A Modular Solid Phase Synthesis Approach for Glycocalix[4]Arene Derivatives and Their Multivalent Presentation on Ultrasmall Gold Nanoparticles

一种用于合成糖萼[4]芳烃衍生物的模块化固相合成方法及其在超小金纳米粒子上的多价化表征

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Abstract

Gold nanoparticles and calix[n]arenes are well-established platforms for creating multivalent carbohydrate ligands that enhance binding avidity and selectivity toward carbohydrate-recognizing receptors, such as bacterial lectins. In this study, we present a modular synthesis protocol for tailor-made and (multi)functional glycocalix[4]arene derivatives using solid-phase polymer synthesis. A calix[4]arene building block with a single carboxyl group on the lower rim and four nitro groups at the upper rim is introduced. This building block is attached to a solid support using standard solid phase peptide coupling conditions, followed by reduction of the upper rim nitro functionalities to yield four amine groups, that are further functionalized through solid-phase polymer synthesis. Using this modular approach, we access a series of glyco-calix[4]arene structures that are then further conjugated onto ultrasmall gold nanoparticles. Conjugation is promoted either via one or via four alkyne groups on the glycocalixarene structure, providing a handle to tune the overall valency of the final glyco[4]calixarene-gold nanoparticle conjugates. Finally, the glycocalix[4]arene derivatives and conjugates are evaluated for their inhibitory potential against bacterial adhesion showing the importance of multivalent carbohydrate presentation to effectively block Escherichia coli (E. coli) adhesion.

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