TY - JOUR
T1 - Computational and Machine Learning-Assisted Discovery and Experimental Validation of Conjugated Sulfonamide Cathodes for Lithium-Ion Batteries
AU - Zhou, Xuan
AU - Xu, Cheng
AU - Guo, Xiaolong
AU - Apostol, Petru
AU - Vlad, Alexandru
AU - Janssen, René A.J.
AU - Er, Süleyman
N1 - Publisher Copyright:
© 2024 Wiley-VCH GmbH.
PY - 2024
Y1 - 2024
N2 - Conjugated sulfonamides (CSAs) stand out for their propitious electroactivity and notable stability in ambient conditions, making them suitable candidates for high-potential cathode materials in lithium-ion batteries (LIBs). This study employs a combination of machine learning, semi-empirical quantum mechanics, and density functional theory methods to evaluate a large library of 11 432 CSA molecules, focusing on material properties crucial for application in batteries, such as synthetic complexity, redox potential, gravimetric charge capacity, and energy density. After applying the thresholds for the synthetic complexity score at 2.62 and the redox potential at 3.25 V versus Li/Li+, we identify 50 CSA molecules that are easy to synthesize and suitable for the positive electrode in LIBs. By ranking on the basis of redox potential, 13 CSA molecules having potentials greater than 3.50 V versus Li/Li+ are identified. Through further investigations using molecular dynamics simulations on these reactant molecules and their lithiated products, a molecule is singled out for synthesis and electrochemical evaluation. This molecule, lithium (2,5-dicyano-1,4-phenylene)bis((methylsulfonyl)amide)(Li2-DCN-PDSA), demonstrates a redox potential surpassing those previously reported within the class of CSA molecules. Moreover, the study explores the quantitative structure-property relations of CSAs, yielding insights for the development of CSA-based LIB cathode materials, informed by the comprehensive data assembled.
AB - Conjugated sulfonamides (CSAs) stand out for their propitious electroactivity and notable stability in ambient conditions, making them suitable candidates for high-potential cathode materials in lithium-ion batteries (LIBs). This study employs a combination of machine learning, semi-empirical quantum mechanics, and density functional theory methods to evaluate a large library of 11 432 CSA molecules, focusing on material properties crucial for application in batteries, such as synthetic complexity, redox potential, gravimetric charge capacity, and energy density. After applying the thresholds for the synthetic complexity score at 2.62 and the redox potential at 3.25 V versus Li/Li+, we identify 50 CSA molecules that are easy to synthesize and suitable for the positive electrode in LIBs. By ranking on the basis of redox potential, 13 CSA molecules having potentials greater than 3.50 V versus Li/Li+ are identified. Through further investigations using molecular dynamics simulations on these reactant molecules and their lithiated products, a molecule is singled out for synthesis and electrochemical evaluation. This molecule, lithium (2,5-dicyano-1,4-phenylene)bis((methylsulfonyl)amide)(Li2-DCN-PDSA), demonstrates a redox potential surpassing those previously reported within the class of CSA molecules. Moreover, the study explores the quantitative structure-property relations of CSAs, yielding insights for the development of CSA-based LIB cathode materials, informed by the comprehensive data assembled.
KW - conjugated sulfonamides
KW - electrochemistry
KW - high-throughput computational screening
KW - lithium-ion batteries
UR - http://www.scopus.com/inward/record.url?scp=85200245503&partnerID=8YFLogxK
U2 - 10.1002/aenm.202401658
DO - 10.1002/aenm.202401658
M3 - Article
AN - SCOPUS:85200245503
SN - 1614-6832
JO - Advanced Energy Materials
JF - Advanced Energy Materials
ER -