Deep Learning-Driven Molecular Generation and Electrochemical Property Prediction for Optimal Electrolyte Additive Design
Source abstract
Abstract
Recently, generative models have rapidly advanced and are being applied to various domains beyond vision and large language models (LLMs). In the field of chemistry and molecular generation, deep learning-based models are increasingly utilized to reduce experimental exploration and research costs. In this study, we conducted research on Variational Autoencoder-based molecular generation and property prediction to screen for optimal molecules in the design of electrolyte additives for lithium-ion batteries. Using a dataset composed of promising electrolyte additive candidate molecules, we generated new molecules and predicted HOMO and LUMO values, which are key factors in electrolyte additive design. For approximately 1000 newly generated electrolyte additive candidate molecules, we performed DFT calculations to obtain HOMO and LUMO values and calculated the mean absolute error (MAE) between the predicted values from the trained model and the DFT-calculated values. As a result, the model demonstrated exceptionally low errors of approximately 0.04996 eV (HOMO) and 0.06895 eV (LUMO), respectively. This means that battery experts can receive recommendations for new molecules, refer to their predicted HOMO and LUMO values, and select potential electrolyte additives for further validation through experiments. By replacing the traditional electrolyte additive development process with deep learning models, this method has the potential to significantly reduce the overall development time and improve efficiency.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Machine Learning in Materials Science · Fuel Cells and Related Materials · Electrocatalysts for Energy Conversion
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Energy IT Convergence Research Center, Korea Electronics Technology Institute, #25, Saenariro, Bundang-gu, Seongnam-si 13509, Gyeonggi-do, Republic of Korea
Funding
Institute of Information & Communications Technology Planning & Evaluation (IITP)
References (71)
Show source-provided references
1. Graph neural networks for materials science and chemistry10.1038/s43246-022-00315-6 ↗
2. A review of graph neural networks: Concepts, architectures, techniques, challenges, datasets, applications, and future directions10.1186/s40537-023-00876-4 ↗
3. Liu, Z., Wan, G., Prakash, B.A., Lau, M.S., and Jin, W. (2024, January 25–29). A Review of Graph Neural Networks in Epidemic Modeling. Proceedings of the 30th ACM SIGKDD Conference on Knowledge Discovery and Data Mining (KDD ’24), Barcelona, Spain.10.1145/3637528.3671455 ↗
4. Vora, L.K., Gholap, A.D., Jetha, K., Thakur, R.R.S., Solanki, H.K., and Chavda, V.P. (2023). Artificial Intelligence in Pharmaceutical Technology and Drug Delivery Design. Pharmaceutics, 15.10.3390/pharmaceutics15071916 ↗
5. Design of functional and sustainable polymers assisted by artificial intelligence10.1038/s41578-024-00708-8 ↗
6. Silicon electro-optic micro-modulator fabricated in standard CMOS technology as components for all silicon monolithic integrated optoelectronic systems10.1088/1361-6439/abf333 ↗
7. Scaling deep learning for materials discovery10.1038/s41586-023-06735-9 ↗
8. Graph neural networks for molecular and materials representation10.20517/jmi.2023.10 ↗
9. Graph neural networks: A review of methods and applications10.1016/j.aiopen.2021.01.001 ↗
10. AI applications through the whole life cycle of material discovery10.1016/j.matt.2020.06.011 ↗
11. AI for dielectric capacitors10.1016/j.ensm.2024.103612 ↗
12. Generative models for molecular discovery: Recent advances and challenges10.1002/wcms.1608 ↗
13. Deep Generative Models in De Novo Drug Molecule Generation10.1021/acs.jcim.3c01496 ↗
14. De novo molecular design and generative models10.1016/j.drudis.2021.05.019 ↗
15. Advances and challenges in deep generative models for de novo molecule generation10.1002/wcms.1395 ↗
16. Deep Learning Methods for Small Molecule Drug Discovery: A Survey10.1109/TAI.2023.3251977 ↗
17. Applications of Deep Learning in Molecule Generation and Molecular Property Prediction10.1021/acs.accounts.0c00699 ↗
18. Deep Learning for Molecular Generation10.4155/fmc-2018-0358 ↗
19. Deep learning for molecular design—A review of the state of the art10.1039/C9ME00039A ↗
20. Generative Deep Learning for Targeted Compound Design10.1021/acs.jcim.0c01496 ↗
21. Molecular generative model based on conditional variational autoencoder for de novo molecular design10.1186/s13321-018-0286-7 ↗
22. Automatic Chemical Design Using a Data-Driven Continuous Representation of Molecules10.1021/acscentsci.7b00572 ↗
23. Design of efficient molecular organic light-emitting diodes by a high-throughput virtual screening and experimental approach10.1038/nmat4717 ↗
24. Kusner, M.J., Paige, B., and Hernández-Lobato, J.M. (2017, January 6–11). Grammar variational autoencoder. Proceedings of the 34th International Conference on Machine Learning, PMLR 70, Sydney, NSW, Australia.
