ORCID Profile
0000-0001-8797-8666
Current Organisations
Politecnico di Torino
,
University of Adelaide
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Publisher: American Association for the Advancement of Science (AAAS)
Date: 17-07-2020
Abstract: Hydrocarbon distillation is a widespread and energy-intensive process. Membranes might offer an alternative approach, but few can survive immersion in organic solvents nor are they able to extract relatively small molecules. Thompson et al. developed a series of polymers of intrinsic microporosity that they used for membrane-based separations of organic compounds in an organic solvent (see the Perspective by Brennecke and Freeman). The new membrane has a molecular weight cutoff of 253 daltons, far lower than existing ones closer to 600 daltons. The polymers were used to separate light shale crude oil and succeeded in fractionation of molecular weights of about 170 daltons. Science this issue p. 310 see also p. 254
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8MH01611A
Abstract: MOFs have demonstrated outstanding properties for the protection and controlled release of different bio-entities, from proteins to living cells.
Publisher: American Chemical Society (ACS)
Date: 20-05-2021
DOI: 10.26434/CHEMRXIV.14604294
Abstract: The use of unsymmetrical components in metallo-supramolecular chemistry allows for low-symmetry architectures with anisotropic cavities toward guest-binding with high specificity and affinity. Unsymmetrical ditopic ligands mixed with Pd(II) have the potential to self-assemble into reduced symmetry Pd sub /sub L sub /sub metallo-architectures. Mixtures of isomers can form, however, resulting in potentially undesirable heterogeneity within a system. Therefore it is paramount to be able to design components that preferentially form a single isomer. Previous data suggested that computational methods could predict with reasonable accuracy whether unsymmetrical ligands would preferentially self-assemble into a single isomer under constraints of geometrical mismatch. We successfully apply a collaborative computational and experimental workflow to mitigate costly trial-and-error synthetic approaches. Our low-cost computational workflow rapidly constructs new unsymmetrical ligands (and Pd sub /sub L sub /sub cage isomers) and ranks their likelihood for forming i cis /i -Pd sub /sub L sub /sub assemblies. From this narrowed search space, we successfully synthesised four new low-symmetry, i cis /i -Pd sub /sub L sub /sub cages, with cavities of different shapes and sizes.
Publisher: American Chemical Society (ACS)
Date: 20-05-2021
DOI: 10.26434/CHEMRXIV.14604294.V1
Abstract: The use of unsymmetrical components in metallo-supramolecular chemistry allows for low-symmetry architectures with anisotropic cavities toward guest-binding with high specificity and affinity. Unsymmetrical ditopic ligands mixed with Pd(II) have the potential to self-assemble into reduced symmetry Pd 2 L 4 metallo-architectures. Mixtures of isomers can form, however, resulting in potentially undesirable heterogeneity within a system. Therefore it is paramount to be able to design components that preferentially form a single isomer. Previous data suggested that computational methods could predict with reasonable accuracy whether unsymmetrical ligands would preferentially self-assemble into a single isomer under constraints of geometrical mismatch. We successfully apply a collaborative computational and experimental workflow to mitigate costly trial-and-error synthetic approaches. Our low-cost computational workflow rapidly constructs new unsymmetrical ligands (and Pd 2 L 4 cage isomers) and ranks their likelihood for forming cis -Pd 2 L 4 assemblies. From this narrowed search space, we successfully synthesised four new low-symmetry, cis -Pd 2 L 4 cages, with cavities of different shapes and sizes.
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C5DT05023E
Abstract: Mixed-ligand syntheses and post-synthetic metal exchange performed on the Mn 3 L 3 structure type results in site-specific manipulations to the framework structure.
