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Wang, Congcheng; Jeong, Won_Joon; Nelson, Douglas_Lars; Sridhara, Hari; Anderson, Sophia_Nicolette; McDowell, Matthew_T (, Advanced Materials)Abstract Solid‐state batteries with alloy‐type negative electrodes can feature enhanced energy density and safety compared to conventional Li‐ion batteries. However, diffusional Li trapping within Li alloys often causes low initial Coulombic efficiency and leads to capacity loss with cycling. Here, a general roll‐pressing prelithiation method compatible with a variety of alloy‐type negative electrodes (silicon, aluminum, tin, and multi‐phase alloys) is introduced, which is shown to improve performance in solid‐state batteries. By warm‐rolling lithium foil of controlled thickness with various alloy‐type electrodes, both slurry‐cast and foil‐type electrodes can be uniformly prelithiated via direct chemical reaction. The prelithiated electrodes exhibit enhanced specific capacity and extended cycle life in batteries with Li6PS5Cl solid‐state electrolyte. Prelithiated multi‐phase foil electrodes with a tailored interface are shown to exhibit superior cycling stability down to 2 MPa stack pressure. This prelithiation technique offers a pathway to overcome intrinsic challenges in alloy anodes for solid‐state batteries.more » « less
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Chin, Jonathan_R; Gardner, Bonnie_G; Frye, Marshall_B; Liu, Derrick_S-H; Marini, Sebastian_A; Shallenberger, Jeffrey; McDowell, Matthew_T; Hilse, Maria; Law, Stephanie; Garten, Lauren_M (, MRS Communications)Abstract Understanding surface stability becomes critical as 2D materials like SnSe are developed for piezoelectric and optical applications. SnSe thin films deposited by molecular beam epitaxy showed no structural changes after a two-year exposure to atmosphere, as confirmed by X-ray diffraction and Raman spectroscopy. X-ray photoelectron spectroscopy and reflectivity show a stable 3.5 nm surface oxide layer, indicating a self-arresting oxidative process. Resistivity measurements show an electrical response dominated by SnSe post-exposure. This work shows that SnSe films can be used in ambient conditions with minimal risk of long-term degradation, which is critical for the development of piezoelectric or photovoltaic devices. Graphical Abstractmore » « less
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Jeong, Won_Joon; Wang, Congcheng; Yoon, Sun_Geun; Liu, Yuhgene; Chen, Timothy; McDowell, Matthew_T (, ACS Energy Letters)
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