25. Dai, H., Tian, Y., Dai, B., Skiena, S.S., and Song, L. (2017, January 4–9). Syntax-Directed Variational Autoencoder for Molecule Generation. Proceedings of the 31st Conference on Neural Information Processing Systems (NIPS 2017), Long Beach, CA, USA.
26. Liu, Q., Allamanis, M., Brockschmidt, M., and Gaunt, A.L. (2018, January 2–8). Constrained graph variational autoencoders for molecule design. Proceedings of the 32nd International Conference on Neural Information Processing Systems (NIPS’18), Montreal, QC, Canada.
27. Jin, W., Barzilay, R., and Jaakkola, T. (2019). Junction Tree Variational Autoencoder for Molecular Graph Generation. arXiv.10.1039/9781788016841-00228 ↗
28. Jin, W., Barzilay, R., and Jaakkola, T. (2020, January 13–18). Hierarchical generation of molecular graphs using structural motifs. Proceedings of the 37th International Conference on Machine Learning (ICML’20), Virtual.
29. Molecular representations for machine learning applications in chemistry10.1002/qua.26870 ↗
30. A review of molecular representation in the age of machine learning10.1002/wcms.1603 ↗
31. Bidirectional generation of structure and properties through a single molecular foundation model10.1038/s41467-024-46440-3 ↗
32. Molecular Generation and Optimization of Molecular Properties Using a Transformer Model10.26599/BDMA.2023.9020009 ↗
33. Transformer-based models for chemical SMILES representation: A comprehensive literature review10.1016/j.heliyon.2024.e39038 ↗
34. Sadeghi, S., Bui, A., Forooghi, A., Lu, J., and Ngom, A. (2024). Can large language models understand molecules?. BMC Bioinform., 25.10.1186/s12859-024-05847-x ↗
35. Machine learning assisted materials design and discovery for rechargeable batteries10.1016/j.ensm.2020.06.033 ↗
36. Artificial Intelligence Applied to Battery Research: Hype or Reality?10.1021/acs.chemrev.1c00108 ↗
37. Data-driven prediction of battery cycle life before capacity degradation10.1038/s41560-019-0356-8 ↗
38. Advanced Machine Learning Approach for Lithium-Ion Battery State Estimation in Electric Vehicles10.1109/TTE.2015.2512237 ↗
39. State of charge estimation for electric vehicle power battery using advanced machine learning algorithm under diversified drive cycles10.1016/j.energy.2018.08.071 ↗
40. State-of-charge estimation of Li-ion batteries using deep neural networks: A machine learning approach10.1016/j.jpowsour.2018.06.104 ↗
41. Machine Learning: An Advanced Platform for Materials Development and State Prediction in Lithium-Ion Batteries10.1002/adma.202101474 ↗
42. A review of the recent progress in battery informatics10.1038/s41524-022-00713-x ↗
43. Predicting the HOMO-LUMO gap of benzenoid polycyclic hydrocarbons via interpretable machine learning10.1016/j.cplett.2023.140358 ↗
44. A Roadmap for Transforming Research to Invent the Batteries of the Future Designed within the European Large Scale Research Initiative BATTERY 2030+10.1002/aenm.202102785 ↗
45. Rechargeable Batteries of the Future—The State of the Art from a BATTERY 2030+ Perspective10.1002/aenm.202102904 ↗
46. Toward Better and Smarter Batteries by Combining AI with Multisensory and Self-Healing Approaches10.1002/aenm.202100362 ↗
47. Electrolyte additives for lithium ion battery electrodes: Progress and perspectives10.1039/C6EE00123H ↗
48. Atomic Insights into the Fundamental Interactions in Lithium Battery Electrolytes10.1021/acs.accounts.0c00412 ↗
