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Controlling pore size and pore functionality in sp(2)-conjugated microporous materials by precursor chemistry and salt templating

  • The synthesis of sp(2)-conjugated, heteroatom-rich, "carbonaceous" materials from economically feasible raw materials and salt templates is reported. Low cost citrazinic acid (2,6-dihydroxy-4-pyridinecarboxylic acid) and melamine are used as components to form a microporous, amorphous framework, where edges of the covalent frameworks are tightly terminated with nitrogen and oxygen moieties. ZnCl2 as the porogen stabilizes structural microporosity as well as nitrogen and oxygen heteroatoms up to comparably high condensation temperatures of 750 and 950 degrees C. The specific surface area up to 1265 m(2) g(-1) is mainly caused by micropores and typical of heteroatom-rich carbon materials with such structural porosity. The unusually high heteroatom content reveals that the edges and pores of the covalent structures are tightly lined with heteroatoms, while C-C or C-H bonds are expected to have a minor contribution as compared to typical carbon materials without or with minor content of heteroatoms. Adsorption of water vapor and carbonThe synthesis of sp(2)-conjugated, heteroatom-rich, "carbonaceous" materials from economically feasible raw materials and salt templates is reported. Low cost citrazinic acid (2,6-dihydroxy-4-pyridinecarboxylic acid) and melamine are used as components to form a microporous, amorphous framework, where edges of the covalent frameworks are tightly terminated with nitrogen and oxygen moieties. ZnCl2 as the porogen stabilizes structural microporosity as well as nitrogen and oxygen heteroatoms up to comparably high condensation temperatures of 750 and 950 degrees C. The specific surface area up to 1265 m(2) g(-1) is mainly caused by micropores and typical of heteroatom-rich carbon materials with such structural porosity. The unusually high heteroatom content reveals that the edges and pores of the covalent structures are tightly lined with heteroatoms, while C-C or C-H bonds are expected to have a minor contribution as compared to typical carbon materials without or with minor content of heteroatoms. Adsorption of water vapor and carbon dioxide are exemplarily chosen to illustrate the impact of this heteroatom functionalization under salt-templating conditions on the adsorption properties of the materials. 27.10 mmol g(-1) of H2O uptake (at p/p(0) = 0.9) can be achieved, which also proves the very hydrophilic character of the pore walls, while the maximum CO2 uptake (at 273 K) is 5.3 mmol g(-1). At the same time the CO2/N-2 adsorption selectivity at 273 K can reach values of up to 60. All these values are beyond those of ordinary high surface area carbons, also differ from those of N-doped carbons, and are much closer to those of organized framework species, such as C2N.zeige mehrzeige weniger

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Metadaten
Verfasserangaben:Sol YoukGND, Jan P. Hofmann, Bolortuya Badamdorj, Antje Volkel, Markus AntoniettiORCiDGND, Martin OschatzORCiDGND
DOI:https://doi.org/10.1039/d0ta05856d
ISSN:2050-7488
ISSN:2050-7496
Titel des übergeordneten Werks (Englisch):Journal of materials chemistry : A, Materials for energy and sustainability
Verlag:Royal Society of Chemistry
Verlagsort:Cambridge
Publikationstyp:Wissenschaftlicher Artikel
Sprache:Englisch
Datum der Erstveröffentlichung:25.09.2020
Erscheinungsjahr:2020
Datum der Freischaltung:13.01.2023
Band:8
Ausgabe:41
Seitenanzahl:10
Erste Seite:21680
Letzte Seite:21689
Fördernde Institution:Max-Planck Society Max Planck Society Foundation CELLEX; German Chemical; Industry Fund (Fonds der Chemischen Industrie, FCI); Liebig Fellowship
Organisationseinheiten:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie
DDC-Klassifikation:5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften
Peer Review:Referiert
Publikationsweg:Open Access / Hybrid Open-Access
Lizenz (Deutsch):License LogoCreative Commons - Namensnennung, 3.0 Deutschland
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