Carbonization of covalent triazine-based frameworks <i>via</i> ionic liquid induction

Jia, Jiangtao; Chen, Zhijie; Belmabkhout, Youssef; Adil, Karim; Bhatt, Prashant M.; Solovyeva, Vera; Shekhah, Osama; Eddaoudi, Mohamed

doi:10.1039/c8ta05583a

Cited by 15 publications

(10 citation statements)

References 44 publications

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“…3A and table S5, the C/N ratio of the CTFs-1 increases notably as a function of increasing synthesis temperature. This observation confirms a reduction in the nitrogen content with an increase in the synthesis temperature because of the partial carbonization of the framework (40,53). Similar to the CTF-1-400 material, the XPS characterization of the samples synthesized at higher temperatures displays the existence of four different types of nitrogen functionalities including still pyridinic nitrogen in the triazine rings (398.4 eV), as well as pyrrolic (400 eV), quaternary (401 eV), and oxidized N-O (404 eV) species (Fig.…”

Section: Mechanistic Proposal For the Oxidative Process Over Ctfs-1supporting

confidence: 72%

Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation

et al. 2020

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Oxygen activation is a critical step in ubiquitous heterogeneous oxidative processes, most prominently in catalysis, electrolysis, and pharmaceutical applications. We present here our findings on metal-free O2 activation on covalent triazine frameworks (CTFs) as an important class of N-rich materials. The O2 activation process was studied for the formation of aldehydes, ketones and imines. A detailed mechanistic study of O2 activation and the role of nitrogen heteroatoms were comprehensively investigated. The electron paramagnetic resonance (EPR) and control experiments provide strong evidence for the reaction mechanism proving the applicability of the CTFs to activate oxygen into superoxide species. This report highlights the importance of a self-templating procedure to introduce N functionalities for the development of metal-free catalytic materials. The presented findings reveal an important step toward the use of CTFs as inexpensive and high-performance alternatives to metal-based materials not only for catalysis but also for biorelated applications dealing with O2 activation.

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Section: Mechanistic Proposal For the Oxidative Process Over Ctfs-1supporting

confidence: 72%

Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation

et al. 2020

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“…MeO -CTF600 was prepared under ionothermal conditions using molten ZnCl 2 , acting both as a Lewis acid cyclotrimerization catalyst and as a reaction medium. Among various recipes of CTF preparation, the ZnCl 2 -mediated ionothermal route is most widely adopted as it results in CTFs with superior textural and functional properties with great tailorability derived via modulation of the ZnCl 2 /monomer ratio and the synthesis temperature. − Recent reports have described that a higher molar ratio (≥10 equiv) of ZnCl 2 resulted in materials with rich structural and porous properties, which are most desirable for the high-capacity capture of small gases. ,− As per the available literature guidelines, in the present study, we have chosen a 10:1 molar ratio of ZnCl 2 to L OMe , and the cyclotrimerization reactions were performed for 48 h at a temperature of 600 °C. The resulted MeO -CTF600 material is completely insoluble in water and any organic solvents, including dilute acids and bases, indicating the formation of networks with excellent physicochemical stability, mandatory for any realistic applications.…”

Section: Resultsmentioning

confidence: 99%

Soft Self-Templating Approach-Derived Covalent Triazine Framework with Bimodal Nanoporosity for Efficient Radioactive Iodine Capture for Safe Nuclear Energy

Das

Sarkar

Patra

et al. 2022

ACS Appl. Nano Mater.

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To achieve a superior removal efficiency of iodine from different phases relevant to radioactive iodine emission (129I/131I) for safe nuclear energy, optimized porous architectures with high surface area and large pore volume featuring appropriate pore size/shape and distribution along with a suitable chemical environment are sought. Herein, we report a soft self-templating synthesis strategy utilizing a low-cost and easily accessible 2,5-dimethoxy terephthalonitrile (L OMe ) monomer to prepare a nitrogen/oxygen codoped nanoporous covalent triazine framework ( MeO -CTF600) possessing an extremely high specific surface area of 2731 m2 g–1 and a record pore volume of 3.33 cm3 g–1. Interestingly, this framework shows extensive bimodal nanoporosity ranging from the micropore (1–2 nm) to narrow mesopore (2–10 nm) region, necessary to achieve superior iodine adsorption. MeO -CTF600 exhibits outstanding iodine capture performance from iodine vapor (578 wt %), including aqueous (221 wt %) and organic (849 mg g–1) solutions of iodine, under nuclear-fuel reprocessing conditions (348 K) compared to benchmark materials. In addition, the framework shows extremely fast adsorption kinetics and regenerability, making it a promising adsorbent tackling all sorts of radioiodine contamination toward clean and safe nuclear power sources.

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“…Many of the aforementioned works are related to covalent triazine-based frameworks, the reason being their great potential for practical applications, for example, gas storage, separation, catalysis, and electronic devices, their high chemical and thermal stability, and their relatively easy and cheap synthesis. All these make CTFs stand out as promising materials for testing in a wide range of applications [92,93].…”

Section: Porous Carbon From Cofsmentioning

confidence: 99%

New and Advanced Porous Carbon Materials in Fine Chemical Synthesis. Emerging Precursors of Porous Carbons

et al. 2019

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The efficiency of porous carbons in fine chemical synthesis, among other application fields, has been demonstrated since both the porous structure and chemical surface provide the appropriated chemical environment favoring a great variety of relevant chemical transformations. In recent years, metal organic frameworks (MOFs) and covalent organic frameworks (COFs) have emerged as interesting opportunities in the preparation of porous carbons with improved physico-chemical properties. Direct calcination of MOFs or COFs, in the presence or not of others carbon or heteroatom sources, could be considered an easy and practical approach for the synthesis of highly dispersed heteroatom-doped porous carbons but also new porous carbons in which single atoms of metallic species are present, showing a great development of the porosity; both characteristics of supreme importance for catalytic applications. The goal of this review is to provide an overview of the traditional methodologies for the synthesis of new porous carbon structures together with emerging ones that use MOFs or COFs as carbon precursors. As mentioned below, the catalytic application in fine chemical synthesis of these kinds of materials is at present barely explored, but probably will expand in the near future.

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Carbonization of covalent triazine-based frameworks via ionic liquid induction

Abstract: A series of porous organic polymers (POPs) were synthesized based on the tetrahedral 1,3,5,7-tetracyanoadamantane as the main building block. This synthetic exploration afforded a drastic porosity alteration/enhancement of the unveiled POPs.

Cited by 15 publications

References 44 publications

Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation

Metal-free activation of molecular oxygen by covalent triazine frameworks for selective aerobic oxidation

Soft Self-Templating Approach-Derived Covalent Triazine Framework with Bimodal Nanoporosity for Efficient Radioactive Iodine Capture for Safe Nuclear Energy

New and Advanced Porous Carbon Materials in Fine Chemical Synthesis. Emerging Precursors of Porous Carbons

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