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Matthew A Baird, Pratima Pathak, Alexandre A Shvartsburg
Nearly all molecules incorporate at least one element with stable isotopes, yielding ubiquitous isotopologic envelopes in mass spectra. Those envelopes split in differential ion mobility (FAIMS) spectra depending on the ion geometry, enabling a new general approach to isomer delineation as we demonstrated for chloroanilines. Here we report that analogous bromoanilines exhibit qualitatively distinct isotopic shifts under identical conditions, some changing signs depending on the gas. This dramatic elemental specificity conveys the breadth and diversity of structural isotopic effect in FAIMS, suggesting unique information-rich patterns for compounds involving various elements and feasibility of enhancing the structural elucidation by atom substitution...
February 1, 2019: Analytical Chemistry
Devin K Schweppe, Satendra Prasad, Michael W Belford, Jose Navarrete-Perea, Derek Bailey, Romain Huguet, Mark P Jedrychowski, Ramin Rad, Graeme McAlister, Susan E Abbatiello, Eloy R Woulters, Vlad Zabrouskov, Jean-Jacques Dunyach, Joao A Paulo, Steven P Gygi
Multiplexed, isobaric tagging methods are powerful techniques to increase throughput, precision and accuracy in quantitative proteomics. The dynamic range and accuracy of quantitation, however, can be limited by co-isolation of tag-containing peptides that release reporter ions and conflate quantitative measurements across precursors. Methods to alleviate these effects often lead to the loss of protein and peptide identifications through online or offline filtering of interference containing spectra. To alleviate this effect, high-Field Asymmetric-waveform Ion Mobility Spectroscopy (FAIMS) has been proposed as a method to reduce precursor co-isolation and improve the accuracy and dynamic range of multiplex quantitation...
January 23, 2019: Analytical Chemistry
Samuli I Nissinen, Antti Roine, Lauri Hokkinen, Markus Karjalainen, Markus Venäläinen, Heli Helminen, Riikka Niemi, Terho Lehtimäki, Tuomo Rantanen, Niku Oksala
BACKGROUND/AIM: Most pancreatic cancer patients are diagnosed at an advanced stage, since the diagnosis is demanding. Field asymmetric waveform ion mobility spectrometry (FAIMS) is a sensitive technique used for the detection of volatile organic compounds (VOC). We evaluated the ability of FAIMS to discriminate between pancreatic cancer and healthy controls from a urine sample. PATIENTS AND METHODS: For a proof-of-concept study in three Finnish hospitals, 68 patients with pancreatic cancer, 36 with acute pancreatitis, 18 with chronic pancreatitis, 8 with pancreatic pre-malign lesions and 52 healthy controls were prospectively recruited...
January 2019: Anticancer Research
Matthew A Baird, Gordon A Anderson, Pavel Vyacheslavovich Shliaha, Ole Nørregaard Jensen, Alexandre A Shvartsburg
Strong orthogonality to mass spectrometry makes differential ion mobility spectrometry (FAIMS) a powerful tool for isomer separations. However, high FAIMS resolution and 2-D FAIMS/MS peak capacity were overall achieved only with buffers rich in He or H2. That obstructed coupling to Fourier-transform mass spectrometers operating in ultrahigh vacuum, but exceptional m/z resolution and accuracy of FTMS are indispensable for frontline biological and environmental applications. By raising the waveform amplitude to 6 kV, we enabled high FAIMS resolution using solely N2 and thus straightforward integration with any MS platform - here Orbitrap XL with electron transfer dissociation (ETD) option...
December 13, 2018: Analytical Chemistry
Siavash Esfahani, Alfian Wicaksono, Ella Mozdiak, Ramesh P Arasaradnam, James A Covington
The electronic nose (eNose) is an instrument designed to mimic the human olfactory system. Usage of eNose in medical applications is more popular than ever, due to its low costs and non-invasive nature. The eNose sniffs the gases and vapours that emanate from human waste (urine, breath, and stool) for the diagnosis of variety of diseases. Diabetes mellitus type 2 (DM2) affects 8.3% of adults in the world, with 43% being underdiagnosed, resulting in 4.9 million deaths per year. In this study, we investigated the potential of urinary volatile organic compounds (VOCs) as novel non-invasive diagnostic biomarker for diabetes...
December 1, 2018: Biosensors
Rian L Griffiths, Anna L Simmonds, John G Swales, Richard J A Goodwin, Helen J Cooper
We have previously demonstrated liquid extraction surface analysis (LESA) high field asymmetric waveform ion mobility spectrometry (FAIMS) mass spectrometry imaging of proteins in thin tissue sections of brain and liver. Here, we present an improved approach that makes use of multiple static FAIMS parameters at each sampled location and allows a significant improvement in the number of proteins, lipids, and drugs that can be imaged simultaneously. The approach is applied to the mass spectrometry imaging of control and cassette-dosed rat kidneys...
