{"title":"Hand-Held Nanoelectrospray Ionization with Frequency and Amplitude Tunability for Metabolomics of Saline Biosamples","authors":"Mengyang Song, Yuze Li*, Wenbo Ma, Junyu Chen* and Zongxiu Nie*, ","doi":"10.1021/acs.analchem.5c03797","DOIUrl":null,"url":null,"abstract":"<p >Pulsed nanoelectrospray ionization (nanoESI) mass spectrometry has been proven to have several merits compared to its direct current (DC) counterparts, such as high sensitivity, high matrix tolerance, and low electrochemical interference. However, the reliance on external devices like signal generators and power amplifiers limits the technology’s suitability for on-site use. Here, we developed a frequency-amplitude tunable hand-held pulsed high-voltage supply specifically designed for nanoESI. This portable detection system eliminates reliance on bulky ancillary equipment of conventional approaches, with a total mass of 185 g and an ergonomic hand-held configuration. Through systematic modulation of frequency (10–50 kHz) and voltage (1.5–6 kV), the device achieves optimal detection performance across diverse analytical standards and complex matrixes, including serum and cellular samples. The pulse-induced self-cleaning effect prevented nozzle clogging while maintaining functionality under high-salt conditions (855 mM NaCl). To demonstrate clinical applicability, we analyzed 198 serum specimens (100 from atherosclerotic cardiovascular disease patients (ASCVD) and 98 age-matched controls), identifying statistically significant dysregulation of multiple metabolites in the ASCVD cohort and achieving a diagnostic accuracy of 85%. Field deployment trials using portable mass spectrometers further validated the system’s potential for rapid on-site diagnostics, establishing a new paradigm for point-of-care analytical technology.</p>","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"97 33","pages":"18327–18334"},"PeriodicalIF":6.7000,"publicationDate":"2025-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Analytical Chemistry","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.analchem.5c03797","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Pulsed nanoelectrospray ionization (nanoESI) mass spectrometry has been proven to have several merits compared to its direct current (DC) counterparts, such as high sensitivity, high matrix tolerance, and low electrochemical interference. However, the reliance on external devices like signal generators and power amplifiers limits the technology’s suitability for on-site use. Here, we developed a frequency-amplitude tunable hand-held pulsed high-voltage supply specifically designed for nanoESI. This portable detection system eliminates reliance on bulky ancillary equipment of conventional approaches, with a total mass of 185 g and an ergonomic hand-held configuration. Through systematic modulation of frequency (10–50 kHz) and voltage (1.5–6 kV), the device achieves optimal detection performance across diverse analytical standards and complex matrixes, including serum and cellular samples. The pulse-induced self-cleaning effect prevented nozzle clogging while maintaining functionality under high-salt conditions (855 mM NaCl). To demonstrate clinical applicability, we analyzed 198 serum specimens (100 from atherosclerotic cardiovascular disease patients (ASCVD) and 98 age-matched controls), identifying statistically significant dysregulation of multiple metabolites in the ASCVD cohort and achieving a diagnostic accuracy of 85%. Field deployment trials using portable mass spectrometers further validated the system’s potential for rapid on-site diagnostics, establishing a new paradigm for point-of-care analytical technology.
脉冲纳米电喷雾质谱(nanoESI)与直流(DC)质谱相比,具有高灵敏度、高基质耐受性和低电化学干扰等优点。然而,对信号发生器和功率放大器等外部设备的依赖限制了该技术在现场使用的适用性。在这里,我们开发了一种专门为纳米esi设计的频率幅度可调手持式脉冲高压电源。这种便携式检测系统消除了对传统方法中笨重的辅助设备的依赖,其总质量为185克,具有符合人体工程学的手持配置。通过系统调制频率(10-50 kHz)和电压(1.5-6 kV),该设备在不同的分析标准和复杂的基质(包括血清和细胞样本)中实现最佳检测性能。脉冲诱导的自清洁效果防止了喷嘴堵塞,同时在高盐条件下(855 mM NaCl)保持了功能。为了证明临床适用性,我们分析了198份血清样本(100份来自动脉粥样硬化性心血管疾病(ASCVD)患者,98份来自年龄匹配的对照组),在ASCVD队列中发现了具有统计学意义的多种代谢物失调,诊断准确率达到85%。使用便携式质谱仪的现场部署试验进一步验证了该系统在快速现场诊断方面的潜力,为即时分析技术建立了新的范例。
期刊介绍:
Analytical Chemistry, a peer-reviewed research journal, focuses on disseminating new and original knowledge across all branches of analytical chemistry. Fundamental articles may explore general principles of chemical measurement science and need not directly address existing or potential analytical methodology. They can be entirely theoretical or report experimental results. Contributions may cover various phases of analytical operations, including sampling, bioanalysis, electrochemistry, mass spectrometry, microscale and nanoscale systems, environmental analysis, separations, spectroscopy, chemical reactions and selectivity, instrumentation, imaging, surface analysis, and data processing. Papers discussing known analytical methods should present a significant, original application of the method, a notable improvement, or results on an important analyte.