Department of Biochemistry, University of California, Riverside, CA 92521, USA.
Department of Bioengineering, University of California, Riverside, CA 92521, USA.
Biomolecules. 2021 Mar 15;11(3):429. doi: 10.3390/biom11030429.
Biological structure-function relationships offer incomparable paradigms for charge-transfer (CT) science and its implementation in solar-energy engineering, organic electronics, and photonics. Electrets are systems with co-directionally oriented electric dopes with immense importance for CT science, and bioinspired molecular electrets are polyamides of anthranilic-acid derivatives with designs originating from natural biomolecular motifs. This publication focuses on the synthesis of molecular electrets with ether substituents. As important as ether electret residues are for transferring holes under relatively high potentials, the synthesis of their precursors presents formidable challenges. Each residue in the molecular electrets is introduced as its 2-nitrobenzoic acid (NBA) derivative. Hence, robust and scalable synthesis of ether derivatives of NBA is essential for making such hole-transfer molecular electrets. Purdie-Irvine alkylation, using silver oxide, produces with 90% yield the esters of the NBA building block for iso-butyl ether electrets. It warrants additional ester hydrolysis for obtaining the desired NBA precursor. Conversely, Williamson etherification selectively produces the same free-acid ether derivative in one-pot reaction, but a 40% yield. The high yields of Purdie-Irvine alkylation and the selectivity of the Williamson etherification provide important guidelines for synthesizing building blocks for bioinspired molecular electrets and a wide range of other complex ether conjugates.
生物结构-功能关系为电荷转移(CT)科学及其在太阳能工程、有机电子学和光子学中的应用提供了无与伦比的范例。电纺丝是具有同向定向电掺杂的系统,对 CT 科学具有重要意义,而仿生分子电纺丝是源自天然生物分子基序的邻苯二甲酸二酰胺的聚酰胺。本出版物重点介绍了带有醚取代基的分子电纺丝的合成。醚电纺丝残基在相对较高的电位下转移空穴非常重要,但其前体的合成具有巨大的挑战。分子电纺丝中的每个残基都以其 2-硝基苯甲酸(NBA)衍生物的形式引入。因此,醚衍生物的稳健和可扩展合成对于制造这种空穴转移分子电纺丝至关重要。使用氧化银的 Purdie-Irvine 烷基化以 90%的产率产生用于异丁基醚电纺丝的 NBA 构建块的酯。它需要额外的酯水解以获得所需的 NBA 前体。相反,Williamson 醚化在一锅反应中选择性地生成相同的游离酸醚衍生物,但产率为 40%。Purdie-Irvine 烷基化的高收率和 Williamson 醚化的选择性为合成仿生分子电纺丝和广泛的其他复杂醚缀合物的构建块提供了重要的指导方针。