Titration Mass Spectroscopy (TMS): A Quantitative Analytical Technology for Rechargeable Batteries.

Abstract

Development of high-energy-density rechargeable battery systems not only needs advanced qualitative characterizations for mechanism exploration but also requires accurate quantification technology to quantitatively elucidate products and fairly assess numerous modification strategies. Herein, as a reliable quantification technology, titration mass spectroscopy (TMS) is developed to accurately quantify O-related anionic redox reactions (Li-O₂ battery and nickel-cobalt-manganese (NCM)/Li-rich cathodes), parasitic carbonate deposition and decomposition (derived from air-exposure degradation and electrolyte oxidation), and dead Li⁰ formation (Li-metal battery and over-discharged graphite anode). TMS technology can harvest key information on products (e.g., quantification of oxidized lattice oxygen and solid electrolyte interphase (SEI)/cathode electrolyte interphase (CEI) components) and guide corresponding design strategy by enhancing understanding of the mechanism (e.g., clearly distinguish the catalytic target of highly oxidative Ni⁴⁺ on the NCM cathode). Not limited as a rigid quantification tool for widely known products/mechanisms, TMS technology has been demonstrated as a powerful and versatile tool for the investigations of advanced batteries.