doi:10.1038/s43246-021-00119-0engHaro, M.Kumar, P.Zhao, J.L.Koutsogiannis, P.Porkovich, A.J.Ziadi, Z.Bouloumis, T.Singh, V.Juarez-Perez, E.J.Toulkeridou, E.Nordlund, K.Djurabekova, F.Sowwan, M.Grammatikopoulos, P.Nano-vault architecture mitigates stress in silicon-based anodes for lithium-ion batteriesART-2021-124030Nanomaterials undergoing cyclic swelling-deswelling benefit from inner void spaces that help accommodate significant volumetric changes. Such flexibility, however, typically comes at a price of reduced mechanical stability, which leads to component deterioration and, eventually, failure. Here, we identify an optimised building block for silicon-based lithium-ion battery (LIB) anodes, fabricate it with a ligand- and effluent-free cluster beam deposition method, and investigate its robustness by atomistic computer simulations. A columnar amorphous-silicon film was grown on a tantalum-nanoparticle scaffold due to its shadowing effect. PeakForce quantitative nanomechanical mapping revealed a critical change in mechanical behaviour when columns touched forming a vaulted structure. The resulting maximisation of measured elastic modulus (similar to 120GPa) is ascribed to arch action, a well-known civil engineering concept. The vaulted nanostructure displays a sealed surface resistant to deformation that results in reduced electrode-electrolyte interface and increased Coulombic efficiency. More importantly, its vertical repetition in a double-layered aqueduct-like structure improves both the capacity retention and Coulombic efficiency of the LIB. Lithiation of anodes during cycling of lithium-ion batteries generates stresses that reduce operation lifetime. Here, a composite silicon-based anode with a nanoscale vaulted architecture shows high mechanical stability and electrochemical performance in a lithium-ion battery.2021http://zaguan.unizar.es/record/14524410.1038/s43246-021-00119-0http://zaguan.unizar.es/record/145244oai:zaguan.unizar.es:145244info:eu-repo/grantAgreement/ES/MICINN/PID2019-108247RA-I00info:eu-repo/grantAgreement/ES/MICINN/RYC-2018-025222-ICommunications materials 2, 1 (2021), 16 [10 pp]byhttp://creativecommons.org/licenses/by/3.0/es/info:eu-repo/semantics/openAccess