Publisher: Wiley
Date: 18-09-2021
Abstract: The dispersion of particulate porous solids in size‐excluded liquids has emerged as a method to create Type III porous liquids, mostly using insoluble microporous materials such as metal–organic frameworks and zeolites. Here, the first ex les of Type III porous liquids based on porous organic cages (POCs) are presented. By exploiting the solution processability of the POCs, racemic and quasiracemic cage microparticles are formed by chiral recognition. Dispersion of these porous microparticles in a range of size‐excluded liquids, including oils and ionic liquids, forms stable POC‐based Type III porous liquids. The flexible pairing between the solid POC particles and a carrier liquid allows the formation of a range of compositions, pore sizes, and other physicochemical properties to suit different applications and operating conditions. For ex le, it is shown that porous liquids with relatively low viscosities or high thermal stability can be produced. A 12.5 wt% Type III porous liquid comprising racemic POC microparticles and an ionic liquid, [BPy][NTf 2 ], shows a CO 2 working capacity (104.30 µmol g L −1 ) that is significantly higher than the neat ionic liquid (37.27 µmol g L −1 ) between 25 and 100 °C. This liquid is colloidally stable and can be recycled at least ten times without loss of CO 2 capacity.
Publisher: MDPI AG
Date: 05-05-2022
DOI: 10.3390/MET12050797
Abstract: The steelmaking process is an energy-intensive multi-stage process, and the step involving the conversion of molten iron to steel, commonly performed in a basic oxygen furnace (BOF), makes an important contribution to greenhouse gas generation. The effective utilization of energy is one of the major challenges in the process, as minor variations of operational parameters can have significant negative effects on the converter in terms of CO2 emissions. A recent study published by the same authors analyzed the BOF process by developing a general mass and energy balance model. The present study utilizes these models to quantify the contribution of global warming potential (GWP) from the BOF and analyses its sensitivity with the parameters such as hot metal composition, the temperature of hot metal, tapping temperature, scrap quantity, and levels of post-combustion. The term GWP in this study refers to the quantified CO2 values obtained by summing up the carbon dioxide associated with the production of CaO associated with the mass of flux and carbon dioxide generated from the off-gas (considering C in hot metal is completely oxidized to CO2). The results from the analysis indicates that for a tapping temperature increase from 1650 °C to 1683 °C, the percentage change in the global warming potential (GWP) was found to be approximately 1%. The study identified that increasing the scrap percentage in the feed would be the most effective approach to effectively utilizing chemical energy from the process and reduce CO2 emissions. However, increasing scrap above 30% of the total feed is likely to raise issues around: (a) the presence of residual elements in scrap affecting the quality of liquid steel, (b) the effective utilization of post-combustion heat within the furnace, and (c) the recovery of off-gas heat for scrap preheating (assuming no steam recovery from the off-gas system). If these issues could be addressed at the industrial level, a significant reduction in CO2 emissions from the BOF process could be achieved.
Publisher: American Chemical Society (ACS)
Date: 12-01-2019
DOI: 10.1021/JACS.8B10302
Abstract: Encapsulation of biomacromolecules in metal-organic frameworks (MOFs) can preserve biological functionality in harsh environments. Despite the success of this approach, termed biomimietic mineralization, limited consideration has been given to the chemistry of the MOF coating. Here, we show that enzymes encapsulated within hydrophilic MAF-7 or ZIF-90 retain enzymatic activity upon encapsulation and when exposed to high temperatures, denaturing or proteolytic agents, and organic solvents, whereas hydrophobic ZIF-8 affords inactive catalase and negligible protection to urease.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3CC00072A
Abstract: An imine-derived isopropyl-functionalised POC was synthesised over competitive aminal formation by introducing an additional amine in the assembly process.
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/C9SC05534G
Abstract: Steric and geometric constraints were used to design unsymmetrical ditopic ligands that form single Pd 2 L 4 cage isomers with high fidelity.
