Academic Journal
Enhanced Catalytic Activity of a Copper(II) Metal–Organic Framework Constructed via Semireversible Single-Crystal-to-Single-Crystal Dehydration
| العنوان: | Enhanced Catalytic Activity of a Copper(II) Metal–Organic Framework Constructed via Semireversible Single-Crystal-to-Single-Crystal Dehydration |
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| المؤلفون: | Siya T. Hulushe, Gareth M. Watkins, Setshaba D. Khanye |
| سنة النشر: | 2024 |
| مصطلحات موضوعية: | Space Science, Chemical Sciences not elsewhere classified, Physical Sciences not elsewhere classified, various analytical techniques, preliminary reaction mechanism, mof chromism achieved, local coordination geometry, coordinatively unsaturated square, good turnover number, heterogeneous catalytic performances, kgd , 2 ″, 2 ′, took 1 week, 6 )- connected, 2 +, enhanced catalytic activity, 4 –, two anhydrous phases, crystal dehydration herein, within 4 h, 2 , 3 , , catalytic activity, via <, turnover frequency, step dehydration, anhydrous counterparts, (< b |
| الوصف: | Herein, we present a copper(II) metal–organic framework, [Cu 2 (btec)(OH 2 ) 4 ]·2H 2 O ( 1 ) [(btec) 4– = 1,2,4,5-benzenetetracarboxylate], that undergoes single-crystal-to-single-crystal transformations into two anhydrous phases 2′ and 2″ with the chemical formula [Cu 2 (btec)] , triggered by two-step dehydration at 403 and 433 K, respectively. After immersion in water for 3 days at room temperature, 2′ transformed into [Cu 2 (btec)(OH 2 )] ( 3 ), while both 2′ and 2″ took 1 week to revert to 1 . Dynamic vapor sorption studies validated water-induced reversible structural transformations at 70% relative humidity (RH). According to single-crystal X-ray diffraction (SC-XRD), the local coordination geometry of the Cu 2+ ion in 2 ′ changed from a saturated octahedron to a coordinatively unsaturated square-based pyramid in 3 , manifested by changes in color and dimensionality. From a topological point of view, all of the scaffolds show a binodal (3,6)-connected kgd topology with the point symbol {4 3 } 2 {4 6 }. In addition, the materials were thoroughly characterized using routine spectroscopic data and various analytical techniques. The catalytic activity of the microporous materials in the liquid-phase oxidation of styrene in acetonitrile, using 30% (wt) H 2 O 2 as the oxidant, was investigated. The excellent performance of the monohydrous phase 3 was shown to be superior to the pristine framework and the anhydrous counterparts, as evidenced by a good turnover number (TON) and turnover frequency (TOF) = 82.6 and 21.0 h –1 , respectively. Within 4 h, the substrates were catalytically oxidized to the desired products with up to 67% conversion and 100% benzaldehyde selectivity. It is worth noting that the accessible active metal sites and higher surface area enhanced the catalytic properties of 3 . Furthermore, the maintenance of catalytic efficiency over five cycles and reusability are illustrated and discussed in terms of the structural differences of the microporous frameworks. Thus, a preliminary reaction ... |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | unknown |
| Relation: | https://figshare.com/articles/journal_contribution/Enhanced_Catalytic_Activity_of_a_Copper_II_Metal_Organic_Framework_Constructed_i_via_i_Semireversible_Single-Crystal-to-Single-Crystal_Dehydration/25199929 |
| DOI: | 10.1021/acsomega.3c05999.s001 |
| الاتاحة: | https://doi.org/10.1021/acsomega.3c05999.s001 https://figshare.com/articles/journal_contribution/Enhanced_Catalytic_Activity_of_a_Copper_II_Metal_Organic_Framework_Constructed_i_via_i_Semireversible_Single-Crystal-to-Single-Crystal_Dehydration/25199929 |
| Rights: | CC BY-NC 4.0 |
| رقم الانضمام: | edsbas.258291B7 |
| قاعدة البيانات: | BASE |
| DOI: | 10.1021/acsomega.3c05999.s001 |
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