Structural, Ionic, and Electronic Properties of Solid-State Phthalimide-Containing Polymers for All-Organic Batteries DOI Creative Commons
Riccardo Alessandri, Cheng-Han Li, Sheila Keating

et al.

JACS Au, Journal Year: 2024, Volume and Issue: 4(6), P. 2300 - 2311

Published: June 7, 2024

Redox-active polymers serving as the active materials in solid-state electrodes offer a promising path toward realizing all-organic batteries. While both cathodic and anodic redox-active are needed, diversity of available is limited. Here, we predict structural, ionic, electronic properties anodic, phthalimide-containing using multiscale approach that combines atomistic molecular dynamics, structure calculations, machine learning surrogate models. Importantly, by combining information from each these scales, able to bridge gap between bottom-up characteristics macroscopic such apparent diffusion coefficients electron transport (Dapp). We investigate impact different polymer backbones two critical factors during battery operation: state charge swelling. Our findings reveal significantly influences packing thermophysical polymers, which, turn, affect ionic transport. A combination molecular-level (such reorganization energy) condensed-phase effective hopping distances) determine predicted ranking capabilities polymers. Dapp for phthalimide-based reference nitroxide radical-based polymer, finding 3 orders magnitude increase (≈10–6 cm2 s–1) with respect reference. This study underscores promise highly capable batteries, due their exceptional capabilities.

Language: Английский

Digitization of flow battery experimental process research and development DOI Open Access
Changyu Chen, Gaole Dai,

Yuechen Gao

et al.

Energy Materials, Journal Year: 2024, Volume and Issue: 4(2)

Published: March 14, 2024

Rising atmospheric CO2 concentrations urgently call for advanced sustainable energy storage solutions, underlining the pivotal role of renewable energies. This perspective delves into capabilities redox flow batteries as potential grid contenders, highlighting their benefits over traditional lithium-ion batteries. While all-vanadium have established themselves, concerns about vanadium availability steered interest toward Organic Flow Batteries. The multifaceted nature organic materials calls an integrated approach combining artificial intelligence, robotics, and material science to enhance battery efficacy. union intelligence robotics expedites research development trajectory, encompassing everything from data assimilation continuous refinement. With burgeoning metaverse, a groundbreaking avenue collaborative emerges, potentially revolutionizing catalyzing progression towards resolutions.

Language: Английский

Citations

4
Evaluating Molecular Similarity Measures: Do Similarity Measures Reflect Electronic Structure Properties? DOI
Rebekah Duke, Chih-Hsuan Yang, Baskar Ganapathysubramanian

et al.

Journal of Chemical Information and Modeling, Journal Year: 2025, Volume and Issue: unknown

Published: April 29, 2025

The rapid adoption of big data, machine learning (ML), and generative artificial intelligence (AI) in chemical discovery has heightened the importance quantifying molecular similarity. Molecular similarity, commonly assessed as distance between fingerprints, is integral to applications such database curation, diversity analysis, property prediction. AI tools frequently rely on these similarity measures cluster molecules under assumption that structurally similar exhibit properties. However, this not universally valid, particularly for continuous properties like electronic structure Despite prevalence fingerprint-based measures, their evaluation largely depended biological activity data sets qualitative metrics, limiting relevance nonbiological domains. To address gap, we propose a framework evaluate correlation Our approach builds concept neighborhood behavior incorporates kernel density estimation (KDE) analysis quantify how well capture relationships. Using set over 350 million molecule pairs with structure, redox, optical properties, systematically several fingerprint generators, functions, Both curated are publicly available.

Language: Английский

Citations

0
ExpFlow: a graphical user interface for automated reproducible electrochemistry DOI Creative Commons
Rebekah Duke, Siamak Mahmoudi, Aman Preet Kaur

et al.

Digital Discovery, Journal Year: 2023, Volume and Issue: 3(1), P. 163 - 172

Published: Dec. 5, 2023

ExpFlow, a software that allows the systematic encoding of laboratory workflows through graphical user interface, facilitates translation human-developed procedures to robotic experimentation.

Language: Английский

Citations

7
Development of a multi‐step screening procedure for redox active molecules in organic radical polymer anodes and as redox flow anolytes DOI Creative Commons
Andreas J. Achazi, Xhesilda Fataj,

Philip Rohland

et al.

Journal of Computational Chemistry, Journal Year: 2024, Volume and Issue: 45(14), P. 1112 - 1129

Published: Jan. 23, 2024

Benzo[d]-X-zolyl-pyridinyl (XO, S, NH) radicals represent a promising class of redox-active molecules for organic batteries. We present multistep screening procedure to identify the most radical candidates. Experimental investigations and highly correlated wave function-based calculations are performed determine benchmark redox potentials. Based on these, accuracies different methods (semi-empirical, density functional theory, function-based), solvent models, dispersion corrections, basis sets evaluated. The developed consists three steps: First, conformer search is with CREST. selected based potentials calculated using GFN2-xTB. Second, HOMO energies reparametrized B3LYP-D3(BJ) def2-SVP set used as selection criteria. final from Gibbs BP86-D3(BJ)/def2-TZVP. With this approach, can be suggested synthesis, structure-property relationships derived.

Language: Английский

Citations

2
In the Mix: A Workshop Merging Computational Chemistry and Electrochemistry Alongside Data Science DOI
Rebekah Duke,

Amelia Kaye Sweet,

Nathan C. Stumme

et al.