49. SEI-forming electrolyte additives for lithium-ion batteries: Development and benchmarking of computational approaches10.1007/s00894-016-3180-0 ↗
50. Challenges with prediction of battery electrolyte electrochemical stability window and guiding the electrode—Electrolyte stabilization10.1016/j.coelec.2018.10.015 ↗
51. Understanding Battery Interfaces by Combined Characterization and Simulation Approaches: Challenges and Perspectives10.1002/aenm.202102687 ↗
52. A perspective on inverse design of battery interphases using multi-scale modelling, experiments and generative deep learning10.1016/j.ensm.2019.06.011 ↗
53. Inverse molecular design using machine learning: Generative models for matter engineering10.1126/science.aat2663 ↗
54. Variational autoencoder-based chemical latent space for large molecular structures with 3D complexity10.1038/s42004-023-01054-6 ↗
55. The Electrolyte Genome project: A big data approach in battery materials discovery10.1016/j.commatsci.2015.02.050 ↗
56. Commentary: The Materials Project: A materials genome approach to accelerating materials innovation10.1063/1.4812323 ↗
57. Tai, K.S., Socher, R., and Manning, C.D. (2015). Improved Semantic Representations From Tree-Structured Long Short-Term Memory Networks. arXiv.10.3115/v1/P15-1150 ↗
58. Message-passing neural networks for high-throughput polymer screening10.1063/1.5099132 ↗
59. Quantum chemistry structures and properties of 134 kilo molecules10.1038/sdata.2014.22 ↗
60. Polykovskiy, D., Zhebrak, A., Sanchez-Lengeling, B., Golovanov, S., Tatanov, O., Belyaev, S., Kurbanov, R., Artamonov, A., Aladinskiy, V., and Veselov, M. (2020). Molecular Sets (MOSES): A Benchmarking Platform for Molecular Generation Models. Front. Pharmacol., 11.10.3389/fphar.2020.565644 ↗
61. PoseBusters: AI-based docking methods fail to generate physically valid poses or generalise to novel sequences10.1039/D3SC04185A ↗
62. Estimation of synthetic accessibility score of drug-like molecules based on molecular complexity and fragment contributions10.1186/1758-2946-1-8 ↗
63. Zhou, G., Gao, Z., Ding, Q., Zheng, H., Xu, H., Wei, Z., Zhang, L., and Ke, G. (2023, January 1–5). Uni-Mol: A Universal 3D Molecular Representation Learning Framework. Proceedings of the Eleventh International Conference on Learning Representations (ICLR 2023), Kigali, Rwanda.10.26434/chemrxiv-2022-jjm0j-v4 ↗
64. Data-driven quantum chemical property prediction leveraging 3D conformations with Uni-Mol+10.1038/s41467-024-51321-w ↗
65. Rong, Y., Bian, Y., Xu, T., Xie, W., Wei, Y., Huang, W., and Huang, J. (2020). Self-Supervised Graph Transformer on Large-Scale Molecular Data. arXiv.
66. What Is High-Throughput Virtual Screening? A Perspective from Organic Materials Discovery10.1146/annurev-matsci-070214-020823 ↗
67. Electrolyte additives for Li-ion batteries: Classification by elements10.1016/j.pmatsci.2024.101349 ↗
68. Computational screening of solid electrolyte interphase forming additives in lithium-ion batteries10.1016/j.comptc.2014.01.014 ↗
69. Tuning the LUMO Energy of an Organic Interphase to Stabilize Lithium Metal Batteries10.1021/acsenergylett.8b02483 ↗
70. Molecular Property Prediction and Molecular Design Using a Supervised Grammar Variational Autoencoder10.1021/acs.jcim.1c01573 ↗
71. Accelerating Electrolyte Discovery for Energy Storage with High-Throughput Screening10.1021/jz502319n ↗