Pei Jingxuan, Zhao Yanfang, Zhang Shuting, Yu Xiang, Tian Zhenfei, Sun Yibo, Ma Shiqing, Zhao Ru-Song, Meng Jianping, Chen Xiangfeng, Chen Fang
Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources, Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, School of Materials Science and Technology, China University of Geosciences (Beijing), Beijing 100083, China.
Shandong Analysis and Test Center, Key Laboratory for Applied Technology of Sophisticated Analytical Instruments of Shandong Province, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250014, China.
ACS Appl Mater Interfaces. 2023 Oct 31. doi: 10.1021/acsami.3c08962.
The development of the valid strategy to enhance laser desorption/ionization efficiency gives rise to widespread concern in surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) technology. Herein, a hybrid of Au NP-decorated graphdiyne (Au/GDY) was fabricated and employed as the SALDI-MS matrix for the first time, and a mechanism based on photothermal and photochemical energy conversions was proposed to understand LDI processes. Given theoretical simulations and microstructure characterizations, it was revealed that the formation of a coupled thermal field and internal electric field endow the as-prepared Au/GDY matrix with superior desorption and ionization efficiency, respectively. Moreover, laser-induced matrix ablation introduced strain and defect level into the Au/GDY hybrid, suppressing the recombination of charge carriers and thereby facilitating analyte ionization. The optimized Au/GDY matrix allowed for reliable detection of trace sulfacetamide and visualization of exogenous/endogenous components in biological tissues. This work offers an integrated solution to promote LDI efficiency based on collaborative photothermal conversion and internal electric field, and may inspire the design of novel semiconductor-based surface matrices.
开发有效的策略以提高激光解吸/电离效率在表面辅助激光解吸/电离质谱(SALDI-MS)技术中引起了广泛关注。在此,首次制备了金纳米粒子修饰的石墨炔(Au/GDY)复合材料并将其用作SALDI-MS基质,并提出了一种基于光热和光化学能量转换的机制来理解激光解吸电离过程。通过理论模拟和微观结构表征发现,耦合热场和内部电场的形成分别赋予了所制备的Au/GDY基质优异的解吸和电离效率。此外,激光诱导的基质烧蚀在Au/GDY复合材料中引入了应变和缺陷能级,抑制了电荷载流子的复合,从而促进了分析物的电离。优化后的Au/GDY基质能够可靠地检测痕量磺胺醋酰,并可视化生物组织中的外源性/内源性成分。这项工作基于协同光热转换和内部电场提供了一种提高激光解吸电离效率的综合解决方案,并可能启发新型半导体基表面基质的设计。