The early 2000s brought a new age in the field of mass spectrometry (MS) with the introduction of ambient ionization MS techniques. As defined by one of its early visionaries, Prof. R. Graham Cooks, ambient ionization refers to \"the ionization of unprocessed or minimally modified samples in their native environment, and it typically refers to the ionization of condensed phase samples in air.\" Since its inception in 2004, many researchers and laboratories have contributed with approaches for sampling and ionization at atmospheric conditions, greatly decreasing experimental complexity and time required for mass spectrometry analyses. In the last 15 years, innovations in the field of ambient ionization MS have grown expansively, pushing these technologies far past their point of conception and integrating them into the broader scientific community in creative and stimulating ways.

Ambient ionization Mass Spectrometry: Recent Developments and Applications

Dalton T. Snyder,† Christopher J. Pulliam,† Zheng Ouyang,‡ and R. Graham Cooks*,† †Department of Chemistry and Center for Analytical Instrumentation Development, Purdue University, West Lafayette, Indiana 47907, United States ‡Weldon School of Biomedical Engineering, Purdue University, West Lafayette, Indiana 47907, United States ■ CONTENTS Ambient Ionization and Sampling 2 Vacuum Systems 4 Analyzers and Configurations 6 MEMS and Other Alternative Fabrication Methods 8 Simulations 9 Electronics and Data Systems 12 Portable Systems 19 Mesoscale Systems 20 Planetary and Space Science Systems 21 Practical Applications 22 Expectations 23 Author Information 23 Corresponding Author 23 Notes 23 Biographies 23 Acknowledgments 24 References 24

Miniature and Fieldable Mass Spectrometers: Recent Advances.

Portable analytical platforms for forensic chemistry: A review.

BACKGROUND: One driving motivation in the development of point-of-care (POC) diagnostics is to conveniently and immediately provide information upon which healthcare decisions can be based, while the patient is on site. Ambient ionization mass spectrometry (MS) allows direct chemical analysis of unmodified and complex biological samples. This suite of ionization techniques was introduced a decade ago and now includes a number of techniques, all seeking to minimize or eliminate sample preparation. Such approaches provide new opportunities for POC diagnostics and rapid measurements of exogenous and endogenous molecules (e.g., drugs, proteins, hormones) in small volumes of biological samples, especially when coupled with miniature mass spectrometers. CONTENT: Ambient MS-based techniques are applied in diverse fields such as forensics, pharmaceutical development, reaction monitoring, and food analysis. Clinical applications of ambient MS are at an early stage but show promise for POC diagnostics. This review provides a brief overview of various ambient ionization techniques providing background, examples of applications, and the current state of translation to clinical practice. The primary focus is on paper spray (PS) ionization, which allows quantification of analytes in complex biofluids. Current developments in the miniaturization of mass spectrometers are discussed. SUMMARY: Ambient ionization MS is an emerging technology in analytical and clinical chemistry. With appropriate MS instrumentation and user-friendly interfaces for automated analysis, ambient ionization techniques can provide quantitative POC measurements. Most significantly, the implementation of PS could improve the quality and lower the cost of POC testing in a variety of clinical settings.

/pdf/ambient-ionization-mass-spectrometry-for-point-of-care-352nh7opnk.pdf

Ambient Ionization Mass Spectrometry for Point-of-Care Diagnostics and Other Clinical Measurements

The direct interface of microextraction technologies to mass spectrometry (MS) has unquestionably revolutionized the speed and efficacy at which complex matrices are analyzed Solid Phase Micro Extraction–Transmission Mode (SPME-TM) is a technology conceived as an effective synergy between sample preparation and ambient ionization Succinctly, the device consists of a mesh coated with polymeric particles that extracts analytes of interest present in a given sample matrix This coated mesh acts as a transmission-mode substrate for Direct Analysis in Real Time (DART), allowing for rapid and efficient thermal desorption/ionization of analytes previously concentrated on the coating, and dramatically lowering the limits of detection attained by sole DART analysis In this study, we present SPME-TM as a novel tool for the ultrafast enrichment of pesticides present in food and environmental matrices and their quantitative determination by MS via DART ionization Limits of quantitation in the subnanogram per mill