Publisher: Wiley
Date: 17-08-2022
Abstract: As hydrogen bonded frameworks are held together by relatively weak interactions, they often form several different frameworks under slightly different synthesis conditions and respond dynamically to stimuli such as heat and vacuum. However, these dynamic restructuring processes are often poorly understood. In this work, three isoreticular hydrogen bonded organic frameworks assembled through charge‐assisted amidinium⋅⋅⋅carboxylate hydrogen bonds ( 1 C/C , 1 Si/C and 1 Si/Si ) are studied. Three distinct phases for 1 C/C and four for 1 Si/C and 1 Si/Si are fully structurally characterized. The transitions between these phases involve extreme yet recoverable molecular‐level framework reorganization. It is demonstrated that these transformations are related to water content and can be controlled by humidity, and that the non‐porous anhydrous phase of 1 C/C shows reversible water sorption through single crystal to crystal restructuring. This mechanistic insight opens the way for the future use of the inherent dynamism present in hydrogen bonded frameworks.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0FD90034F
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2CC00532H
Abstract: Metal–organic cages are macrocyclic structures that can possess an intrinsic void for application in encapsulation, sensing and catalysis. In this article, we highlight approaches and limitations to their computational design.
Publisher: Wiley
Date: 02-2023
Abstract: We derive design principles for the assembly of rectangular tetramines into Zn 8 L 6 pseudo‐cubic coordination cages. Because of the rectangular, as opposed to square, geometry of the ligand panels, and the possibility of either Δ or Λ handedness of each metal center at the eight corners of the pseudo‐cube, many different cage diastereomers are possible. Each of the six tetra‐aniline subcomponents investigated in this work assembled with zinc(II) and 2‐formylpyridine in acetonitrile into a single Zn 8 L 6 pseudo‐cube diastereomer, however. Each product corresponded to one of four diastereomeric configurations, with T , T h , S 6 or D 3 symmetry. The preferred diastereomer for a given tetra‐aniline subcomponent was shown to be dependent on its aspect ratio and conformational flexibility. Analysis of computationally modeled in idual faces or whole pseudo‐cubes provided insight as to why the observed diastereomers were favored.
Publisher: Wiley
Date: 11-08-2021
Abstract: Unsymmetrical ditopic ligands can self‐assemble into reduced‐symmetry Pd 2 L 4 metallo‐cages with anisotropic cavities, with implications for high specificity and affinity guest‐binding. Mixtures of cage isomers can form, however, resulting in undesirable system heterogeneity. It is paramount to be able to design components that preferentially form a single isomer. Previous data suggested that computational methods could predict with reasonable accuracy whether unsymmetrical ligands would preferentially self‐assemble into single cage isomers under constraints of geometrical mismatch. We successfully apply a collaborative computational and experimental workflow to mitigate costly trial‐and‐error synthetic approaches. Our rapid computational workflow constructs unsymmetrical ligands and their Pd 2 L 4 cage isomers, ranking the likelihood for exclusively forming cis ‐Pd 2 L 4 assemblies. From this narrowed search space, we successfully synthesised four new, low‐symmetry, cis ‐Pd 2 L 4 cages.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8SC00825F
Abstract: The surface charge and chemistry of a protein determines its ability to facilitate biomimetic mineralisation.
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C7SC00201G
Abstract: Charge-assisted hydrogen bonds between a tetratopic receptor and terephthalate anions assemble a switchable supramolecular framework material in water.
Publisher: American Chemical Society (ACS)
Date: 03-05-2019
DOI: 10.26434/CHEMRXIV.8067176.V1
Abstract: While numerous hydrogen bonded organic frameworks (HOFs) have been reported, typically these cannot be prepared predictably or in a modular fashion. In this work, we report a family of nine diamondoid crystalline porous frameworks assembled via hydrogen bonding between poly-amidinium and poly-carboxylate tectons in aqueous media. Importantly, both the cationic and anionic components can be varied and additional functionality can be incorporated into the frameworks, which show good stability including to prolonged heating in DMSO or water.
