The Effect of Linker‐to‐Metal Energy Transfer on the Photooxidation Performance of an Isostructural Series of Pyrene‐Based Rare‐Earth Metal–Organic Frameworks

Author:

Quezada‐Novoa Victor1,Titi Hatem M.2,Villanueva Francisco Yarur3,Wilson Mark W. B.3,Howarth Ashlee J.1ORCID

Affiliation:

1. Department of Chemistry and Biochemistry Concordia University 7141 Sherbrooke St. W. Montreal Quebec H4B 1R6 Canada

2. Department of Chemistry McGill University 801 Sherbrooke St. W. Montreal Quebec H3A 0B8 Canada

3. Department of Chemistry University of Toronto 80 St. George Street Toronto Ontario M5S 3H6 Canada

Abstract

AbstractThe tetratopic linker, 1,3,6,8‐tetrakis(p‐benzoic acid)pyrene (H4TBAPy) along with rare‐earth (RE) ions is used for the synthesis of 9 isostructures of a metal–organic framework (MOF) with shp topology, named RE‐CU‐10 (RE = Y(III), Gd(III), Tb(III), Dy(III), Ho(III), Er(III), Tm(III), Yb(III), and Lu(III)). The synthesis of each RE‐CU‐10 analogue requires different reaction conditions to achieve phase pure products. Single crystal X‐ray diffraction indicates the presence of a RE9‐cluster in Y‐ to Tm‐CU‐10, while a RE11‐cluster is observed for Yb‐ and Lu‐CU‐10. The photooxidation performance of RE‐CU‐10 analogues is evaluated, observing competition between linker‐to‐metal energy transfer versus the generation of singlet oxygen. The singlet oxygen produced is used to detoxify a mustard gas simulant 2‐chloroethylethyl sulfide, with half‐lives ranging from 4.0 to 5.8 min, some of the fastest reported to date using UV‐irradiation and < 1 mol% catalyst, in methanol under O2 saturation.

Funder

Natural Sciences and Engineering Research Council of Canada

Canada Foundation for Innovation

Publisher

Wiley

Subject

Biomaterials,Biotechnology,General Materials Science,General Chemistry

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