Journal of Chemical Education, Journal Year: 2024, Volume and Issue: 101(11), P. 5060 - 5067

Published: Oct. 17, 2024

As chemistry expands to more complex and interdisciplinary areas, a new generation of diverse researchers must engage with science learn effective cross-disciplinary collaboration communication. To these ends, we designed implemented In the Mix, graduate student-led, two-day workshop for undergraduate students promoting collaborative in context energy storage innovations. The interactive was future emerging gain hands-on experience data science, computational chemistry, electrochemistry techniques that are critical developing materials battery technologies. Participants also visited commercial renewable facilities help them connect discovery-based research industry broader societal considerations. content structure ensured participants experienced interrelatedness fields understood importance yield scientific advances real-world applications. An external team evaluated participants' perceptions their experiences. While our storage, goals outcomes applicable other contexts. Interdisciplinary, experiential workshops key avenue broadening participation research, ideas presented here can be readily modified contexts and/or incorporated as impact activities.

Language: Английский

Citations

1
Towards Reproducible and Automated Electrochemistry DOI Creative Commons
Rebekah Duke, Siamak Mahmoudi, Aman Preet Kaur

et al.

Published: July 31, 2023

Ensuring scientific reproducibility holds increasing importance in chemistry as it underpins the credibility and integrity of research findings. However, reproducing experiments measurements is often hindered by incomplete or ambiguous procedural data literature. Additionally, time-consuming process generation limits scale experiments. Growing efforts towards automation will contribute to enhancing reproducibility. Nevertheless, both manual development automated require improved methods for recording sharing experimental procedures machine-readable formats. Here we develop ExpFlow, a reporting software that currently targets electrochemistry. The ExpFlow allows researchers systematically encode laboratory through graphical user interface operates like fill-in-the-blank lab notebook. Built-in calculators derive properties such diffusion coefficient charge-transfer rate constant. ExpFlow’s workflows enable easy translation human-developed robotic experimentation. We deploy with system perform cyclic voltammetry measurements, several literature-reported electrochemical results. Ultimately, these tools facilitate high-throughput experimentation, reproducibility, eventually data-driven discovery

Language: Английский

Citations

2
Extracting Recalcitrant Redox Data on Fluorophores to Pair with Optical Data for Predicting Small-Molecule, Ionic Isolation Lattices DOI Creative Commons
Michaela K. Loveless, Minwei Che, Alec J. Sanchez

et al.

Digital Discovery, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

We used a semimanual approach to mine optical data from the literature using expert annotations. identify 47 dye candidates for emissive SMILES materials. This workflow has promise design of other

Language: Английский

Citations

0
Beyond conventional batteries: a review on semi-solid and redox targeting flow batteries-LiFePO4 as a case study DOI

Nabil El Halya,

Marwa Tayoury,

Mohamed Aqil

et al.

Sustainable Energy & Fuels, Journal Year: 2024, Volume and Issue: 8(11), P. 2330 - 2356

Published: Jan. 1, 2024

Semi-solid and redox targeting flow batteries present high energy densities compared to conventional batteries. LiFePO 4 active material is a promising catholyte for semi-solid

Language: Английский

Citations

0
Structural, Ionic, and Electronic Properties of Solid-State Phthalimide-Containing Polymers for All-Organic Batteries DOI Creative Commons
Riccardo Alessandri, Cheng-Han Li, Sheila M. Keating

et al.

Published: March 21, 2024

Redox-active polymers serving as the active materials in solid-state electrodes offer a promising path towards realizing all-organic batteries. While both cathodic and an- odic redox-active are needed, diversity of available anodic is limited. Here, we predict structural, ionic, electronic properties anodic, phthalimide-containing using multiscale approach that combines atomistic molecular dynamics, structure calculations, machine learning surrogate models. Importantly, by combining information from each these scales, able to bridge gap between bottom-up characteristics macro- scopic such apparent diffusion coefficients electron transport ($D_{app}$). We investigate impact different polymer backbones two critical factors during battery operation: state charge swelling. Our findings reveal significantly influences packing thermophys- ical polymers, which, turn, affect ionic transport. A combination molecular-level (such reorganization energy) condensed-phase effective hopping distances) determine predicted ranking capabilities polymers. Dapp for phthalimide-based reference nitroxide radical-based polymer, finding three orders magnitude increase $D_{app}$ ($\approx 10^{−6}$ cm$^2$ s$^{−1}$) with respect reference. This study underscores promise highly capable batteries, due their exceptional capabilities.

Language: Английский

Citations

0
Structural, Ionic, and Electronic Properties of Solid-State Phthalimide-Containing Polymers for All-Organic Batteries DOI Creative Commons
Riccardo Alessandri, Cheng-Han Li, Sheila Keating

et al.

JACS Au, Journal Year: 2024, Volume and Issue: 4(6), P. 2300 - 2311

Published: June 7, 2024

Redox-active polymers serving as the active materials in solid-state electrodes offer a promising path toward realizing all-organic batteries. While both cathodic and anodic redox-active are needed, diversity of available is limited. Here, we predict structural, ionic, electronic properties anodic, phthalimide-containing using multiscale approach that combines atomistic molecular dynamics, structure calculations, machine learning surrogate models. Importantly, by combining information from each these scales, able to bridge gap between bottom-up characteristics macroscopic such apparent diffusion coefficients electron transport (Dapp). We investigate impact different polymer backbones two critical factors during battery operation: state charge swelling. Our findings reveal significantly influences packing thermophysical polymers, which, turn, affect ionic transport. A combination molecular-level (such reorganization energy) condensed-phase effective hopping distances) determine predicted ranking capabilities polymers. Dapp for phthalimide-based reference nitroxide radical-based polymer, finding 3 orders magnitude increase (≈10–6 cm2 s–1) with respect reference. This study underscores promise highly capable batteries, due their exceptional capabilities.

Language: Английский

Citations

0