Exhaled breath analysis in patients with potentially curative lung cancer undergoing surgery: a longitudinal study
Jonas Herth, Felix Schmidt, Sarah Basler, Noriane A Sievi and Malcolm Kohler
Exhaled breath analysis has emerged as a non-invasive and promising method for early detection of lung cancer, offering a novel approach for diagnosis through the identification of specific biomarkers present in a patient's breath…
Alternative electrolyte solutions for untargeted breath metabolomics using secondary-electrospray ionization high-resolution mass spectrometry
Cedric Wüthrich, Renato Zenobi, Stamatios Giannoukos
Rationale
Secondary-electrospray ionization (SESI) coupled with high-resolution mass spectrometry is a powerful tool for the discovery of biomarkers in exhaled breath. A primary electrospray consisting of aqueous formic acid (FA) is currently used to charge the volatile organic compounds in breath. To investigate whether alternate electrospray compositions could enable different metabolite coverage and sensitivities, the electrospray dopants NaI and AgNO3 were tested….
Advances in secondary electrospray ionization for breath analysis and volatilomics
Stamatios Giannoukos, Cedric Wüthrich
The measurement of volatile organic compounds (VOCs) originating from organisms allows continuous monitoring and a unique insight into the metabolism. One method offering the sensitivity to detect these VOCs is secondary electrospray ionization coupled to high-resolution mass spectrometry (SESI-HRMS). SESI was derived from electrospray ionization (ESI) and has found widespread application in clinical research and monitoring of animals. This review discusses the technical aspects behind SESI, the advancements, and the technical hurdles faced. Additionally, the recent advances in the applications of SESI in human and animal-centered research are presented.
Preservation of exhaled breath samples for analysis by off-line SESI-HRMS: proof-of-concept study
Rosa A Sola-Martínez, Jiafa Zeng, Mo Awchi, Amanda Gisler, Kim Arnold, Kapil Dev Singh, Urs Frey, Manuel Cánovas Díaz, Teresa de Diego Puente, Pablo Sinues
Secondary electrospray ionization-high resolution mass spectrometry (SESI-HRMS) is an established technique in the field of breath analysis characterized by its short analysis time, as well as high levels of sensitivity and selectivity. Traditionally, SESI-HRMS has been used for real-time breath analysis, which requires subjects to be at the location of the analytical platform. Therefore, it limits the possibilities for an introduction of this methodology in day-to-day clinical practice. However, recent methodological developments have shown feasibility on the remote sampling of exhaled breath in Nalophan® bags prior to measurement using SESI-HRMS…
Elucidating the Role of Ion Suppression in Secondary Electrospray Ionization
Cedric Wüthrich, Stamatios Giannoukos, Renato Zenobi
Ion suppression is a known matrix effect in electrospray ionization (ESI), ambient pressure chemical ionization (APCI), and desorption electrospray ionization (DESI), but its characterization in secondary electrospray ionization (SESI) is lacking. A thorough understanding of this effect is crucial for quantitative applications of SESI, such as breath analysis. In this study, gas standards were generated by using an evaporation-based system to assess the susceptibility and suppression potential of acetone, deuterated acetone, deuterated acetic acid, and pyridine. Gas-phase effects were found to dominate ion suppression, with pyridine exhibiting the most significant suppressive effect, which is potentially linked to its gas-phase basicity. The impact of increased acetone levels on the volatiles from exhaled breath condensate was also examined…
Direct Mass Spectrometric Analysis of Exhaled Breath: Advances towards Clinical Application
Bettina Streckenbach
Metabolomics, or the comprehensive study of metabolites and involved processes, provides insights into the current physiological state of humans. In the clinical setting, the detection and quantification of specific metabolites has proven to be invaluable in diagnostic testing. Herein, body samples that are non-invasively accessible are of particular interest…
New Insights into Online Molecular Characterization of Organic Aerosol in China Using Extractive Electrospray Ionization and Ultrahigh Resolution Mass Spectrometry (EESI-Orbitrap)
Qi, Lu ; Lee Chuan, Ping ; Giannoukos, Stamatios ; Wang, Dongyu ; Li, Zhiyu ; Ran, Weikang ; Ye, Penglin ; Wang, Liwei ; Wang, Meng ; Lin, Yue ; Han, Yuemei ; Wang, Qiyuan ; Baltensperger, Urs ; El-Haddad, Imad ; Cao, Junji ; Prevot, Andre; Slowik, Jay
