Minimizing transient microenvironment-associated variability for analysis of environmental anthropogenic contaminants via ambient ionization

Emmons, Ronald V.; Gionfriddo, Emanuela

doi:10.1016/j.scitotenv.2021.145789

Cited by 14 publications

(9 citation statements)

References 42 publications

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“…Optimal electric grid voltage values are significantly lower than conventional voltages used for DART (absolute voltage values within 300 and 400 V), a parameter seldomly optimized in literature. This trend has also been observed in the DART-MS analysis of positive ion species, 34 it being posited that the voltage applied to the electric grid could negatively affect the transmission of ions to the MS inlet. Comparing the mass spectra obtained for GenX between the two end points at −100 and −300 V (Figure S7), the [M − H] − ion is unable to be discriminated from noise at −300 V (m/z = 329) but is readily apparent at −100 V. This voltage played a very minor role in the response of sulfonic acids (Figures 1 and S8); higher response values were obtained with lower absolute voltage but were not statistically significant in the CCD.…”

Section: ■ Results and Discussionmentioning

confidence: 59%

“…Initial experiments showed no direct desorption of PFAS from SPME devices (fibers and blades) via DART, as the plasma stream was unable to disrupt the ion-exchange interaction between the analytes and the device’s extraction phase. Desorption from SPME devices into DART plasma has been demonstrated in other works, utilizing neutral extraction phases. − Therefore, a liquid desorption step was carried out before DART analysis in 80:20 methanol:water. While ammonium hydroxide was optimized as the best additive for SPME desorption for the model analytes when analyzed through LC-MS/MS, ammonium formate has also demonstrated to be effective as a desorption additive when analyzing a larger range of PFAS .…”

Section: Resultsmentioning

confidence: 99%

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Rapid Screening and Quantification of PFAS Enabled by SPME-DART-MS

Emmons

Fatigante

Olomukoro

et al. 2023

J. Am. Soc. Mass Spectrom.

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Per-and polyfluoroalkyl substances (PFAS), an emerging class of toxic anthropogenic chemicals persistent in the environment, are currently regulated at the low part-per-trillion level worldwide in drinking water. Quantification and screening of these compounds currently rely primarily on liquid chromatography hyphenated to mass spectrometry (LC-MS). The growing need for quicker and more robust analysis in routine monitoring has been, in many ways, spearheaded by the advent of direct ambient mass spectrometry (AMS) technologies. Direct analysis in real time (DART), a plasma-based ambient ionization technique that permits rapid automated analysis, effectively ionizes a broad range of compounds, including PFAS. This work evaluates the performance of DART-MS for the screening and quantification of PFAS of different chemical classes, employing a central composite design (CCD) to better understand the interactions of DART parameters on their ionization. Furthermore, in-source fragmentation of the model PFAS was investigated based on the DART parameters evaluated. Preconcentration of PFAS from water samples was achieved by solid phase microextraction (SPME), and extracts were analyzed using the optimized DART-MS conditions, which allowed obtaining linear dynamic ranges (LDRs) within 10 and 5000 ng/L and LOQs of 10, 25, and 50 ng/L for all analytes. Instrumental analysis was achieved in less than 20 s per sample.

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Section: ■ Results and Discussionmentioning

confidence: 59%

Section: Resultsmentioning

confidence: 99%

Rapid Screening and Quantification of PFAS Enabled by SPME-DART-MS

Emmons

Fatigante

Olomukoro

et al. 2023

J. Am. Soc. Mass Spectrom.

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“…The technique was able to detect triclosan in raw and treated wastewater in good agreement with LC‐MS. DART‐MS has also been applied to the analysis of pesticides and pharmaceuticals in surface water, though using a solid phase microextraction (SPME) extraction step in an attempt to improve reproducibility by reducing background interferences 114 …”

