NDLI: Two linkers are better than one: enhancing CO<sub>2</sub> capture and separation with porous covalent triazine-based frameworks from mixed nitrile linkers

Content Provider	Royal Society of Chemistry (RSC)
Author	Dey, Subarna Bhunia, Asamanjoy Buntkowsky, Gerd Janiak, Christoph Breitzke, Hergen Groszewicz, Pedro B.
Copyright Year	2017
Abstract	Covalent triazine-based framework (CTF) materials were synthesized by combining two different nitrile building blocks: the tetranitrile tetrakis(4-cyanophenyl)ethylene (M) was reacted with either terephthalonitrile (M1), tetrafluoroterephthalonitrile (M2), 4,4′-biphenyldicarbonitrile (M3) or 1,3,5-benzenetricarbonitrile (M4) under ionothermal conditions (ZnCl2, 400 °C) to yield mixed-nitrile MM′-CTFs MM1 to MM4. Comparative 1H/13C and 19F/13C CP MAS analyses of MM2(300) (synthesized at 300 °C) suggest that the hydrogenated and fluorinated carbon atoms are in close vicinity (<5 Å) to each other and support the formulation of the MM2(300) sample as a copolymeric CTF. Systematic N2, CO2 and CH4 gas sorption studies were performed up to 1 bar at 273 K and 293 K. The specific BET surface areas of MM1–MM4 were 1800, 1360, 1884 and 1407 m2 g−1, respectively. The CO2 uptake capacity of mixed-nitrile MM1, MM2 and MM4 was higher than the CO2 uptake of the respective individual single-nitrile M- or M′-CTF despite a higher surface area of the M-CTF PCTF-1 (2235 m2 g−1). The synergistic increase in the CO2 uptake of the mixed-nitrile MM′-CTFs is due to the higher CO2-accessible micropore volume Vmicro(CO2) and the higher micropore volume fraction V0.1/Vtot of the MM′-CTFs compared to the M- or M′-CTFs. The surface area of porous materials does not play the most important role in CO2 storage at low pressure but the CO2-accessible micropore volume is the more decisive factor. Further, MM2 shows the second highest (of known CTFs synthesized at 400 °C) CO2 uptake capacity of 4.70 mmol g−1 at 273 K and 1 bar because of its large micropore fraction (82%), which may be due to the release of fluorous decomposition products (‘defluorination carbonization’) during its synthesis. The CO2/N2 adsorption selectivities of mixed-nitrile MM1, MM2 and MM4 CTFs were also higher than those of the single-nitrile component M- or M′-CTFs.
Starting Page	3609
Ending Page	3620
Page Count	12
File Format	HTM / HTML PDF
ISSN	20507488
Volume Number	5
Issue Number	7
Journal	Journal of Materials Chemistry A
DOI	10.1039/c6ta07076k
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	CTF BET Nitrile Ethylene Memory Stick BMW M3 Fluorine-19 nuclear magnetic resonance Magic angle spinning Carbon Sorption Carbonization Adsorption
Content Type	Text
Resource Type	Article
Subject	Chemistry Renewable Energy, Sustainability and the Environment Materials Science

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