October 29, 2018: Analytical Chemistry
Andrea S Martinez-Vernon, James A Covington, Ramesh P Arasaradnam, Siavash Esfahani, Nicola O'Connell, Ioannis Kyrou, Richard S Savage
MOTIVATION: The measurement of disease biomarkers in easily-obtained bodily fluids has opened the door to a new type of non-invasive medical diagnostics. New technologies are being developed and fine-tuned in order to make this possibility a reality. One such technology is Field Asymmetric Ion Mobility Spectrometry (FAIMS), which allows the measurement of volatile organic compounds (VOCs) in biological samples such as urine. These VOCs are known to contain a range of information on the relevant person's metabolism and can in principle be used for disease diagnostic purposes...
2018: PloS One
Riikka J Niemi, Antti N Roine, Emmi Eräviita, Pekka S Kumpulainen, Johanna U Mäenpää, Niku Oksala
AIM: We hypothesized that field asymmetric waveform ion mobility spectrometry (FAIMS) as a novel artificial olfactory technology could differentiate urine of women with malignant ovarian tumors from controls and women with benign tumors, based on previous findings on the ability of canine olfactory system to "smell" cancer. PATIENTS AND METHODS: Preoperative urine samples from 51 women with ovarian tumors, both benign and malignant, and from 18 women with genital prolapse, as controls, were collected...
September 23, 2018: Gynecologic Oncology
Paolo Devanna, Maartje van de Vorst, Rolph Pfundt, Christian Gilissen, Sonja C Vernes
Intellectual disability (ID) is a severe neurodevelopmental disorder with genetically heterogeneous causes. Large-scale sequencing has led to the identification of many gene-disrupting mutations; however, a substantial proportion of cases lack a molecular diagnosis. As such, there remains much to uncover for a complete understanding of the genetic underpinnings of ID. Genetic variants present in non-coding regions of the genome have been highlighted as potential contributors to neurodevelopmental disorders given their role in regulating gene expression...
September 2018: Human Genetics
Sibylle Pfammatter, Eric Bonneil, Francis P McManus, Satendra Prasad, Derek J Bailey, Michael Belford, Jean-Jacques Dunyach, Pierre Thibault
The depth of proteomic analyses is often limited by the overwhelming proportion of confounding background ions that compromise the identification and quantification of low abundance peptides. To alleviate these limitations, we present a new high field asymmetric waveform ion mobility spectrometry (FAIMS) interface that can be coupled to the Orbitrap Tribrid mass spectrometers. The interface provides several advantages over previous generations of FAIMS devices, including ease of operation, robustness, and high ion transmission...
October 2018: Molecular & Cellular Proteomics: MCP
Christopher P Ireland, Michael Coto, Lauren Brown, Russell Paris, Caterina Ducati
We demonstrate a versatile protocol to be used for determining the effectiveness of photocatalysts in degrading indoor air concentration (ppb) volatile organic carbons (VOCs), illustrating this with a titanium dioxide based catalyst, and the VOC 2-propanol. The protocol takes advantage of field asymmetric ion mobility spectroscopy (FAIMS), an analysis tool that is capable of continuously identifying and monitoring the concentration of VOCs such as 2-propanol and acetone at the ppb level. The continuous nature of FAIMS allows detailed kinetic analysis, and long-term reactions, offering a significant advantage over gas chromatography, a batch process traditionally used in air purification characterization...
June 14, 2018: Journal of Visualized Experiments: JoVE
Alexander S Hebert, Satendra Prasad, Michael W Belford, Derek J Bailey, Graeme C McAlister, Susan E Abbatiello, Romain Huguet, Eloy R Wouters, Jean-Jacques Dunyach, Dain R Brademan, Michael S Westphall, Joshua J Coon
Liquid chromatography (LC) prefractionation is often implemented to increase proteomic coverage; however, while effective, this approach is laborious, requires considerable sample amount, and can be cumbersome. We describe how interfacing a recently described high-field asymmetric waveform ion mobility spectrometry (FAIMS) device between a nanoelectrospray ionization (nanoESI) emitter and an Orbitrap hybrid mass spectrometer (MS) enables the collection of single-shot proteomic data with comparable depth to that of conventional two-dimensional LC approaches...
August 7, 2018: Analytical Chemistry
Pratima Pathak, Matthew A Baird, Alexandre A Shvartsburg
Nearly all molecules incorporate elements with stable isotopes. The resulting isotopologue envelopes in mass spectra tell the exact stoichiometry but nothing about the geometry. Chromatography and electrophoresis at high resolution also can distinguish isotopologues, again without revealing structural information. In high-definition differential ion mobility (FAIMS) spectra, these envelopes universally split in a structure-specific manner, providing a new general approach to isomer delineation. Here, we show that the peak shifts from instances of the same isotope are equal and can be averaged into characteristic elemental shifts, namely 13 C and 37 Cl for dichloroanilines (DCA)...
