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A significant challenge in creating supramolecular materials is that conjugating molecular functionalities to building blocks often results in dissociation or undesired morphological transformation of their assemblies. Here we present a facile strategy to preserve structurally labile peptide assemblies after molecular modification of the self‐assembling peptides. Sheet‐forming peptides are designed to afford a staggered alignment with the segments bearing chemical modification sites protruding from the sheet surfaces. The staggered assembly allows for simultaneous separation of attached molecules from each other and from the underlying assembly motifs. Strikingly, using PEGs as the external molecules, PEG400‐ and PEG700‐peptide conjugates directly self‐associate into nanosheets with the PEG chains localized on the sheet surfaces. In contrast, the sheet formation based on in‐register lateral packing of peptides does not recur upon the peptide PEGylation. This strategy allows for fabrication of densely modified assemblies with a variety of molecules, as demonstrated using biotin (hydrophobic molecule), c(RGDfK) (cyclic pentapeptide), and nucleic acid aptamer (negatively charged ssDNA). The staggered co‐assembly also enables extended tunability of the amount/density of surface molecules, as exemplified by screening ligand‐appended assemblies for cell targeting. This study paves the way for functionalization of historically challenging fragile assemblies while maintaining their overall morphology. [ABSTRACT FROM AUTHOR]

Constructing stable electrode/electrolyte interphase with fast interfacial kinetics is vital for fast‐charging batteries. Herein, we investigate the interphase that forms between a high‐voltage Na3V2(PO4)2F3 cathode and the electrolytes consisting of 3.0, 1.0, or 0.3 M NaClO4 in an organic carbonate solvent (47.5 : 47.5 : 5 mixture of EC: PC: FEC) during charging up to 4.5 V at 55 °C. It is found that a higher anion/solvent ratio in electrolyte solvation structure induces anion‐dominated interphase containing more inorganic species and more anion derivatives (CxClOy), which leads to a larger interfacial Na+ transport resistance and more unfavorable gas evolution. In comparison, a low anion/solvent ratio derives stable anion‐tuned interphase that enables better interfacial kinetics and cycle ability. Importantly, the performance of a failed cathode is restored by triggering the decomposition of CxClOy species. This work elucidates the role of tuning interphase in fast‐charging batteries. [ABSTRACT FROM AUTHOR]

Rücktitelbild: Naphthodithiophene Diimide Based Chiral -Conjugated Nanopillar Molecules (Angew. Keywords: conjugation; cycloparaphenylenes; macrocycles; nanopillar molecules; naphthodithiophene diimide EN conjugation cycloparaphenylenes macrocycles nanopillar molecules naphthodithiophene diimide 24932 24932 1 11/02/21 20211108 NES 211108 B Chirale I i -konjugierte Nanosäulenmoleküle b auf der Basis von Naphthodithiophen-Diimid zeichnen sich durch eine starre Säulenform und eine Fülle einzigartiger optischer und chiraler Eigenschaften aus, die sie zu idealen Bausteinen für den Aufbau wichtiger supramolekularer 2D-Architekturen machen. Conjugation, cycloparaphenylenes, macrocycles, nanopillar molecules, naphthodithiophene diimide. [Extracted from the article]