Abstract

The hierarchical control in biogenic minerals, from precise nanomorphology control to subsequent macroscopic assembly, remains a formidable challenge in artificial synthesis. Studies in biomineralization, however, are largely limited to atomicandmolecular scale crystallization, devoting little attention to biomolecular higher-order structures (HOSs) which critically impact long-range assembly of biominerals. Here we demonstrate a biomimetic route and quantitative simulationsthat explore peptide HOSs on guiding nanocrystal formation and anisotropic assembly into hierarchical structures. It is found that thePt{100}-specific peptide T7 (Ac-TLTTLTN-CONH2) adopts ST-turnsecondary structure, promoting cubic Pt nanocrystal formation at low concentration, and spontaneously transforms into a β-sheet with increased concentration. The β-sheet T7-Pt{100} specificity drives cubic Pt nanocrystals to self-assemble into large-area, long-range, [100] linear assemblies. This study provides a robust demonstration for bio/nonbiogenic material specificity, nanoscale synthesis, and long-range self-organization with biomolecular HOSs and opens vast opportunities for multiscale programmable structures.

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