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Although reliable rechargeable batteries represent a key transformative technology for electric vehicles, portable electronics, and renewable energy, there are few nondestructive diagnostic techniques compatible with realistic commercial cell enclosures. Many battery failures result from the loss or chemical degradation of electrolyte. In this work, we present measurements through battery enclosures that allow quantification of electrolyte amount and composition. The study employs instrumentation and techniques developed in the context of zero-to-ultralow-field nuclear magnetic resonance (ZULF NMR), with optical atomic magnetometers as the detection elements. In contrast to conventional NMR methodology, which suffers from skin-depth limitations, the reduced resonance frequencies in ZULF NMR make battery housing and electrodes transparent to the electromagnetic fields involved. As demonstrated here through simulation and experiment, both the solvent and lithium-salt components of the electrolyte (LiPF6) signature could be quantified using our techniques. Further, we show that the apparatus is compatible with measurement of pouch-cell batteries. 

Abstract Zero- to ultralow-field (ZULF) nuclear magnetic resonance (NMR) is an emerging tool for precision chemical analysis. In this work, we study dynamic processes and investigate the influence of chemical exchange on ZULF NMRJ-spectra. We develop a computational approach that allows quantitative calculation ofJ-spectra in the presence of chemical exchange and apply it to study aqueous solutions of [¹⁵N]ammonium (¹⁵N$${\mathrm{H}}_4^ +$$ $H_4^{+}$) as a model system. We show that pH-dependent chemical exchange substantially affects theJ-spectra and, in some cases, can lead to degradation and complete disappearance of the spectral features. To demonstrate potential applications of ZULF NMR for chemistry and biomedicine, we show a ZULF NMR spectrum of [2-¹³C]pyruvic acid hyperpolarized via dissolution dynamic nuclear polarization (dDNP). We foresee applications of affordable and scalable ZULF NMR coupled with hyperpolarization to study chemical exchange phenomena in vivo and in situations where high-field NMR detection is not possible to implement.