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Malonatophosphate as an SEI- and CEI-forming additive that outperforms malonatoborate for thermally robust lithium-ion batteries

Malonatophosphate as an SEI- and CEI-forming additive that outperforms malonatoborate for thermally robust lithium-ion batteries
Park, Jong WonPark, Doh HeeGo, SoohyunNam, Dae-HyunOh, JihunHan, Young-KyuLee, Hochun
Issued Date
Energy Storage Materials, v.50, pp.75 - 85
Author Keywords
Lithium− ion batteriesCathode electrolyte interphaseSolid electrolyte interphaseLithium difluoro(fluoromalonato)borateLithium tetrafluoro(fluoromalonato)phosphate
Ni-rich nickel-cobalt-manganese layered oxides have been widely used as advanced cathode materials; however, they exhibit poor thermal stability at elevated temperatures. Therefore, in this study, we synthesized lithium tetrafluoro(fluoromalonato)phosphate (LFMP) as a dual-functional electrolyte additive to improve the thermal stability of LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode and graphite anode materials. The LFMP additive imparts excellent cyclability, storage performance, and mitigated gas evolution of NCM811/graphite cells at 60°C compared to its boron analog, lithium difluoro(fluoromalonato)borate (LFMB). The vast advantages of the LFMP additive can be attributed to the following two-fold origin: (i) On the NCM811 cathode, LFMP derives a cathode electrolyte interphase (CEI) that suppresses electrolyte decomposition and gas evolution more effectively than LFMB; (ii) On the graphite anode, LFMP induces a LiF-rich solid electrolyte interphase (SEI) that is more resistant to attack by phosphorus pentafluoride (PF5) than an LFMB-induced organic-rich SEI. Our first-principles calculations corroborate that the CEI and SEI layers derived by LFMP are superior to those of LFMB owing to the strong binding with a superoxide radical (O2▪−) and weak binding with PF5 and favorable LiF formation, respectively. Considering its advantages, LFMP is an outstanding electrolyte additive for thermally stable NCM811/graphite batteries. This study opens a new avenue for using malonatophosphates as a new class of electrolyte additives for enhanced surface stability of Ni-rich cathodes and graphite anodes. © 2022
Elsevier BV
Related Researcher
  • 남대현 Nam, Dae-Hyun 에너지공학과
  • Research Interests Carbon dioxide reduction; Water splitting; Energy conversion; Electrochemistry; Materials Science
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Appears in Collections:
Department of Energy Science and Engineering Renewable Energy Conversion Materials Laboratory 1. Journal Articles
Department of Energy Science and Engineering Electrochemistry Laboratory for Sustainable Energy(ELSE) 1. Journal Articles


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