(4k) Understanding the Relationship between Composition and Functionality in Lithium Metal Solid Electrolyte Interphases

I earned my B.S.E. in Chemical Engineering at Case Western Reserve University, doing research in electrochemistry with Professor Rohan Akolkar. I am currently in the final year of my Chemical Engineering PhD studies at MIT, where I have worked with Professors Karthish Manthiram and Betar Gallant, researching lithium interfacial behavior in electrosynthesis and energy storage systems. I plan to graduate in the spring or summer of 2025 and begin a postdoc in the fall of 2025. Throughout my education, I have been motivated by an interest in sustainability and a desire to contribute to the decarbonization of energy and industry.

PhD Work

My research has centered on understanding the passivation of lithium (Li) in electrochemical systems. Metallic Li is thermodynamically unstable in practical electrolytes, and as a result, it forms a passivation layer of reduced electrolyte species at its surface, typically tens of nanometers thick and containing a mixture of organic and inorganic species. This film, called the solid electrolyte interphase (SEI), mediates reactivity and transport at the Li interface and is strongly influential on the functionality of Li systems.

In my first project, I studied the influence of the SEI in Li-mediated electrochemical ammonia synthesis (LiMEAS). LiMEAS is among the most promising ambient-temperature electrochemical methods to electrify NH₃ synthesis, leveraging the ability of Li to activate the N₂ bond, forming Li₃N, which can then be protonated (e.g. by reaction with ethanol) to yield NH₃. We developed a multiscale approach to study the influence of Li passivation on this pathway, combining product quantification techniques with spectroscopy and cryo-electron microscopy (performed in collaboration with Professor Yuzhang Li’s group at UCLA). Through this study, we observed that the proton donor governs the reactivity of Li with N₂. Without ethanol present, the SEI passivates Li, inhibiting N₂ reduction; with the addition of ethanol, the SEI is disrupted, allowing Li to be consumed by reactions with N₂, ethanol, and other electrolyte components. This dual function of the proton donor—to both disrupt passivation and protonate—is vital to the functionality of LiMEAS.

Next, I transitioned to studying the SEI in Li metal batteries. Replacing graphite anodes with metallic Li could unlock ~10x higher gravimetric energy densities in Li-ion batteries, but Li anodes have yet to achieve the cycling efficiencies required for long-term, safe operation. The SEI is a key factor in determining their performance, yet our understanding of the functionality of common SEI materials remains limited. We set out to understand the role of Li₂CO₃, which has been previously associated with improved cyclability achieved through CO_2­ saturation of electrolytes, but possesses several decomposition pathways that call into question its ability to effectively passivate Li. We developed a two-pronged approach to study this material: (i) the synthesis and study of a model Li₂CO₃-containing SEI, and (ii) cycling and titration-based quantification of species generated by cycling of Li-Cu cells with or without additive CO₂. Using these platforms, we observed that Li₂CO₃ has a higher Li⁺ conductivity than other previously-measured ionic SEI phases, and that its enrichment leads to less accumulation of electronically-isolated, inactive Li. These findings highlight the utility of Li₂CO₃ as an SEI phase, particularly in elevating the performance of low-cost carbonate electrolytes.

Research Interests

Upon finishing my PhD, I plan to pursue a postdoctoral position with a focus on electrochemical technologies relevant to decarbonization. Some of the topics I find most interesting are earth-abundant battery chemistries for grid-scale energy storage, electrochemical resource recovery and recycling, and molten salt metallurgy. I would relish the opportunity to learn new experimental techniques such as solid-state NMR, synchrotron-based spectroscopies, and in situ characterization techniques, and to deepen my understanding of the physics underlying these methods.

Selected Works

K Steinberg and BM Gallant, “Revealing the Role of Lithium Carbonate at Lithium Metal Anodes Through Study of Gas-Reacted Interphases,” under review.

GM Hobold, C Wang, K Steinberg, Y Li, and BM Gallant, “High lithium oxide prevalence in the lithium solid-electrolyte interphase for high Coulombic efficiency,” Nature Energy 9, 580-591, (2023).

K Steinberg, X Yuan, CK Klein, N Lazouski, M Mecklenburg, K Manthiram, Y Li, “Imaging of nitrogen fixation at lithium solid electrolyte interphases via cryo-electron microscopy,” Nature Energy 8, 138-148, (2023).

N Lazouski, KJ Steinberg, ML Gala, D Krishnamurthy, V Viswanathan, K Manthiram, “Proton donors induce a differential transport effect for selectivity toward ammonia in lithium-mediated nitrogen reduction,” ACS Catalysis 12, 5197-5208, (2022).