Polyethylene Glycol Surface Modification and Polythiophene Side-Chain Chemistry: A Combined Strategy toward High-Capacity Lithium-Ion Battery Anodes

Li, Han; Ren, Haoze; Rodriguez Campos, Armando; Qin, Siyu; Thorpe, Ryan; Sun, Zeyuan; Sun, Mengting; Takeuchi, Esther S.; Marschilok, Amy C.; Takeuchi, Kenneth J.; Reichmanis, Elsa

doi:10.1021/acsaem.5c01648

Polyethylene Glycol Surface Modification and Polythiophene Side-Chain Chemistry: A Combined Strategy toward High-Capacity Lithium-Ion Battery Anodes

Journal Article · Wed Jul 30 00:00:00 EDT 2025 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.5c01648· OSTI ID:2583412

^[1]; ^[1]; Rodriguez Campos, Armando ^[2]; ^[1]; Thorpe, Ryan ^[1]; ^[1]; ^[1]; ^[3]; ^[3]; ^[3]; ^[1]

Lehigh Univ., Bethlehem, PA (United States)
Stony Brook Univ., NY (United States)
Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

In the development of high-capacity lithium-ion batteries (LIBs), the combined optimization of active material interfaces and polymer binder chemistry plays a critical role in improving electrode performance and longevity. This work explores a dual design strategy incorporating polyethylene glycol (PEG) surface modification and carboxylated polythiophene side-chain tailoring to enhance the electrochemical behavior of magnetite (Fe₃O₄)-based anodes. PEG is employed to improve interfacial stability, while carboxylated polythiophene binders with varying alkyl side-chain lengths─poly[3-(potassium-4-butanoate)thiophene-2,5-diyl] (P3KBT), poly[3-(potassium-5-pentanoate)thiophene-2,5-diyl] (P3KPT), and poly[3-(potassium-6-hexanoate)thiophene-2,5-diyl] (P3KHT)─are used to modulate molecular interactions and ion transport. Among these three analogs, the PEG–Fe₃O₄–P3KHT electrode exhibits superior ion-transfer kinetics, the highest capacity retention, and the lowest charge-transfer resistance after extended cycling. Compared to their non-PEG analogs, PEG-coated electrodes demonstrate enhanced structural integrity and electrochemical behavior, emphasizing the synergistic effects of surface modification and side-chain chemistry. These findings highlight the importance of interfacial interactions and molecular design in achieving robust and high-performance composite anodes for next-generation LIBs.

View Accepted Manuscript (DOE)

Research Organization:: Stony Brook Univ., NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012673

OSTI ID:: 2583412

Journal Information:: ACS Applied Energy Materials, Journal Name: ACS Applied Energy Materials Journal Issue: 15 Vol. 8; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Polyethylene Glycol Surface Modification and Polythiophene Side-Chain Chemistry: A Combined Strategy toward High-Capacity Lithium-Ion Battery Anodes

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