Giving Gold Wings: Ultrabright and Fragmentation Free Mass Spectrometry Reporters for Barcoding, Bioconjugation Monitoring, and Data Storage
Giving Gold Wings: Ultrabright and Fragmentation Free Mass Spectrometry Reporters for Barcoding, Bioconjugation Monitoring, and Data Storage
复制标题
赋予金翼：用于条形码、生物共轭监测和数据存储的超亮、无碎片质谱报告仪
DOI：
10.1002/anie.202219182
复制
发表时间：
2023
期刊：
影响因子：
--
通讯作者：
Camden, Jon P.
中科院分区：
文献类型：
--
作者：
Dominique, Nathaniel L.;Jensen, Isabel M.;Kaur, Gurkiran;Kotseos, Chandler Q.;Boggess, William C.;Jenkins, David M.;Camden, Jon P.
激光解吸/电离质谱（LDI - MS）的广泛应用突出了对明亮和可复用的标记平台的需求。虽然配体覆盖的Au纳米颗粒（AuNPs）已经成为一种很有前途的LDI - MS造影剂，但主要的硫醇配体存在离子产率低和广泛断裂的问题。在这项工作中，我们开发了一个N -杂环碳（NHC）配体平台，提高了AuNP LDI - MS的性能。NHC支架被调整为产生条形码AuNPs，当与硫醇- AuNPs作为基准时，它是明亮的质量标签，并在高产率下形成不破碎的离子。为了说明NHC配体的转化潜力，质量标签被用于三个正交应用：监测生物偶联反应，执行多路成像，存储和读取编码信息。这些结果表明，NHC -纳米颗粒系统是LDI - MS的理想平台，大大拓宽了纳米颗粒造影剂的范围。
The widespread application of laser desorption/ionization mass spectrometry (LDI‐MS) highlights the need for a bright and multiplexable labeling platform. While ligand‐capped Au nanoparticles (AuNPs) have emerged as a promising LDI‐MS contrast agent, the predominant thiol ligands suffer from low ion yields and extensive fragmentation. In this work, we develop a N‐heterocyclic carbene (NHC) ligand platform that enhances AuNP LDI‐MS performance. NHC scaffolds are tuned to generate barcoded AuNPs which, when benchmarked against thiol‐AuNPs, are bright mass tags and form unfragmented ions in high yield. To illustrate the transformative potential of NHC ligands, the mass tags were employed in three orthogonal applications: monitoring a bioconjugation reaction, performing multiplexed imaging, and storing and reading encoded information. These results demonstrate that NHC‐nanoparticle systems are an ideal platform for LDI‐MS and greatly broaden the scope of nanoparticle contrast agents.