Especially, Cage-NTBA-COF exhibits capacity 304 wt%, 14-fold higher than sample packed itself. The strong interactions between adsorbed species revealed by spectral analyses. This work demonstrates that, utilizing reticular chemistry strategy extend close-packed porous solids, inherent properties can be greatly exploited targeted applications.

Language: Английский

Citations

71
Topological Isomerism in Three-Dimensional Covalent Organic Frameworks DOI

Yaozu Liu,

Jingwei Li, Jia Lv

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(17), P. 9679 - 9685

Published: April 18, 2023

Although isomerism is a typical and significant phenomenon in organic chemistry, it rarely found covalent framework (COF) materials. Herein, for the first time, we report controllable synthesis of topological isomers three-dimensional COFs via distinctive tetrahedral building unit under different solvents. Based on this strategy, both with dia or qtz net (termed JUC-620 JUC-621) have been obtained, their structures are determined by combining powder X-ray diffraction transmission electron microscopy. Remarkably, these architectures show distinct difference porous features; example, JUC-621 exhibits permanent mesopores (up to ∼23 Å) high surface area (∼2060 m2 g-1), which far surpasses those (pore size ∼12 Å 980 g-1). Furthermore, mesoporous can remove dye molecules efficiently achieves excellent iodine adsorption 6.7 g 2.3 times that microporous (∼2.9 This work thus provides new way constructing COF promotes structural diversity promising applications

Language: Английский

Citations

65
Linking Nitrogen-Rich Organic Cages into Isoreticular Covalent Organic Frameworks for Enhancing Iodine Adsorption Capability DOI
Ke Cheng, Hailian Li, Zuyong Li

et al.

ACS Materials Letters, Journal Year: 2023, Volume and Issue: 5(6), P. 1546 - 1555

Published: April 24, 2023

By linking a nitrogen-rich organic cage with linear connectors, three cage-based isoreticular covalent frameworks, i.e., Cage-IRCOF-1, Cage-IRCOF-2, Cage-IRCOF-3, were successfully designed and synthesized by Schiff-base polycondensation reactions. The structure determination simulations from powder X-ray diffraction measurements indicated that these COFs have high crystallinity derived the packing of covalently linked two-dimensional layer frameworks. As porous materials, iodine capture studies carried out, proving they displayed obvious enhancements in uptake as compared pristine itself. In particular, Cage-IRCOF-1 an adsorption capacity 262 wt %, which is 12 times higher than solid packed Spectral revealed there strong interactions between groups adsorbed species. This work demonstrated discrete cages into reticular crystalline effective adsorbents can be fabricated for targeted applications.

Language: Английский

Citations

64
Engineering the pore environment of antiparallel stacked covalent organic frameworks for capture of iodine pollutants DOI Creative Commons

Yinghui Xie,

Qiuyu Rong,

Fengyi Mao

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 26, 2024

Abstract Radioiodine capture from nuclear fuel waste and contaminated water sources is of enormous environmental importance, but remains technically challenging. Herein, we demonstrate robust covalent organic frameworks (COFs) with antiparallel stacked structures, excellent radiation resistance, high binding affinities toward I 2 , CH 3 I, − under various conditions. A neutral framework (ACOF-1) achieves a affinity through the cooperative functions pyridine-N hydrazine groups stacking layers, resulting in capacity ~2.16 g/g for ~0.74 at 25 °C dynamic adsorption Subsequently, post-synthetic methylation ACOF-1 converted sites to cationic pyridinium moieties, yielding (namely ACOF-1R) enhanced triiodide ion water. ACOF-1R can rapidly decontaminate iodine polluted groundwater drinking levels uptake ~4.46 established column breakthrough tests. The specific moieties make promising adsorbents radioiodine pollutants treatment practical

Language: Английский

Citations

62
Pore Space Partition Synthetic Strategy in Imine-linked Multivariate Covalent Organic Frameworks DOI
Mengjie Hao,

Yinghui Xie,

Ming Lei

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 146(3), P. 1904 - 1913

Published: Dec. 22, 2023

Partitioning the pores of covalent organic frameworks (COFs) is an attractive strategy for introducing microporosity and achieving new functionality, but it technically challenging to achieve. Herein, we report a simple partitioning micropores/mesopores multivariate COFs. Our approach relies on predesign synthesis multicomponent COFs through imine condensation reactions with aldehyde groups anchored in COF pores, followed by inserting additional symmetric building blocks (with C2 or C3 symmetries) as pore partition agents. This allowed tetragonal hexagonal be partitioned into two three smaller micropores, respectively. The synthesized library pore-partitioned was then applied capture iodine pollutants (i.e., I2 CH3I). rich inventory deep exploration relationships between adsorbent composition, architecture, adsorption capacity CH3I under wide-ranging conditions. Notably, one our developed (COF 3-2P) exhibited greatly enhanced dynamic performances compared its parent 3) breakthrough tests, setting benchmark COF-based adsorbents. Results present effective design toward functional tunable environments, functions, properties.

Language: Английский

Citations

53