Publisher: The Royal Society
Date: 02-2023
DOI: 10.1098/RSOS.220813
Abstract: Porous molecular materials are constructed from molecules that assemble in the solid-state such that there are cavities or an interconnected pore network. It is challenging to control the assembly of these systems, as the interactions between the molecules are generally weak, and subtle changes in the molecular structure can lead to vastly different intermolecular interactions and subsequently different crystal packing arrangements. Similarly, the use of different solvents for crystallization, or the introduction of solvent vapour, can result in different polymorphs and pore networks being formed. It is difficult to uniquely describe the pore networks formed, and thus we analyse 1033 crystal structures of porous molecular systems to determine the underlying topology of their void spaces and potential guest diffusion networks. Material-agnostic topology definitions are applied. We use the underlying topological nets to examine whether it is possible to apply isoreticular design principles to porous molecular materials. Overall, our automatic analysis of a large dataset gives a general insight into the relationships between molecular topologies and the topological nets of their pore network. We show that while porous molecular systems tend to pack similarly to non-porous molecules, the topologies of their pore distributions resemble those of more prominent porous materials, such as metal–organic frameworks and covalent organic frameworks.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3SC03991A
Publisher: AIP Publishing
Date: 06-2021
DOI: 10.1063/5.0049708
Abstract: Computational software workflows are emerging as all-in-one solutions to speed up the discovery of new materials. Many computational approaches require the generation of realistic structural models for property prediction and candidate screening. However, molecular and supramolecular materials represent classes of materials with many potential applications for which there is no go-to database of existing structures or general protocol for generating structures. Here, we report a new version of the supramolecular toolkit, stk, an open-source, extendable, and modular Python framework for general structure generation of (supra)molecular structures. Our construction approach works on arbitrary building blocks and topologies and minimizes the input required from the user, making stk user-friendly and applicable to many material classes. This version of stk includes metal-containing structures and rotaxanes as well as general implementation and interface improvements. Additionally, this version includes built-in tools for exploring chemical space with an evolutionary algorithm and tools for database generation and visualization. The latest version of stk is freely available at ukasturcani/stk.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2SC03856K
Abstract: Cuboctahedral [Pd 12 L 24 ] 24+ cages based on low-symmetry ligands can potentially form a vast number of isomers, but the self-assembly process was found to be highly selective.
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7DT04595F
Abstract: The strained complexes cis -β-[Ru(phen′)(bb 7 )] 2+ isomerise to the corresponding cis -α isomers, with cis -α-[Ru(Me 4 phen)(bb 7 )] 2+ showing good antibacterial activity.
Publisher: Wiley
Date: 02-2023
Abstract: We derive design principles for the assembly of rectangular tetramines into Zn 8 L 6 pseudo‐cubic coordination cages. Because of the rectangular, as opposed to square, geometry of the ligand panels, and the possibility of either Δ or Λ handedness of each metal center at the eight corners of the pseudo‐cube, many different cage diastereomers are possible. Each of the six tetra‐aniline subcomponents investigated in this work assembled with zinc(II) and 2‐formylpyridine in acetonitrile into a single Zn 8 L 6 pseudo‐cube diastereomer, however. Each product corresponded to one of four diastereomeric configurations, with T , T h , S 6 or D 3 symmetry. The preferred diastereomer for a given tetra‐aniline subcomponent was shown to be dependent on its aspect ratio and conformational flexibility. Analysis of computationally modeled in idual faces or whole pseudo‐cubes provided insight as to why the observed diastereomers were favored.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3CC01111A
Abstract: We examined the effect of two different types of linker distribution—random or correlated distribution—on the pore size and shape within single-layers of three multi-component COFs.