Section: Applications Of Ambient Ionization Mass Spectrometrymentioning

confidence: 99%

“…154 Finally, the implementation of different internal standard strategies has been explored with DESI, demonstrating optimal and inappropriate methods for the introduction of internal standards to achieve the best quantitative results. 155 Interestingly, there has been a recent increase in the supplemen- coupled with a range of AIMS techniques, including PESI for the detection of drugs of abuse, 156 both PESI and CBS to monitor drug biotransformations, 157 DART to detect pesticides and pharmaceuticals in surface water 114 and using the SPME device itself as an ESI emitter for direct analysis of biological samples in front of the MS inlet. 158 A primary advantage of AIMS is the potential to take the instrument into the field to perform rapid on-site testing, yet many techniques…”

Section: Technological Advancementsmentioning

confidence: 99%

Applications of ambient ionization mass spectrometry in 2021: An annual review

Rankin‐Turner

Reynolds

Turner

et al. 2022

Analytical Science Advances

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Ambient ionization mass spectrometry (AIMS) has revolutionized the field of analytical chemistry, enabling the rapid, direct analysis of samples in their native state. Since the inception of AIMS almost 20 years ago, the analytical community has driven the further development of this suite of techniques, motivated by the plentiful advantages offered in addition to traditional mass spectrometry. Workflows can be simplified through the elimination of sample preparation, analysis times can be significantly reduced and analysis remote from the traditional laboratory space has become a real possibility. As such, the interest in AIMS has rapidly spread through analytical communities worldwide, and AIMS techniques are increasingly being integrated with standard laboratory operations. This annual review covers applications of AIMS techniques throughout 2021, with a specific focus on AIMS applications in a number of key fields of research including disease diagnostics, forensics and security, food safety testing and environmental sciences. While some new techniques are introduced, the focus in AIMS research is increasingly shifting from the development of novel techniques toward efforts to improve existing AIMS techniques, particularly in terms of reproducibility, quantification and ease-of-use.

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“…10 The innate variability of the transient environment around an ambient ion source led several groups to enclose a conventional SPME fiber during desorption and ionization. The enclosures featured either a thermal desorption unit attached to but independent of the dielectric barrier discharge or DART ion source and MS inlet, 11,12 or a junction for the enclosed DART to itself desorb analyte. 13 In each case, the regulated heat source allowed the SPME analytes to be desorbed at the correct manufacturer-recommended temperature, as opposed to assuming that the DART helium temperature setting would accurately represent the temperature at the sorptive surface.…”

Section: ■ Introductionmentioning

confidence: 99%

Selective Sampling to and Desorption from Single Solid-Phase Microextraction Arrow Fiber for Replicative and Quantitative Analysis

Newsome,

Birdsall,

Cody

2024

J. Am. Soc. Mass Spectrom.

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New analytical functionality is demonstrated with an enclosed interface that joins a solid phase microextraction (SPME) device, a direct analysis in real time (DART) probe, and a high-resolution mass spectrometer. With a single 20 mm long SPME Arrow, the interface is able to perform five discrete DART analyses on different areas of the same fiber in 1 min of practical operation time. Three-fiber replicates for 15 runs total produce 15% or better center of variance (CV) values for both volatile headspace sampling and direct immersion sampling of a solvated analyte. Chemometric analysis of rapidly acquired headspace data is able to distinguish volatile profiles. Selective desorption within the interface also confers the ability to selectively sample to discrete areas of a fiber, and three different headspace samples or five different liquid samples can be acquired and differentiated with one Arrow. A five-point standard addition curve is constructed to measure the concentration of the solvated analyte. Unmodified commercial components of the analysis system include the fiber itself, the Orbitrap and AccuTOF mass spectrometer platforms, and the conditioning gas chromatograph inlet. Machine diagrams for the SPME-DART interface and Arrow fiber holder are included.

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Minimizing transient microenvironment-associated variability for analysis of environmental anthropogenic contaminants via ambient ionization

Cited by 14 publications

References 42 publications

Rapid Screening and Quantification of PFAS Enabled by SPME-DART-MS

Rapid Screening and Quantification of PFAS Enabled by SPME-DART-MS

Applications of ambient ionization mass spectrometry in 2021: An annual review

Selective Sampling to and Desorption from Single Solid-Phase Microextraction Arrow Fiber for Replicative and Quantitative Analysis

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