Modulating the Electromechanical Response of Bio-Inspired Amino Acid-Based Architectures through Supramolecular Co-Assembly

Wei Ji*, Bin Xue, Yuanyuan Yin, Sarah Guerin, Yuehui Wang, Lei Zhang, Yuanqi Cheng, Linda J.W. Shimon, Yu Chen*, Damien Thompson*, Rusen Yang, Yi Cao, Wei Wang, Kaiyong Cai, Ehud Gazit*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

19 Scopus citations

Abstract

Supramolecular packing dictates the physical properties of bio-inspired molecular assemblies in the solid state. Yet, modulating the stacking modes of bio-inspired supramolecular assemblies remains a challenge and the structure-property relationship is still not fully understood, which hampers the rational design of molecular structures to fabricate materials with desired properties. Herein, we present a co-assembly strategy to modulate the supramolecular packing of N-terminally capped alanine-based assemblies (Ac-Ala) by changing the amino acid chirality and mixing with a nonchiral bipyridine derivative (BPA). The co-assembly induced distinct solid-state stacking modes determined by X-ray crystallography, resulting in significantly enhanced electromechanical properties of the assembly architectures. The highest rigidity was observed after the co-assembly of racemic Ac-Ala with a bipyridine coformer (BPA/Ac-DL-Ala), which exhibited a measured Young's modulus of 38.8 GPa. Notably, BPA crystallizes in a centrosymmetric space group, a condition that is broken when co-crystallized with Ac-L-Ala and Ac-D-Ala to induce a piezoelectric response. Enantiopure co-assemblies of BPA/Ac-D-Ala and BPA/Ac-L-Ala showed density functional theory-predicted piezoelectric responses that are remarkably higher than the other assemblies due to the increased polarization of their supramolecular packing. This is the first report of a centrosymmetric-crystallizing coformer which increases the single-crystal piezoelectric response of an electrically active bio-inspired molecular assembly. The design rules that emerge from this investigation of chemically complex co-assemblies can facilitate the molecular design of high-performance functional materials comprised of bio-inspired building blocks.

Original languageEnglish
Pages (from-to)18375-18386
Number of pages12
JournalJournal of the American Chemical Society
Volume144
Issue number40
DOIs
StatePublished - 12 Oct 2022

Funding

FundersFunder number
Higher
Joint NSFC-ISF3145/19, 11804148
European Commission
Science Foundation Ireland12/RC/2275 P2
National Natural Science Foundation of China52103148
Chongqing University
Natural Science Foundation of Jiangsu ProvinceBK20180320, 020414380187
Fundamental Research Funds for the Central Universitiescx2021055, 2022CDJXY-026, 2021CDJQY-021
Irish Centre for High-End Computing21/PATH-S/9737

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