Publisher: No publisher found
Date: 2022
DOI: 10.1021/JACS.2C06833
Publisher: American Chemical Society (ACS)
Date: 10-05-2021
DOI: 10.26434/CHEMRXIV.14179022
Abstract: Computational software workflows are emerging as all-in-one solutions to speed up the discovery of new materials. / Many computational approaches require the generation of realistic structural models for property prediction and candidate screening. However, molecular and supramolecular materials represent classes of materials with many potential applications for which there is no go-to database of existing structures or general protocol for generating structures. Here, we report a new version of the supramolecular toolkit, i stk /i , an open-source, extendable and modular Python framework for general structure generation of (supra)molecular structures. Our construction approach follows a bottom-up process and minimises the input required from the user, making i stk /i user-friendly and applicable to many material classes. This version of i stk /i includes metal-containing structures and rotaxanes as well as general implementation and interface improvements. Additionally, this version includes built-in tools for exploring chemical space with an evolutionary algorithm and tools for database generation and visualisation. The latest version of i stk /i is freely available at ukasturcani/stk /
Publisher: Wiley
Date: 03-07-2019
Abstract: While numerous hydrogen-bonded organic frameworks (HOFs) have been reported, typically these cannot be prepared predictably or in a modular fashion. In this work, we report a family of nine diamondoid crystalline porous frameworks assembled via hydrogen bonding between poly-amidinium and poly-carboxylate tectons. The frameworks are prepared at room temperature in either water or water/alcohol mixtures. Importantly, both the cationic and anionic components can be varied and additional functionality can be incorporated into the frameworks, which show good stability including to prolonged heating in DMSO or water.
Publisher: American Chemical Society (ACS)
Date: 25-07-2017
Publisher: American Chemical Society (ACS)
Date: 08-2023
DOI: 10.26434/CHEMRXIV-2023-Q0J0L
Abstract: Cages are macrocyclic structures with an intrinsic internal cavity that support applications in separations, sensing and catalysis. These materials can be synthesised via self-assembly of organic or metal-organic building blocks. Their bottom-up synthesis and the ersity in building block chemistry allows for fine-tuning of their shape and properties toward a target property. However, it is not straightforward to predict the outcome of self-assembly, and, thus, the structures that are practically accessible during synthesis. Indeed, such a prediction becomes more difficult as problems related to the flexibility of the building blocks or increased combinatorics lead to a higher level of complexity and increased computational costs. Molecular models, and their coarse-graining into simplified representations, may be very useful to this end. Here, we develop a minimalistic toy model of cage-like molecules to explore the stable space of different cage topologies based on a few fundamental geometric building block parameters. Our results capture, despite the simplifications of the model, known geometrical design rules in synthetic cage molecules and uncover the role of building block coordination number and preorganisation on the stability of cage topologies. This leads to a large-scale and systematic exploration of design principles, generating data that we expect could be analysed through expandable approaches toward the rational design of self-assembled porous architectures.
Publisher: American Chemical Society (ACS)
Date: 13-10-2022
Publisher: American Chemical Society (ACS)
Date: 14-06-2021
DOI: 10.1021/JACS.1C05172
Publisher: American Chemical Society (ACS)
Date: 03-05-2019
DOI: 10.26434/CHEMRXIV.8067176
Abstract: While numerous hydrogen bonded organic frameworks (HOFs) have been reported, typically these cannot be prepared predictably or in a modular fashion. In this work, we report a family of nine diamondoid crystalline porous frameworks assembled via hydrogen bonding between poly-amidinium and poly-carboxylate tectons in aqueous media. Importantly, both the cationic and anionic components can be varied and additional functionality can be incorporated into the frameworks, which show good stability including to prolonged heating in DMSO or water.
Publisher: The Royal Society of Chemistry
Date: 21-07-2020
DOI: 10.1039/9781839160233-00280
Abstract: 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 ex les of the application of artificial intelligence to the fields of porous organic materials, organic electronics, and organic systems with other desired physical properties.
