Jacob Florian

All Publications

• Revealing Solvent-Assisted Li+ Transport in the Solid Electrolyte Interphase operando. Journal of the American Chemical Society Florian, J., Lyu, H., Choi, I. R., Mondonico, L., Lam, S., Zhao, Y., Kim, M. J., Westover, A., Cui, Y., Sacci, R. L., Bao, Z. 2025

  Abstract

  The performance of energy-dense lithium metal batteries is critically influenced by the properties of the solid electrolyte interphase (SEI). Yet, progress in understanding this layer has been limited by the lack of accurate operando characterization because the SEI evolves dynamically during cycling. Here, we apply dynamic electrochemical impedance spectroscopy (dEIS) to resolve the real-time evolution of the SEI on lithium metal in ether-based electrolytes with varying degrees of fluorination. We find that faster stabilization of the compact SEI resistance correlates with improved passivation and higher Coulombic efficiency. Unexpectedly, compact SEI resistance correlates directly with Li+ solvation energy, revealing that weaker Li+ solvation increases not only bulk but also interphase resistance. These findings challenge the conventional view of the SEI as a purely solid-phase conductor and instead support a solvent-assisted Li+ transport mechanism within the compact SEI. This framework emphasizes the need to balance SEI ionic conductivity with the Li+ solvation environment to maximize lithium metal battery performance.

  View details for DOI 10.1021/jacs.5c14284

  View details for PubMedID 41202327

• Asymmetric ether solvents for high-rate lithium metal batteries NATURE ENERGY Choi, I., Chen, Y., Shah, A., Florian, J., Serrao, C., Holoubek, J., Lyu, H., Zhang, E., Lee, J., Lin, Y., Kim, S., Park, H., Zhang, P., Lee, J., Qin, J., Cui, Y., Bao, Z. 2025

  View details for DOI 10.1038/s41560-025-01716-w

  View details for Web of Science ID 001421539700001

• Analyzing Structure-Activity Variations for Mn-Carbonyl Complexes in the Reduction of CO2 to CO INORGANIC CHEMISTRY Florian, J., Cole, J. M. 2022: 318-335

  Abstract

  Contemporary electrocatalysts for the reduction of CO2 often suffer from low stability, activity, and selectivity, or a combination thereof. Mn-carbonyl complexes represent a promising class of molecular electrocatalysts for the reduction of CO2 to CO as they are able to promote this reaction at relatively mild overpotentials, whereby rare-earth metals are not required. The electronic and geometric structure of the reaction center of these molecular electrocatalysts is precisely known and can be tuned via ligand modifications. However, ligand characteristics that are required to achieve high catalytic turnover at minimal overpotential remain unclear. We consider 55 Mn-carbonyl complexes, which have previously been synthesized and characterized experimentally. Four intermediates were identified that are common across all catalytic mechanisms proposed for Mn-carbonyl complexes, and their structures were used to calculate descriptors for each of the 55 Mn-carbonyl complexes. These electronic-structure-based descriptors encompass the binding energies, the highest occupied and lowest unoccupied molecular orbitals, and partial charges. Trends in turnover frequency and overpotential with these descriptors were analyzed to afford meaningful physical insights into what ligand characteristics lead to good catalytic performance, and how this is affected by the reaction conditions. These insights can be expected to significantly contribute to the rational design of more active Mn-carbonyl electrocatalysts.

  View details for DOI 10.1021/acs.inorgchem.2c03391

  View details for Web of Science ID 000904442000001

  View details for PubMedID 36541860

  View details for PubMedCentralID PMC9832541