Forster, Alexander Zhang, Jinsong Fadillah, Laras Braks, Leonie Fu, Tingting El Kazzi, Mario Choi, Jang Wook Coskun, Ali 2025 Despite their improved safety, high energy density when paired with Li metal anode, all-solid-state batteries (ASSBs) continue to face significant challenges, notably the interface with the cathode active material (CAM), which is prone to both physical and (electro-)chemical degradation during cycling, especially when employing high-Ni CAMs. To address this issue, here, we introduced an organic surface anchoring strategy to stabilize the CAM surface and CAM-solid electrolyte interface using trifluoroacetamide (TFAA). A weak acid-base interaction between the CAM and TFAA creates a passivating layer, incorporating in-situ generated LiF, as a highly competitive alternative to conventional sol-gel-applied inorganic coating, i.e., LiNbO3 (LNO). Comparative electrochemical and physicochemical characterization of pristine, LNO-coated, and TFAA-coated NMC811 verified the efficiency of the organic anchoring strategy. Furthermore, we observed significant suppression in the formation of POx, SOx, and P-Sn-P species, indicating efficient mitigation of the (electro-)chemical oxidation of LPSCl at the interface, thus enabling an improved capacity retention of 95% after 100 cycles at 0.1 C. application/pdf https://folia.unifr.ch/global/documents/333350 https://folia.unifr.ch/documents/333350/files/manuscript.pdf eng info:eu-repo/semantics/altIdentifier/doi/10.1021/acsenergylett.5c02831 info:eu-repo/semantics/openAccess License undefined ACS Energy Letters. - 2025 All Solid State batteries Solid Electrolyte Organic coating Supramolecular Chemistry info:eu-repo/classification/udc/54 Molecular surface coating of high-voltage cathodes in LPSCl-based all-solid-state lithium metal batteries http://purl.org/coar/resource_type/c_6501