Publisher: American Chemical Society (ACS)
Date: 29-10-2018
Abstract: The ability to align porous metal-organic frameworks (MOFs) on substrate surfaces on a macroscopic scale is a vital step toward integrating MOFs into functional devices. But macroscale surface alignment of MOF crystals has only been demonstrated in a few cases. To accelerate the materials discovery process, we have developed a high-throughput computational screening algorithm to identify MOFs that are likely to undergo macroscale aligned heterepitaxial growth on a substrate. Screening of thousands of MOF structures by this process can be achieved in a few days on a desktop workstation. The algorithm filters MOFs based on surface chemical compatibility, lattice matching with the substrate, and interfacial bonding. Our method uses a simple new computationally efficient measure of the interfacial energy that considers both bond and defect formation at the interface. Furthermore, we show that this novel descriptor is a better predictor of aligned heteroepitaxial growth than other established interface descriptors, by testing our screening algorithm on a s le set of copper MOFs that have been grown heteroepitaxially on a copper hydroxide surface. Application of the screening process to several MOF databases reveals that the top candidates for aligned growth on copper hydroxide comprise mostly MOFs with rectangular lattice symmetry in the plane of the substrate. This result indicates a substrate-directing effect that could be exploited in targeted synthetic strategies. We also identify that MOFs likely to form aligned heterostructures have broad distributions of in-plane pore sizes and anisotropies. Accordingly, this suggests that aligned MOF thin films with a wide range of properties may be experimentally accessible.
Publisher: American Chemical Society (ACS)
Date: 09-03-2021
DOI: 10.26434/CHEMRXIV.14179022.V1
Abstract: Computational software workflows are emerging as all-in-one solutions to speed up the discovery of new materials.Many computational approaches require the generation of realistic structural models for property prediction and candidate screening. However, molecular and supramolecular materials represent classes of materials with many potential applications for which there is no go-to database of existing structures or general protocol for generating structures. Here, we report a new version of the supramolecular toolkit, stk , an open-source, extendable and modular Python framework for general structure generation of (supra)molecular structures. Our construction approach follows a bottom-up process and minimises the input required from the user, making stk user-friendly and applicable to many material classes. This version of stk includes metal-containing structures and rotaxanes as well as general implementation and interface improvements. Additionally, this version includes built-in tools for exploring chemical space with an evolutionary algorithm and tools for database generation and visualisation. The latest version of stk is freely available at ukasturcani/stk
Publisher: Wiley
Date: 11-08-2021
Abstract: Unsymmetrical ditopic ligands can self‐assemble into reduced‐symmetry Pd 2 L 4 metallo‐cages with anisotropic cavities, with implications for high specificity and affinity guest‐binding. Mixtures of cage isomers can form, however, resulting in undesirable system heterogeneity. It is paramount to be able to design components that preferentially form a single isomer. Previous data suggested that computational methods could predict with reasonable accuracy whether unsymmetrical ligands would preferentially self‐assemble into single cage isomers under constraints of geometrical mismatch. We successfully apply a collaborative computational and experimental workflow to mitigate costly trial‐and‐error synthetic approaches. Our rapid computational workflow constructs unsymmetrical ligands and their Pd 2 L 4 cage isomers, ranking the likelihood for exclusively forming cis ‐Pd 2 L 4 assemblies. From this narrowed search space, we successfully synthesised four new, low‐symmetry, cis ‐Pd 2 L 4 cages.
Publisher: American Chemical Society (ACS)
Date: 10-05-2021
DOI: 10.26434/CHEMRXIV.14179022.V2
Abstract: Computational software workflows are emerging as all-in-one solutions to speed up the discovery of new materials.Many computational approaches require the generation of realistic structural models for property prediction and candidate screening. However, molecular and supramolecular materials represent classes of materials with many potential applications for which there is no go-to database of existing structures or general protocol for generating structures. Here, we report a new version of the supramolecular toolkit, stk , an open-source, extendable and modular Python framework for general structure generation of (supra)molecular structures. Our construction approach follows a bottom-up process and minimises the input required from the user, making stk user-friendly and applicable to many material classes. This version of stk includes metal-containing structures and rotaxanes as well as general implementation and interface improvements. Additionally, this version includes built-in tools for exploring chemical space with an evolutionary algorithm and tools for database generation and visualisation. The latest version of stk is freely available at ukasturcani/stk
Publisher: Springer Science and Business Media LLC
Date: 16-10-2023
Location: United Kingdom of Great Britain and Northern Ireland
No related grants have been discovered for Andrew Tarzia.