Despite extensive study, the sources and processes governing the formation and chemical evolution of haze pollution episodes in urban China remain unclear. Real-time molecular characterization of organic aerosol (OA) represents a promising approach to this problem. Extractive electrospray ionization (EESI) mass spectrometry allows real-time detection of individual OA components, while avoiding thermal decomposition and ionization-induced fragmentation. In previous field measurements, the EESI source was coupled with time-of-flight (TOF) mass analyzers, which are limited to a mass resolution of ~12,000 (at 200 m/z)…
High-frequency gaseous and particulate chemical characterization using extractive electrospray ionization mass spectrometry (Dual-Phase-EESI-TOF)
Chuan Ping Lee, Mihnea Surdu, David M. Bell, Josef Dommen, Mao Xiao, Xueqin Zhou, Andrea Baccarini, Stamatios Giannoukos, Günther Wehrle, Pascal André Schneider, Andre S. H. Prevot, Jay G. Slowik, Houssni Lamkaddam, Dongyu Wang, Urs Baltensperger, and Imad El Haddad
To elucidate the sources and chemical reaction pathways of organic vapors and particulate matter in the ambient atmosphere, real-time detection of both the gas and particle phase is needed. State-of-the-art techniques often suffer from thermal decomposition, ionization-induced fragmentation, high cut-off size of aerosols or low time resolution. In response to all these limitations, we developed a new technique that uses extractive electrospray ionization (EESI) for online gas and particle chemical speciation, namely the dual-phase extractive electrospray ionization time-of-flight mass spectrometer (Dual-Phase-EESI-TOF or Dual-EESI for short)….
Detection of trace metals in biogas using extractive electrospray ionization high-resolution mass spectrometry
Stamatios Giannoukos, Mohamed Tarik, Christian Ludwig, Serge Biollaz, Jay Slowik, Urs Baltensperger, Andre Stephan Henry Prevot
On-line measurements of metal emissions in energy conversion systems at very low concentrations are difficult to perform using existing techniques. Metals are of high importance due to their detrimental impact on human health, the environment and various industrial processes and/or equipment. Herewith and for the first time, we report the real-time detection and characterization of metals and trace elements in a Swiss biogas production plant using a novel technology based on an extractive electrospray ionization (EESI) source coupled to a high-resolution time-of-flight mass spectrometer (TOF-MS)…
Real-Time Detection of Aerosol Metals Using Online Extractive Electrospray Ionization Mass Spectrometry
Stamatios Giannoukos, Chuan Ping Lee, Mohamed Tarik, Christian Ludwig, Serge Biollaz, Houssni Lamkaddam, Urs Baltensperger, Andre Stephan Henry Prevot, and Jay Slowik
Metal emissions are of major environmental and practical concern because of their highly toxic effects on human health and ecosystems. Current technologies available in the market for their detection are typically limited by a time resolution of 1 h or longer (e.g., via semicontinuous X-ray fluorescence measurements) or are nonquantitative (e.g., laser ablation mass spectrometry). In this work, we report the development of a novel technique for the real-time detection and monitoring of metal particles in situ using an extractive electrospray ionization (EESI) source coupled to a high-resolution time-of-flight mass spectrometer (TOF-MS)…
On-line Breath Metabolomics with Ambient High-Resolution Mass Spectrometry
Martin Thomas Gaugg
Respiratory diseases are among the leading causes of death worldwide and pose a great financial burden on the health care system. During the last decades the medical community has started to recognize that a patient’s individual set of genes, along with environmental factors, are immensely important for the diagnosis and treatment of diseases. This has led to a strong drive towards further developments in personalized and evidencebased medicine. Understanding the underlying metabolic fundamentals of diseases is crucial to provide the appropriate patient care.One of the fastest methods to obtain new insights in this regard is to analyze metabolites in exhaled breath, which offers a non-invasive window into human metabolism, and which can be monitored in real time.
Novel strategies for online detection of doping compounds in breath using secondary electrospray ionization mass spectrometry
Lukas Christian Meier
It has been known for years that breath analysis has the potential of becoming a powerful tool to acquire information on the health status of individuals. Using mass spectrometry (MS) for breath analysis would allow for the detection of hundreds of compounds simultaneously and even render real time (online) monitoring of the individual’s health status possible. Unfortunately, the efficient transfer of breath into mass spectrometers is difficult to achieve. Therefore, only very volatile organic compounds (VOCs) being present in breath at high concentrations have been measured so far. The work presented in this thesis intends to extend the range of compounds being detected in breath towards higher masses, less volatile and less concentrated compounds…