Limited stability of most electrode materials (EM) and electrolytes under stringent operating conditions is a matter of concern for the battery research community and industry. In past few years, it has been demonstrated that EMs degrade through their reactive interface with the electrolyte. Undesirable interfacial reactions result in formation of solid precipitates that impede the charge transfer and can serve as an active site for electrolyte consumption, anode corrosion and passivation, thereby, leading to inefficient lithium/sodium ion and metal-O2 batteries (LIB/SIB/LOB). Especially, the progress of high energy and high voltage batteries is mostly restricted by issues associated with the electrode/electrolyte interfacial instability and electro-chemomechanical degradation under the operation conditions. As a result, strategies that (1) stabilize the interface by designing a protection layer commonly known as “artificial solid electrolyte interface (ASEI)” and (2) that can electro/chemically catalyse the reactions and bring the potentials to lower values can significantly enhance battery performance by stabilizing the functional interface and addressing the deleterious reactions between electrode and electrolyte. Nevertheless, there is a dire need of in-operando and in-situ analytical tools to deconvolute the degradation paths to have targeted solutions based on the instability of the components. Online electrochemical mass spectrometry in synergy with solid state NMR can prove to be on such tool.
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