8 results found
Thompson KA, Mathias R, Kim D, et al., 2020, N-Aryl-linked spirocyclic polymers for membrane separations of complex hydrocarbon mixtures, Sciene, Vol: 369, Pages: 310-315, ISSN: 0036-8075
The fractionation of crude-oil mixtures through distillation is a large-scale, energy-intensive process. Membrane materials can avoid phase changes in such mixtures and thereby reduce the energy intensity of these thermal separations. With this application in mind, we created spirocyclic polymers with N-aryl bonds that demonstrated noninterconnected microporosity in the absence of ladder linkages. The resulting glassy polymer membranes demonstrated nonthermal membrane fractionation of light crude oil through a combination of class- and size-based “sorting” of molecules. We observed an enrichment of molecules lighter than 170 daltons corresponding to a carbon number of 12 or a boiling point less than 200°C in the permeate. Such scalable, selective membranes offer potential for the hybridization of energy-efficient technology with conventional processes such as distillation.
Bennett S, Tarzia A, Zwijnenburg MA, et al., 2020, Chapter 12: Artificial Intelligence Applied to the Prediction of Organic Materials, RSC Theoretical and Computational Chemistry Series, Pages: 280-310
© 2020 The Royal Society of Chemistry. Artificial intelligence is beginning to significantly increase the rate at which new materials are discovered, by influencing almost all aspects of the materials design process, especially structure and property prediction. Embracing more efficient, data-driven approaches has the potential to significantly increase the number of organic materials that can be screened for useful applications. However, there are various challenges, including representing extended materials in a machine-readable format and obtaining sufficient amounts of training data to generate useful predictive models. This chapter discusses some of the key artificial intelligence techniques that have been applied to organic material prediction and discovery and covers examples of the application of artificial intelligence to the fields of porous organic materials, organic electronics, and organic systems with other desired physical properties.
Lewis JEM, Tarzia A, White AJP, et al., 2019, Conformational control of Pd2L4 assemblies with unsymmetrical ligands, Chemical Science, Vol: 11, Pages: 677-683, ISSN: 2041-6520
With increasing interest in the potential utility of metallo-supramolecular architectures for applications as diverse as catalysis and drug delivery, the ability to develop more complex assemblies is keenly sought after. Despite this, symmetrical ligands have been utilised almost exclusively to simplify the self-assembly process as without a significant driving force a mixture of isomeric products will be obtained. Although a small number of unsymmetrical ligands have been shown to serendipitously form well-defined metallo-supramolecular assemblies, a more systematic study could provide generally applicable information to assist in the design of lower symmetry architectures. Pd2L4 cages are a popular class of metallo-supramolecular assembly; research seeking to introduce added complexity into their structure to further their functionality has resulted in a handful of examples of heteroleptic structures, whilst the use of unsymmetrical ligands remains underexplored. Herein we show that it is possible to design unsymmetrical ligands in which either steric or geometric constraints, or both, can be incorporated into ligand frameworks to ensure exclusive formation of single isomers of three-dimensional Pd2L4 metallo-supramolecular assemblies with high fidelity. In this manner it is possible to access Pd2L4 cage architectures of reduced symmetry, a concept that could allow for the controlled spatial segregation of different functionalities within these systems. The introduction of steric directing groups was also seen to have a profound effect on the cage structures, suggesting that simple ligand modifications could be used to engineer structural properties.
Boer SA, Morshedi M, Tarzia A, et al., 2019, Molecular Tectonics: A Node-and-Linker Building Block Approach to a Family of Hydrogen-Bonded Frameworks, CHEMISTRY-A EUROPEAN JOURNAL, Vol: 25, Pages: 10006-10012, ISSN: 0947-6539
Liang W, Xu H, Carraro F, et al., 2019, Enhanced Activity of Enzymes Encapsulated in Hydrophilic Metal-Organic Frameworks, JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, Vol: 141, Pages: 2348-2355, ISSN: 0002-7863
Tarzia A, Takahashi M, Falcaro P, et al., 2018, High-Throughput Screening of Metal Organic Frameworks for Macroscale Heteroepitaxial Alignment, ACS APPLIED MATERIALS & INTERFACES, Vol: 10, Pages: 40938-40950, ISSN: 1944-8244
Maddigan NK, Tarzia A, Huang DM, et al., 2018, Protein surface functionalisation as a general strategy for facilitating biomimetic mineralisation of ZIF-8., Chem Sci, Vol: 9, Pages: 4217-4223, ISSN: 2041-6520
The durability of enzymes in harsh conditions can be enhanced by encapsulation within metal-organic frameworks (MOFs) via a process called biomimetic mineralisation. Herein we show that the surface charge and chemistry of a protein determines its ability to seed MOF growth. We demonstrate that chemical modification of amino acids on the protein surface is an effective method for systematically controlling biomimetic mineralisation by zeolitic imidazolate framework-8 (ZIF-8). Reaction of surface lysine residues with succinic (or acetic) anhydride facilitates biomimetic mineralisation by increasing the surface negative charge, whereas reaction of surface carboxylate moieties with ethylenediamine affords a more positively charged protein and hinders the process. Moreover, computational studies confirm that the surface electrostatic potential of a protein is a good indicator of its ability to induce biomimetic mineralisation. This study highlights the important role played by protein surface chemistry in encapsulation and outlines a general method for facilitating the biomimetic mineralisation of proteins.
Tarzia A, Thornton AW, Doonan CJ, et al., 2017, Molecular Insight into Assembly Mechanisms of Porous Aromatic Frameworks, JOURNAL OF PHYSICAL CHEMISTRY C, Vol: 121, Pages: 16381-16392, ISSN: 1932-7447
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