New Wine in Old Bottle: Crown Ether-Functionalized Digital Polymer toward Efficient MALDI-TOF MS/MS Decoding via a Classical Supramolecular Interaction,ACS Macro Letters

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New Wine in Old Bottle: Crown Ether-Functionalized Digital Polymer toward Efficient MALDI-TOF MS/MS Decoding via a Classical Supramolecular Interaction
ACS Macro Letters ( IF 5.1 ) Pub Date : 2024-07-23 , DOI: 10.1021/acsmacrolett.4c00360
Xiaoman Huang ₁ , Zhilin Yang _{1,

2} , Xiaojie Yang ₁ , Zhishan Liang ₁ , Qinmeng Zhong ₁ , Lihua Hu ₃ , Zhihao Huang _{1,

4} , Zhengbiao Zhang _{1,

5}

Affiliation

Digital polymers (DPs), which serve as promising molecular-level storage media, have increasingly garnered interest. Their application significantly depends on the efficiency of the information writing (synthesis) and reading processes (sequencing). For reading, rational incorporation of weak bonds in the main chain was applied in most cases in order to improve readability of the tandem mass spectra (MS/MS), which would limit the chain length of DPs, thus reducing the information storage capacity. In this study, the introduction of commercially available crown ether (CE) at the terminus of digital oligo(γ-butyrolactone)s (DOBLs) significantly enhances the predictability and fidelity of matrix-assisted laser desorption/ionization time-of-flight tandem mass spectra (MALDI-TOF MS/MS), thus improving the decoding process. The use of crown ether, leveraging a well-established supramolecular interaction with alkali cations known since 1967, offers a strong affinity between ionization agents and CE motifs, to form a selective effect of the desired fragments during the tandem MS. This method is particularly effective for long-chain DPs, extending up to 32-mer, and allows for customizable fragmentation patterns. The incorporation of CE at the DP chain end presents a novel and efficient strategy for enhancing MS/MS readability and amplifying the information storage capacity of polymers.

中文翻译：

新瓶装新酒：冠醚功能化数字聚合物通过经典超分子相互作用实现高效 MALDI-TOF MS/MS 解码

数字聚合物（DP）作为有前途的分子级存储介质，越来越引起人们的兴趣。它们的应用很大程度上取决于信息写入（合成）和读取过程（排序）的效率。在读取方面，大多数情况下会在主链中合理掺入弱键，以提高串联质谱（MS/MS）的可读性，但这会限制DP的链长，从而降低信息存储容量。在这项研究中，在数字寡聚（γ-丁内酯）（DOBL）末端引入市售冠醚（CE）显着增强了基质辅助激光解吸/电离飞行时间串联质量的可预测性和保真度谱（MALDI-TOF MS/MS），从而改进解码过程。使用冠醚，利用自 1967 年以来已知的与碱金属阳离子的超分子相互作用，在电离剂和 CE 基序之间提供强大的亲和力，在串联 MS 过程中形成所需片段的选择性效应。该方法对于长链 DP 特别有效，可延伸至 32 聚体，并允许定制片段模式。在 DP 链末端掺入 CE 为增强 MS/MS 可读性和放大聚合物的信息存储能力提供了一种新颖有效的策略。

更新日期：2024-07-23

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