Abstract

Operando characterization techniques including diffraction, microscopy, spectroscopy, etc. are emerging in the last few decades for the study of lithium-ion batteries (LIBs).[1] One of the many advantages of those techniques is that it can help to firmly understand the dynamic behaviors of battery components during the real operations, from various perspectives such as the physical/electrochemical/mechanical properties. Among all operando characterization methods, diffraction using X-rays, electrons, and neutrons undoubtedly plays a vital role as it manages to answer the fundamental questions on the structural changes of any battery components, particularly the electrode materials. Compared to X-ray/electron, neutron diffraction (ND) has irreplaceable advantages for the study of LIBs. For example, neutrons are sensitive to light elements such as Li, C and O, which are often difficult to detect with X-ray/electron diffraction. Neutrons also offer drastically different scattering lengths for neighboring elements in the periodic table or isotopes for the same element. This feature enables the distinction between 3d transition-metal elements (Mn, Fe, Co and Ni) those are frequently used in cathode materials for LIBs. Unlike diffraction, neutron radiography (NR) has often been overlooked to study LIBs, despite it can provide full-scaled imaging information of a battery thanks to the excellent penetration depth of neutrons and good contrast between elements. In this presentation, the speaker will introduce the most-recent developments made in Spallation Neutron Source (SNS)/High Flux Isotope Reactor (HFIR) of Oak Ridge National Laboratory, dedicating to realize operando neutron scattering characterizations for the study of LIBs.[2] Operando ND and NR will be discussed individually based on the distinct scientific questions they could address. [1] C. P. Grey; J. M. Tarascon, Sustainability and in situ monitoring in battery development, Nat. Mat., 2017, 16, 45–56. [2] B. H. Song, et al. Metastable Li1+δMn2O4 (0 ≤ δ ≤ 1) Spinel Phases Revealed by in Operando Neutron Diffraction and First-Principles Calculations, Chem. Mater. 2019, 31, 124−134.

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