Navigating the Expansive Landscapes of Soft Materials: A User Guide for High-Throughput Workflows

Day, Erin C.; Chittari, Supraja S.; Bogen, Matthew P.; Knight, Abigail S.

doi:10.1021/acspolymersau.3c00025

“…Moreover, understanding the compositional differences between the dead and living chains provides new insights into the details of the RAFT polymerization kinetics. As automated systems for polymer synthesis become increasingly accessible for RHP production, the necessity for strategically designing statistical RHP ensembles to achieve target properties is critical. , There are potentially over 300 commodity methacrylate monomers that are available for synthesizing RHP materials . The systematic methodology presented here will become invaluable for designing fit-for-purpose RHPs.…”

Section: Discussionmentioning

confidence: 99%

Mapping Composition Evolution through Synthesis, Purification, and Depolymerization of Random Heteropolymers

Yu,

Liu,

Yin

et al. 2024

J. Am. Chem. Soc.

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Random heteropolymers (RHPs) consisting of three or more comonomers have been routinely used to synthesize functional materials. While increasing the monomer variety diversifies the sidechain chemistry, this substantially expands the sequence space and leads to ensemble-level sequence heterogeneity. Most studies have relied on monomer composition and simulated sequences to design RHPs, but the questions remain unanswered regarding heterogeneities within each RHP ensemble and how closely these simulated sequences reflect the experimental outcomes. Here, we quantitatively mapped out the evolution of monomer compositions in four-monomer-based RHPs throughout a design-synthesis-purification-depolymerization process. By adopting a Jaacks method, we first determined 12 reactivity ratios directly from quaternary methacrylate RAFT copolymerization experiments to account for the influences of competitive monomer addition and the reversible activation/deactivation equilibria. The reliability of in silico analysis was affirmed by a quantitative agreement (<4% difference) between the simulated RHP compositions and the experimental results. Furthermore, we mapped out the conformation distribution within each ensemble in different solvents as a function of monomer chemistry, composition, and segmental characteristics via high-throughput computation based on selfconsistent field theory (SCFT). These comprehensive studies confirmed monomer composition as a viable design parameter to engineer RHP-based functional materials as long as the reactivity ratios are accurately determined and the livingness of RHP synthesis is ensured.

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“…This platform linked key features and properties of polymers, utilizing the compiled database for training, and resulting in reasonable predictions for polymer properties. Such studies contribute more widely to developing research workflows for soft material innovation 39 .…”

Section: Introductionmentioning

confidence: 99%

Efficient Exploration of Highly Conductive Pyrrolidinium-based Ionic Plastic Crystals Using Materials Informatics

Ootahara,

Hatakeyama-Sato,

Thomas

et al. 2024

Preprint

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Ionic plastic crystals (IPCs), which are soft crystals with plasticity and ionic conductivity, are expected to be applied as solid electrolytes in battery applications. Further improvement of ionic conductivity is necessary for practical use as an electrolyte for energy storage devices. Materials Informatics (MI) is a method of incorporating information science in materials development. In this research, MI is being used to develop IPCs with high ionic conductivity. By using informatics science in addition to chemical knowledge, this research can be carried out efficiently and innovatively. The synthesis of eight new compounds resulted in six of them being solid at room temperature, while two of them were in a liquid state, namely ionic liquids. We evaluated the phase transition temperatures and ionic conductivity for each compound. Notably, N-ethyl-N-methylpyrrolidinium trifluoromethyltrifluoroborate ([C2mpyr][CF3BF3]) exhibited a high ionic conductivity of 1.75×10-4 S cm-1 at 25 oC, which is one of the highest values reported among IPCs to date. The combination of an experimental and MI based approach revealed an improved understanding of the relationship between ion size and ionic conductivity for a series of pyrrolidinium-based IPCs, and it is expected that further improvements to this approach will yield greater understanding of structure-property relationships.

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“…Such studies contribute more widely to developing research workflows for soft material innovation. 37 In previous research undertaken at one of our laboratories, new molecular design guidelines were established for SPEs (vide supra) with high lithium-ion conductivity using MI. 38 The largest machine-readable database of Li…”

Section: Introductionmentioning

confidence: 99%

Efficient Exploration of Highly Conductive Pyrrolidinium-based Ionic Plastic Crystals Using Materials Informatics

Ootahara,

Hatakeyama-Sato,

Thomas

et al. 2024

Preprint

0

View full text Add to dashboard Cite

Ionic plastic crystals (IPCs), which are soft crystals with plasticity and ionic conductivity, are expected to be applied as solid electrolytes in battery applications. Further improvement of ionic conductivity is necessary for practical use as an electrolyte for energy storage devices. Materials Informatics (MI) is a method of incorporating information science in materials development. In this research, MI is being used to develop IPCs with high ionic conductivity. By using informatics science in addition to chemical knowledge, this research can be carried out efficiently and innovatively. The synthesis of eight new compounds resulted in six of them being solid at room temperature, while two of them were in a liquid state, namely ionic liquids. We evaluated the phase transition temperatures and ionic conductivity for each compound. Notably, N-ethyl-N-methylpyrrolidinium trifluoromethyltrifluoroborate ([C2mpyr][CF3BF3]) exhibited a high ionic conductivity of 1.75×10-4 S cm-1 at 25 oC, which is one of the highest values reported among IPCs to date. The combination of an experimental and MI based approach revealed an improved understanding of the relationship between ion size and ionic conductivity for a series of pyrrolidinium-based IPCs, and it is expected that further improvements to this approach will yield greater understanding of structure-property relationships.

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Navigating the Expansive Landscapes of Soft Materials: A User Guide for High-Throughput Workflows

Cited by 6 publications

References 297 publications

Mapping Composition Evolution through Synthesis, Purification, and Depolymerization of Random Heteropolymers

Mapping Composition Evolution through Synthesis, Purification, and Depolymerization of Random Heteropolymers

Efficient Exploration of Highly Conductive Pyrrolidinium-based Ionic Plastic Crystals Using Materials Informatics

Efficient Exploration of Highly Conductive Pyrrolidinium-based Ionic Plastic Crystals Using Materials Informatics

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