基于软电离质谱技术的金属纳米团簇合成、结构解析与催化反应机理研究的进展  

Recent Advances in Synthesis,Structure Analysis,and Catalytic Reaction Mechanism of Metal Nanoclusters Based on Soft Ionization Mass Spectrometry

作　　者：张丽丽 周健 房聪 孙晓岩 ZHANG Li-li;ZHOU Jian;FANG Cong;SUN Xiao-yan(Qingdao Institute of Bioenergy and Bioprocess Technology,Chinese Academy of Sciences,Qingdao 266101,China;University of Chinese Academy of Sciences,Beijing 100049,China;Shandong Energy Institute,Qingdao 266101,China;Qingdao New Energy Shandong Laboratory,Qingdao 266101,China)

机构地区：[1]中国科学院青岛生物能源与过程研究所,山东青岛266101 [2]中国科学院大学,北京100049 [3]山东能源研究院,山东青岛266101 [4]青岛新能源山东省实验室,山东青岛266101

出　　处：《质谱学报》2024年第1期69-89,I0003,共22页Journal of Chinese Mass Spectrometry Society

基　　金：山东省自然科学基金(ZR2021QB128,ZR2022MA040);山东能源研究院创新基金(SEII202122);山东省泰山学者青年专家计划(tsqn201909161);强基计划(QIBEBT S202306)。

摘　　要：原子数精确的金属纳米团簇为研究纳米材料的结构演化和构效关系提供了绝佳模型,然而,由于团簇生长过程的不确定性、结晶过程的复杂性以及自身稳定性较差等因素,使其在精准合成、结构解析以及催化机理研究方面面临挑战。质谱技术具有高分辨率、高灵敏度、快速响应的特性,尤其是结合软电离技术(主要包括电喷雾电离和基质辅助激光解吸电离),近年来在凝聚相团簇研究中发挥着重要作用。例如,通过监测中间体的变化可以解析团簇的生长过程,使用串联质谱技术可以推测团簇结构特征,利用离子-分子反应方法以及在线反应监测技术能够揭示催化反应微观机理等。本文主要总结了2种软电离质谱技术在金属团簇合成、结构解析以及催化反应机理研究的进展,并展望其应用前景。Metal nanoclusters(NCs)are stable aggregates at the molecular level,consisting of several to hundreds of metal atoms bound together by physical or chemical interaction.These nanoclusters exhibit unique physicochemical properties that have garnered significant attention in various fields,including biology,catalysis,sensing,and drug delivery.In the field of catalytic reactions,atomically precise metal nanoclusters have acted as an archetypical model for elucidating the structural evolution and structure-property relationship of nanomaterials.However,due to the factors such as the uncertainty of the growth mechanism,the complexity of the crystallization process,and the inherent poor stability,the cluster research faces some challenges in the precise synthesis,structural analysis as well as the comprehension of catalytic reaction mechanism which hinder the full exploration and understanding of these fascinating properties of clusters.Recent years,mass spectrometry(MS)has emerged as a crucial tool in biomolecular analysis and the detection of organic reaction intermediates due to its high sensitivity,high resolution,and fast response.In cluster chemistry,the researchers have also introduced this technique into the study of metal nanoclusters with precise atomic numbers,which have played an important role in the synthesis of clusters and the analysis of their structures as well as reaction mechanisms.The ion source,as the"heart"of the MS,can ionize the analyte and then be detected by MS.Currently,the main ionization methods used for cluster analysis are electrospray ionization(ESI)and matrix-assisted laser desorption/ionization(MALDI).These two"soft"ionization techniques can obtain the quasi-molecular ion peaks of the clusters without destroying the structure of the clusters,thus determining the composition of the clusters.In addition,MS enables real-time characterization of the reaction process in solution,allowing for online monitoring of complex reaction components,providing an experimental basis for synthesis proce

关 键 词：金属纳米团簇 质谱 实时监测 反应中间体 

分 类 号：O657.63[理学—分析化学]