Daxian Cao

The surge in electric vehicle demand has propagated the extensive application of lithium-ion batteries (LIBs) in recent years. Gaining significant traction due to their promising high-energy density and elevated safety over traditional LIBs, all-solid-state Li batteries (ASLBs) have nonetheless been faced with hurdles relating to battery performance. These include concerns with interfacial compatibility, structural stability, Li dendrite inhibition, and large-scale manufacturing. To tackle these issues, it is necessary to employ advanced characterization methods to comprehend the intrinsic mechanisms within ASLBs. In this article, we advocate for the use of neutron imaging as a nondestructive approach for the operando visualization of ASLBs. We draw comparisons with other operando visualization strategies, underline the benefits of neutron imaging, and discuss its potential applicability in the scrutiny of all-solid-state Li metal batteries and all-solid-state Li-sulfur batteries. Neutron imaging provides valuable insights into the dynamics of Li concentration, reaction mechanisms, and transport constraints in ASLBs. These insights are pivotal in contributing to the evolution of high-performance all-solid-state batteries. Graphical abstract This article discusses the application of neutron imaging for operando characterization of all-solid-state batteries. It compares neutron imaging to other techniques and highlights its advantages in visualizing light elements such as lithium. It also covers recent progress in using neutron imaging to investigate reaction mechanisms, lithium dynamics, and failure modes in all-solid-state lithium metal and lithium sulfur batteries. It also analyzes the future outlook for neutron imaging as a powerful nondestructive tool to gain insights into interfacial phenomena in all-solid-state batteries.