Singlet oxygen evolution from layered transition metal oxide cathode materials and its implications for lithium-ion batteries
By J. Wandt, A. Freiberg, A. Ogrodnik, H. Gasteiger. Materials Today, 2018
387 citations recorded by the source corpus.
Abstract For achieving higher energy density lithium-ion batteries, the improvement of cathode active materials is crucial. The most promising cathode materials are nickel-rich layered oxides LiNixCoyMnzO2 (NCM) and over lithiated NCM (often called HE-NCM). Unfortunately, the full capacity of NCM cannot be utilized due to its limited cycle-life at high state-of-charge (SOC), while HE-NCM requires high voltages. By operando emission spectroscopy, we show for the first time that highly reactive singlet oxygen is released when charging NCM and HE-NCM to an SOC beyond ≈80%. In addition, on-line mass-spectrometry reveals the evolution of CO and CO2 once singlet oxygen is detected, providing significant evidence for the reaction between singlet oxygen and electrolyte to be a chemical reaction. It is controlled by the SOC rather than by potential, as would be the case for a purely electrochemical electrolyte oxidation. Singlet oxygen formation therefore imposes a severe challenge to the development of high-energy batteries based on layered oxide cathodes, shifting the focus of research from electrochemically stable 5 V-electrolytes to chemical stability toward singlet oxygen.
Subfields: Electrical and Electronic Engineering, Materials Chemistry
View Paper: https://www.semanticscholar.org/paper/10086aee67f484675cb8094069e677b1faa69627
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Citations in the corpus
- A review of gas evolution in lithium ion batteries (2020, background): “It has been found that oxygen evolution is not dependent on cell potential but is reliant on the state of charge (SOC) and is onset at a SOC of 80% for NMC materials [40,43].”
- A review of the degradation mechanisms of NCM cathodes and corresponding mitigation strategies (2023, background): “Furthermore, it was shown by operando emission spectroscopy that oxygen evolves in the form of singlet oxygen 1O2[76], which is very reactive and either undergoes quenching to form ground state triplet oxygen or attacks the electrolyte, evoking further gas release in the form of CO and CO2[40,75,76]”
- Degradation Mechanisms and Mitigation Strategies of Nickel-Rich NMC-Based Lithium-Ion Batteries (2019, background): “> 80%) [86], CO and CO2 can also be traced back to the reaction between O2 and alkyl carbonate electrolytes (Eq.”