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Instruments / Technical Area	Publication Details	Published
I19-Small Molecule Single Crystal Diffraction	A transformation network culminating in a heteroleptic Cd6L6L'2 twisted trigonal prism Dawei Zhang , Tanya K. Ronson , Lin Xu , Jonathan R. Nitschke Journal Of The American Chemical Society DOI: 10.1021/jacs.0c03798 Diamond Proposal Number(s): [11397] Show Abstract ▼ Abstract: Transformations between three-dimensional metallosupramolecular assemblies can enable switching between the different functions of these structures. Here we report a network of such transformations, based upon a subcomponent displacement strategy. The flow through this network is directed by the relative reactivities of different amines, aldehydes, and di(2-pyridyl)ketone. The network provides access to an unprecedented heteroleptic Cd6L6L'2 twisted trigonal prism. The principles underpinning this network thus allow for the design of diverse structural transformations, converting one helicate into another, a helicate into a tetrahedron, a tetrahedron into a different tetrahedron, and a tetrahedron into the new trigonal prismatic structure type. The selective conversion from one host to another also enabled the uptake of a desired guest from a mixture of guests.	May 2020
I19-Small Molecule Single Crystal Diffraction	Improved acid resistance of a metal-organic cage enables cargo release and exchange between hosts Lin Xu , Dawei Zhang , Tanya Ronson , Jonathan Nitschke Angewandte Chemie International Edition DOI: 10.1002/anie.202001059 Diamond Proposal Number(s): [15768] Show Abstract ▼ Abstract: Here we introduce the use of di(2‐pyridyl)ketone in subcomponent self‐assembly. When combined with a flexible triamine and zinc bis(trifluoromethylsulfon)imide, this ketone formed a new Zn 4 L 4 tetrahedron 1 bearing twelve uncoordinated pyridyl units around its metal‐ion vertices. The acid stability of 1 was found to be greater than that of the analogous tetrahedron 2 built from 2‐formylpyridine. Intriguingly, the peripheral presence of additional pyridine rings in 1 resulted in distinct guest binding behavior from that of 2 , affecting guest scope as well as binding affinities. The different stabilities and guest affinities of capsules 1 and 2 enabled the design of systems whereby different cargoes could be moved between cages using acid and base as chemical stimuli.	Feb 2020
I19-Small Molecule Single Crystal Diffraction	Enantiopure [Cs+/Xe⊂Cryptophane]⊂FeII4L4 hierarchical superstructures Dawei Zhang , Tanya K. Ronson , Jake L. Greenfield , Thierry Brotin , Patrick Berthault , Estelle Leonce , Junlong Zhu , Lin Xu , Jonathan R. Nitschke Journal Of The American Chemical Society DOI: 10.1021/jacs.9b02866 Diamond Proposal Number(s): [15768] Show Abstract ▼ Abstract: Hierarchically nested hosts offer new opportunities to control the guest binding of the inner host, functionalize the cavity of the outer host, and investigate communication between different layers. Here we report a self-assembled triazatruxene-based FeII4L4 capsule, which was able to encapsulate a covalent cage, cryptophane-111 (CRY). The resulting cage-in-cage complex was capable of accommodating a cesium cation or xenon atom with altered guest binding behavior compared to the CRY alone. A crystal structure of the Russian doll complex [Cs+⊂CRY]⊂FeII4L4 unambiguously demonstrated the unusual encapsulation of a cation within a capsule bearing a 8+ charge. Moreover, the binding of enantiopure CRY occurred with high enantioselectivity (530-fold) between the two enantiomers of the tetrahedron. This discrimination resulted in stereochemical information transfer from the inner covalent cage to the outer self-assembled capsule, leading to the formation of enantiopure [guest⊂cage]⊂cage complexes. The stereochemistry of the tetrahedron persisted even after displacement of CRY with an achiral guest.	Apr 2019
I19-Small Molecule Single Crystal Diffraction	Selective Anion Extraction and Recovery Using a FeII4L4 Cage Dawei Zhang , Tanya Kimberley Ronson , Jesús Mosquera , Alexandre Martinez , Jonathan R. Nitschke Angewandte Chemie International Edition DOI: 10.1002/anie.201800459 Diamond Proposal Number(s): [15768] Show Abstract ▼ Abstract: Selective anion extraction is useful for the recovery and purification of valuable chemicals, and in the removal of pollutants from the environment. Here we report that FeII4L4 cage 1 is able to extract an equimolar amount of ReO4−, a high-value anion and a nonradioactive surrogate of TcO4−, from water to nitromethane. Importantly, the extraction was efficiently performed even in the presence of 10 other common anions in water, highlighting the high selectivity of 1 for ReO4−. The extracted guest could be released into water as the cage disassembled in ethyl acetate, and then 1 could be recycled by switching the solvent to acetonitrile. The versatile solubility of the cage also enabled complete extraction of ReO4− (as the tetrabutylammonium salt) from an organic phase into water by using the sulfate salt of 1 as the extractant.	Feb 2018

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