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

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

作者地址："[Ji, Wei; Wang, Yuehui; Cai, Kaiyong] Chongqing Univ, Coll Bioengn, Key Lab Biorheol Sci & Technol, Minist Educ, Chongqing 400044, Peoples R China; [Xue, Bin; Cheng, Yuanqi; Cao, Yi; Wang, Wei] Nanjing Univ, Dept Phys, Natl Lab Solid State Microstruct, Nanjing 210093, Jiangsu, Peoples R China; [Yin, Yuanyuan] Chongqing Med Univ, Stomatol Hosp, Chongqing Key Lab Oral Dis & Biomed Sci, Chongqing Municipal Key Lab Oral Biomed Engn High, Chongqing 401147, Peoples R China; [Guerin, Sarah; Thompson, Damien] Univ Limerick, Bernal Inst, Dept Phys, Limerick V94 T9PX, Ireland; [Zhang, Lei] CAEP Software Ctr High Performance Numer Simulat, Beijing 100088, Peoples R China; [Shimon, Linda J. W.] Weizmann Inst Sci, Dept Chem Res Support, IL-76100 Rehovot, Israel; [Chen, Yu; Gazit, Ehud] Tel Aviv Univ, Shmunis Sch Biomedicine & Canc Res, George S Wise Fac Life Sci, IL-6997801 Tel Aviv, Israel; [Yang, Rusen] Xidian Univ, Sch Adv Mat & Nanotechnol, Xian 710126, Peoples R China"

通信作者："Ji, W (通讯作者)，Chongqing Univ, Coll Bioengn, Key Lab Biorheol Sci & Technol, Minist Educ, Chongqing 400044, Peoples R China.; Thompson, D (通讯作者)，Univ Limerick, Bernal Inst, Dept Phys, Limerick V94 T9PX, Ireland.; Chen, Y; Gazit, E (通讯作者)，Tel Aviv Univ, Shmunis Sch Biomedicine & Canc Res, George S Wise Fac Life Sci, IL-6997801 Tel Aviv, Israel."

来源：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

ESI学科分类：CHEMISTRY

WOS号：WOS:000867392000001

JCR分区：Q1

影响因子：15

年份：2022

卷号：　

期号：　

开始页：　

结束页：　

文献类型：Article; Early Access

关键词：　

摘要："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."

基金机构："National Natural Science Foundation of China [11804148, 52103148]; Fundamental Research Funds for the Central Universities [020414380187, 2021CDJQY-021, 2022CDJXY-026]; Chongqing University; Joint NSFC-ISF Grant [3145/19]; Natural Science Foundation of Jiangsu province [BK20180320]; Science Foundation Ireland (SFI) [12/RC/2275 P2]; Science Foundation Ireland [21/PATH-S/9737]; European Union; Returning Overseas Scholar Innovation Program [cx2021055]"

基金资助正文："This work was supported by the National Natural Science Foundation of China (No. 52103148) (W.J.), the Fundamental Research Funds for the Central Universities (No. 2021CDJQY-021 and 2022CDJXY-026) (W.J.), Returning Overseas Scholar Innovation Program (cx2021055) (W.J.), the Start-up Funding from Chongqing University (W.J.), Joint NSFC-ISF Grant (No. 3145/19) (E.G.), the National Natural Science Foundation of China (No. 11804148) (B.X.), the Natural Science Foundation of Jiangsu province (No. BK20180320) (B.X.), the Fundamental Research Funds for the Central Universities (No. 020414380187) (B.X.), Science Foundation Ireland (SFI) under award number 12/RC/2275 P2 (D.T. and S.G.), and supercomputing resources to S.G. and D.T. at the SFI/Higher Education Authority Irish Center for High-End Computing (ICHEC). S.G. would like to acknowledge funding from Science Foundation Ireland under grant number 21/PATH-S/9737. S.G. is funded by the European Union. Views and opinions expressed are however those of the author only and do not necessarily reflect those of the European Union or the European Research Council. Neither the European Union nor the granting authority can be held responsible for them. The authors thank Dr. Sigal Rencus Lazar and Ms. Yin Chen for manuscript editing and graphical assistance and Ms. Ranran Jiao for thermal stability experimental assistance."