Ultrafast Screening and Quantitation of Pesticides in Food and Environmental Matrices by Solid-Phase Microextraction–Transmission Mode (SPME-TM) and Direct Analysis in Real Time (DART)

An ambient method for rapid monitoring and quantitation of drugs of abuse in dried blood spots was developed using paper spray tandem mass spectrometry (PS-MS).

/pdf/quantitative-paper-spray-mass-spectrometry-analysis-of-drugs-45oq8sxipo.pdf

Quantitative paper spray mass spectrometry analysis of drugs of abuse.

Rapid qualitative and quantitative analysis of 4-methylimidazole (4-MEI) in caramel and beverage samples is demonstrated using the paper spray form of ambient ionization mass spectrometry. The minimum level of pure 4-MEI detectable using multiple reaction monitoring (MRM) in a triple quadrupole instrument was 3 pg μL−1 in neat solvent and 5 pg μL−1 in a matrix containing caramel. This method was used to analyze 11 caramel samples for 4-MEI. After implementing effective quality control protocols, average relative standard deviations for paper spray triple quadrupole MS were less than 15% and the linear dynamic range was three orders of magnitude. Results obtained on three different days by two different analyst groups agreed closely. An ion trap tandem MS method of approximate quantitative analysis is also described and it gave similar precision to the triple quadrupole experiment when fluctuations in ion currents were cancelled by simultaneously isolating the analyte and internal standard and fragmenting both in an ion trap simultaneous MRM experiment. As another alternative, a rapid qualitative screening method based on the use of high-resolution measurements instead of tandem mass spectrometry using an Orbitrap was also tested and found to give a detection limit of 100 pg μL−1.

Direct analysis of 4-methylimidazole in foods using paper spray mass spectrometry.

Paper spray (PS) ambient ionization is implemented using a portable mass spectrometer and applied to the detection of alkyl quaternary ammonium salts in a complex oil matrix These salts are commonly used as active components in the formulation of corrosion inhibitors They were identified in oil and confirmed by their fragmentation patterns recorded using tandem mass spectrometry (MS/MS) The cations of alkyl and benzyl-substituted quaternary ammonium salts showed characteristic neutral losses of CnH2n (n carbon number of the longest chain) and C7H8, respectively Individual quaternary ammonium compounds were detected at low concentrations (<1 ng μL−1) and over a dynamic range of ∼5 pg μL−1 to 500 pg μL−1 (ppb) Direct detection of these compounds in complex oil samples without prior sample preparation or pre-concentration was also demonstrated using a home-built miniature mass spectrometer at levels below 1 ng μL−1

https://www.rsc.org/suppdata/an/c3/c3an00249g/c3an00249g.pdf

In situ analysis of corrosion inhibitors using a portable mass spectrometer with paper spray ionization.

The application of zero volt paper spray to the discrimination between species of bacteria is demonstrated here. While absolute signal intensities of representative lipids from bacterial membranes were three orders of magnitude lower than for conventional paper spray performed at high potential (kilovolts), the significant reduction in noise offset this disadvantage, resulting in clear separation in principal component analysis space between Gram positive and Gram negative bacteria as well as excellent separation between bacteria species.

Analysis of bacteria using zero volt paper spray

The invention generally relates to sample analysis systems and methods of use thereof. In certain aspects, the invention provides a system for analyzing a sample that includes an ion generator configured to generate ions from a sample. The system additionally includes an ion separator configured to separate at or above atmospheric pressure the ions received from the ion generator without use of laminar flowing gas, and a detector that receives and detects the separated ions.

Sample analysis systems and methods of use thereof

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