(303b) Advancing Energy Sustainability: In Situ 3D Neutron and X-Ray Imaging for Electrochemical Systems

Efforts to decarbonize and achieve net-zero greenhouse gas (GHG) emissions by 2050¹ rely heavily on electrifying the transportation sector—responsible for 28% of U.S. GHG emissions²—and decarbonizing energy-intensive chemical processes, such as ammonia (NH₃) synthesis and CO₂ conversion. While next-generation batteries must be low-cost, safe, fast-charging, long-lasting, and composed of abundant materials,³ electrochemical processes for NH₃ and CO₂ activation offer transformative pathways for sustainable energy storage and production.⁴ However, challenges such as interfacial degradation, electrochemical-mechanical instabilities, and limited mechanistic understanding of key degradation phenomena hinder the practical implementation of these systems.⁵

In this seminar, I will demonstrate how advanced in situ/operando neutron and X-ray 3D imaging diagnostics, integrated with electrochemistry, address key challenges in energy storage and conversion systems.⁶ The discussion will focus on: (A) Technique development, including the feasibility of simultaneous neutron and X-ray tomography for visualizing graphite electrode degradation after fast charging.⁷ (B) Electrochemical engineering advancements, including the development of a neutron-friendly battery for in situ lithium detection during fast charging⁸ and an anode-free solid-state battery compatible with simultaneous neutron and X-ray tomography. (C) Insights into 3D lithium plating morphologies, spatial heterogeneities in fast-charged lithium-ion batteries,^9-10and how lithium penetration and current density drive mechanical instabilities at solid-solid interfaces in anode-free solid-state batteries.¹¹

These studies provide a deeper understanding of electrode deterioration, lithium behavior, and electrochemical-mechanical instabilities, which are critical for advancing lithium-ion batteries, solid-state batteries, and electrochemical systems for sustainable NH₃ synthesis and CO₂ conversion. This work highlights the essential role of advanced in situ 3D characterization and electrochemistry in advancing energy sustainability.

• Net Zero Coalition | United Nations: https://www.un.org/en/climatechange/net-zero-coalition.
• United States Environmental Protection Agency: https://www.epa.gov/greenvehicles/fast-facts-transportation-greenhouse-gas-emissions.
• Wang, C. Y., Liu, T., Yang, X. G., Ge, S., Stanley, N. V., Rountree, E. S., ... & McCarthy, B. D. (2022). Fast charging of energy-dense lithium-ion batteries. Nature, 611(7936), 485-490.
• Mallapragada, D. S., Dvorkin, Y., Modestino, M. A., Esposito, D. V., Smith, W. A., Hodge, B. M., ... & Taylor, A. D. (2023). Decarbonization of the chemical industry through electrification: Barriers and opportunities. Joule, 7(1), 23-41.
• Paul, P. P., Chen, B. R., Langevin, S. A., Dufek, E. J., Weker, J. N., & Ko, J. S. (2022). Interfaces in all solid state Li-metal batteries: a review on instabilities, stabilization strategies, and scalability. Energy Storage Materials, 45, 969-1001.
• Yusuf, M., (2025). In Situ 3D Neutron and X-ray Imaging for Battery Diagnostics. The Electrochemical Society Interface. [Invited Perspective, In Press]
• Yusuf, M., LaManna, J. M., Paul, P. P., Agyeman-Budu, D. N., Cao, C., Dunlop, A. R., ... & Weker, J. N. (2022). Simultaneous neutron and X-ray tomography for visualization of graphite electrode degradation in fast-charged lithium-ion batteries. Cell Reports Physical Science, 3(11). [Editor's Choice 2022, Most-Read Article of November 2022].
• Yusuf, M., et al. Neutron-friendly Li-ion battery coin cell for in situ 3D visualization of Li plating, In Preparation.
• Yusuf, M. (2022). The In-situ Characterization of Fast-charging Degradation Modes in Li-ion Batteries Using High-resolution Neutron Imaging. The Electrochemical Society Interface, 31(4), 38. [2022 Edward G. Weston Fellowship – Summary Report.]
• Yusuf, M., Kaestner, A., Wied, M., LaManna, J., Vo, N. T., Dunlop, A. R., ... & Weker, J. N. (2024). Visualizing 3D Morphologies and Spatial Heterogeneities of Li after Fast-Charging via In-situ Neutron Tomography. ChemRxiv. https://doi.org/10.26434/chemrxiv-2024-w1rmf. (2024 Energy Technology Division Graduate Student Award sponsored by BioLogic at 245th Electrochemical Society Meeting.)
• Yusuf, M. (2024). In Situ Simultaneous Neutron and X-ray Tomography of Solid-Solid interfaces in Anode-Free Solid-state Batteries. The Electrochemical Society Interface, 33(4), 36 [2024 Colin Garfield Fink Fellowship – Summary Report.]

Keywords: energy sustainability, in situ 3D imaging, electrochemical systems, batteries, N₂ and CO₂ activation