Effect of single-walled carbon nanotube sub-carbon additives and graphene oxide coating for enhancing the 5 V LiNi0.5Mn1.5O4 cathode material performance in lithium-ion batteries

• Main Authors: Tsai, Yi-De, Shih, Jeng-Ywan, Li, Ying-Jeng James, Hung, Tai-Feng, Hsu, Li-Fan, Ramraj, Sayee Kannan, Rajan, Jose, Karuppiah, Chelladurai, Yang, Chun-Chen
• Format: Article
• Language: English; English
• Published: ACS Publications 2022
• Subjects: QC Physics; QD Chemistry; TK Electrical engineering. Electronics Nuclear engineering
• Online Access: http://umpir.ump.edu.my/id/eprint/38067/1/2022--p16--ACS-SCE-Effect%20of%20Single-Walled%20Carbon%20Nanotube%20Sub-carbon%20Additives%20and%20GO%20for%205V%20LNMO.pdf; http://umpir.ump.edu.my/id/eprint/38067/7/Effect%20of%20single-walled%20carbon%20nanotube%20sub-carbon%20additives%20and%20graphene%20oxide%20.pdf; http://umpir.ump.edu.my/id/eprint/38067/; https://doi.org/10.1021/acssuschemeng.2c04808; https://doi.org/10.1021/acssuschemeng.2c04808

High-voltage spinel LiNi0.5Mn1.5O4 (LNMO) is a promising cathode material for next-generation lithium-ion batteries (LIBs), but its poor cycle performance has impeded its commercialization. In this study, we developed highly stable LNMO cathode materials having an octahedral morphology through a solid-state high-energy ball-mill–cum–spray-drying method. We also developed a novel strategy for modifying this cathode material with two kinds of carbon materials, thereby improving the electrochemical cycling performance. Introducing single-walled carbon nanotubes (SWCNTs) as a sub-carbon conductive additive during the slurry preparation process improved the conductivity of electrons between the particles of the cathode material. The LNMO electrode modified with the SWCNT sub-carbon additives exhibited an average Coulombic efficiency of 99.4% after 500 cycles at 1C, compared with 98.9% for the pristine LNMO-based electrode. Furthermore, we used a wet-chemical method to coat graphene oxide (GO) onto the post-sintered LNMO cathode material to act as a protective layer, preventing corrosion induced by HF in the electrolyte. The capacity retention of the GO-coated LNMO electrode after 500 cycles at 1C (91.8%) was higher than that of the pristine LNMO (52.5%). The corresponding dual-modification strategy, combining the SWCNTs and GO, provided LNMO cathode materials exhibiting superior rate performance and cyclability, with an average Coulombic efficiency of 99.3% and capacity retention of 92.9% after 500 cycles at 1C. Thus, the LNMO cathode materials prepared in this study possessed excellent electrochemical properties favoring their marketability, applicability, and competitiveness for application in high-voltage LIBs.