August 7, 2018: Analytical Chemistry
Daniel J C Berkhout, Britt J van Keulen, Hendrik J Niemarkt, Jet R Bessem, Willem P de Boode, Veerle Cossey, Neil Hoogenes, Christiaan V Hulzebos, Ellen Klaver, Peter Andriessen, Anton H van Kaam, Boris W Kramer, Richard A van Lingen, Aaron Schouten, Johannes B van Goudoever, Daniel C Vijlbrief, Mirjam M van Weissenbruch, Alfian N Wicaksono, James A Covington, Marc A Benninga, Nanne K H de Boer, Tim G J de Meij
Background: The intestinal microbiota has increasingly been considered to play a role in the etiology of late-onset sepsis (LOS). We hypothesize that early alterations in fecal volatile organic compounds (VOCs), reflecting intestinal microbiota composition and function, allow for discrimination between infants developing LOS and controls in a preclinical stage. Methods: In 9 neonatal intensive care units in the Netherlands and Belgium, fecal samples of preterm infants born at a gestational age ≤30 weeks were collected daily, up to the postnatal age of 28 days...
June 21, 2018: Clinical Infectious Diseases: An Official Publication of the Infectious Diseases Society of America
Aaron J O'Sullivan, Cian O'Mahony, Leo Meunier, Nik Loveridge, Aideen I McKevitt
Children with phenylketonuria (PKU) and severe cow's milk protein allergy (CMPA) consume prescribed, specially formulated, foods for special medical purposes (FSMPs) in addition to having restricted intake of normal foods. These vulnerable patients are exposed to artificial sweeteners from the consumption of a combination of both free and prescribed foods. Young patients with PKU and CMPA aged from 1 to 3 years have a higher risk of exceeding the acceptable daily intake (ADI) for sweeteners than age-matched healthy children...
August 2018: Food Additives & Contaminants. Part A, Chemistry, Analysis, Control, Exposure & Risk Assessment
Sofie Bosch, Sofia El Manouni El Hassani, James A Covington, Alfian N Wicaksono, Marije K Bomers, Marc A Benninga, Chris J J Mulder, Nanne K H de Boer, Tim G J de Meij
Fecal volatile organic compounds (VOCs) are increasingly considered to be potential noninvasive, diagnostic biomarkers for various gastrointestinal diseases. Knowledge of the influence of sampling conditions on VOC outcomes is limited. We aimed to evaluate the effects of sampling conditions on fecal VOC profiles and to assess under which conditions an optimal diagnostic accuracy in the discrimination between pediatric inflammatory bowel disease (IBD) and controls could be obtained. Fecal samples from de novo treatment-naïve pediatric IBD patients and healthy controls (HC) were used to assess the effects of sampling conditions compared to the standard operating procedure (reference standard), defined as 500 mg of sample mass diluted with 10 mL tap water, using field asymmetric ion mobility spectrometry (FAIMS)...
July 3, 2018: Analytical Chemistry
Kyana Y Garza, Clara L Feider, Dustin R Klein, Jake A Rosenberg, Jennifer S Brodbelt, Livia S Eberlin
Analysis of large biomolecules including proteins has proven challenging using ambient ionization mass spectrometry imaging techniques. Here, we have successfully optimized desorption electrospray ionization mass spectrometry (DESI-MS) to detect intact proteins directly from tissue sections and further integrated DESI-MS to a high field asymmetric waveform ion mobility (FAIMS) device for protein imaging. Optimized DESI-FAIMS-MS parameters were used to image mouse kidney, mouse brain, and human ovarian and breast tissue samples, allowing detection of 11, 16, 14, and 16 proteoforms, respectively...
July 3, 2018: Analytical Chemistry
Cecilie Rosting, Jinglei Yu, Helen J Cooper
Despite the great potential of dried blood spots (DBS) as a source of endogenous proteins for biomarker discovery, the literature relating to nontargeted bottom-up proteomics of DBS is sparse, primarily due to the inherent complexity and very high dynamic range associated with these samples. Here, we present proof-of-concept results in which we have coupled high field asymmetric waveform ion mobility spectrometry (FAIMS) with liquid chromatography-tandem mass spectrometry (LC-MS/MS) for nontargeted bottom-up proteomics of DBS with the aim of addressing these challenges...
June 1, 2018: Journal of Proteome Research
Sibylle Pfammatter, Eric Bonneil, Francis P McManus, Pierre Thibault
The small ubiquitin-like modifier (SUMO) is a member of the family of ubiquitin-like modifiers (UBLs) and is involved in important cellular processes, including DNA damage response, meiosis and cellular trafficking. The large-scale identification of SUMO peptides in a site-specific manner is challenging not only because of the low abundance and dynamic nature of this modification, but also due to the branched structure of the corresponding peptides that further complicate their identification using conventional search engines...
June 2018: Journal of the American Society for Mass Spectrometry
Chia-Wei Tsai, Christopher A Tipple, Richard A Yost
RATIONALE: Paper spray ionization (PSI) is an attractive ambient ionization source for mass spectrometry (MS) since it allows the combination of surface sampling and ionization. The minimal sample preparation inherent in this approach greatly reduces the time needed for analysis. However, the ions generated from interfering compounds in the sample and the paper substrate may interfere with the analyte ions. Therefore, the integration of PSI with high-field asymmetric ion mobility spectrometry (FAIMS) is of significant interest since it should reduce the background ions entering the mass analyzer without complicating the analysis or increasing analysis time...
April 15, 2018: Rapid Communications in Mass Spectrometry: RCM
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