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Computationally-Inspired Discovery of an Unsymmetrical Porous Organic Cage

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Title: Computationally-Inspired Discovery of an Unsymmetrical Porous Organic Cage
Authors: Berardo, E
Greenaway, R
Turcani, L
Alston, B
Bennison, M
Miklitz, M
Clowes, R
Briggs, M
Cooper, A
Jelfs, K
Item Type: Journal Article
Abstract: A completely unsymmetrical porous organic cage was synthesised from a C2v symmetrical building block that was identified by a computational screen. The cage was formed through a 12-fold imine condensation of a tritopic C2v symmetric trialdehyde with a ditopic C2 symmetric diamine in a [4 + 6] reaction. The cage was rigid and microporous, as predicted by the simulations, with an apparent Brunauer–Emmett–Teller surface area of 578 m2 g−1. The reduced symmetry of the tritopic building block relative to its topicity meant there were 36 possible structural isomers of the cage. Experimental characterisation suggests a single isomer with 12 unique imine environments, but techniques such as NMR could not conclusively identify the isomer. Computational structural and electronic analysis of the possible isomers was used to identify the most likely candidates, and hence to construct a 3-dimensional model of the amorphous solid. The rational design of unsymmetrical cages using building blocks with reduced symmetry offers new possibilities in controlling the degree of crystallinity, porosity, and solubility, of self-assembled materials.
Issue Date: 21-Dec-2018
Date of Acceptance: 17-Nov-2018
URI: http://hdl.handle.net/10044/1/66448
DOI: https://dx.doi.org/10.1039/c8nr06868b
ISSN: 2040-3364
Publisher: Royal Society of Chemistry
Start Page: 22381
End Page: 22388
Journal / Book Title: Nanoscale
Volume: 10
Issue: 47
Copyright Statement: © The Royal Society of Chemistry 2018.
Sponsor/Funder: The Royal Society
Engineering & Physical Science Research Council (EPSRC)
Engineering & Physical Science Research Council (E
Engineering & Physical Science Research Council (EPSRC)
Commission of the European Communities
Funder's Grant Number: UF120469
EP/M017257/1
EP/N004884/1
EP/P005543/1
758370
Keywords: Science & Technology
Physical Sciences
Technology
Chemistry, Multidisciplinary
Nanoscience & Nanotechnology
Materials Science, Multidisciplinary
Physics, Applied
Chemistry
Science & Technology - Other Topics
Materials Science
Physics
NMR CHEMICAL-SHIFTS
MOLECULAR-DYNAMICS
BASIS-SETS
DENSITY FUNCTIONALS
FORCE-FIELD
DESIGN
SHAPE
SELECTIVITY
DIFFUSION
H-1
10 Technology
02 Physical Sciences
03 Chemical Sciences
Publication Status: Published
Embargo Date: 2019-11-20
Online Publication Date: 2018-11-20
Appears in Collections:Chemistry
Faculty of Natural Sciences



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