Polymer substrate with surface solvent reservoir for polymer-spray mass spectrometric analysis of hydrophilic drugs

Dulay, Maria T.; Boeser, Cornelia L.; Walker, Katherine L.; Feider, Clara L.; Zare, Richard N.

doi:10.1016/j.talo.2021.100048

Cited by 5 publications

(10 citation statements)

References 42 publications

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“…In terms of target species, the Nafion desalting process is demonstrated to be applicable for peptides, proteins, nucleotides, or other acidic metabolites such as carboxylate compounds. Additionally, it is worth noting that this in situ desalting material is supposed to be a universal solution for various alternative spray MS substrates such as for porous ones like paper ( Damon, et al, 2016 ), or those hydrophobic materials such as organosiloxanes ( Dulay and Zare, 2017 ; Dulay et al, 2021 ), polystyrene ( Wang et al, 2017 ), carbon nanotubes (Song et al, 2020), and Teflon ( Narayanan et al, 2020 ).…”

Section: Resultsmentioning

confidence: 99%

Introducing Nafion for In Situ Desalting and Biofluid Profiling in Spray Mass Spectrometry

2022

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We introduce Nafion into the ambient ionization technique of spray mass spectrometry to serve for in situ desalting and direct analysis of biological fluids. Nafion was coated onto the surface of the triangular spray tip as the cation exchange material. Because the sulfonic group from the Nafion membrane effectively exchanges their carried protons with inorganic salt ions (e.g., Na+ and K+), the analyte’s ionization efficiency can be significantly enhanced by reducing ion suppression. The desalting efficiency can reach 90% and the maximum tolerance of the absolute salt amount reaches 100 μmol. The mass spectral profile can also be simplified by removing the multiple adducted ion types from small-molecule drugs and metabolites ([M + Na]+ and [M + K]+), or multiply charged ions formed by proteins ([M + nNa]n+ and [M + nK]n+). Thus, the Nafion coating makes less ambiguous data interpretation collected from spray mass spectrometry for qualitative profiling or quantitative measurement of a target analyte.

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Section: Resultsmentioning

confidence: 99%

Introducing Nafion for In Situ Desalting and Biofluid Profiling in Spray Mass Spectrometry

2022

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“…Previously, our group has developed a series of polymer-based ambient ionization methods [24][25][26][27], which have shown advantages in weak absorption of hydrophilic species, stronger ion intensity, and more stable signal duration [28]. Among these AIMS methods, conductive-polymer-spray-ionization mass spectrometry (CPSI-MS) has been successfully used for salivary metabolic profiling and oral cancer diagnosis [12].…”

Section: Introductionmentioning

confidence: 99%

“…Motivated by this past work, we were inspired to integrate liquid-phase HDX with AIMS to develop a simple, robust, and cost-effective method for distinguishing isobaric ions in untargeted metabolomic studies. Previously, our group has developed a series of polymer-based ambient ionization methods [24][25][26][27], which have shown advantages in weak absorption of hydrophilic species, stronger ion intensity, and more stable signal duration [28]. Among these AIMS methods, conductive-polymer-spray-ionization mass spectrometry (CPSI-MS) has been successfully used for salivary metabolic profiling and oral cancer diagnosis [12].…”

Section: Introductionmentioning

confidence: 99%

Distinguishing between Isobaric Ions Using Microdroplet Hydrogen–Deuterium Exchange Mass Spectrometry

Song

Mofidfar

et al. 2021

Metabolites

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Isobaric ions having the same mass-to-charge ratio cannot be separately identified by mass spectrometry (MS) alone, but this limitation can be overcome by using hydrogen–deuterium exchange (HDX) in microdroplets. Because isobaric ions may contain a varied number of exchangeable sites and different types of functional groups, each one produces a unique MS spectral pattern after droplet spray HDX without the need for MS/MS experiments or introduction of ion mobility measurements. As an example of the power of this approach, isobaric ions in urinary metabolic profiles are identified and used to distinguish between healthy individuals and those having bladder cancer.

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“…[23][24][25] Our group also proposes using polymer substrate instead of paper and has achieved remarkable improvements in ionization efficiency, signal stability, and the wide coverage of hydrophilic species. [26][27][28][29] This approach of polymer spray ionization has shown a good response for biological fluid metabolic profiling. In previous work, we have reported the practical value of conductive polymer spray ionization mass spectrometry (CPSI-MS) in the discrimination of OSCC with premalignant lesion (PML) and healthy contrast (HC).…”

Section: Introductionmentioning

confidence: 99%

“…Various surface coatings or modifications have been reported to overcome these issues 23–25 . Our group also proposes using polymer substrate instead of paper and has achieved remarkable improvements in ionization efficiency, signal stability, and the wide coverage of hydrophilic species 26–29 . This approach of polymer spray ionization has shown a good response for biological fluid metabolic profiling.…”

Section: Introductionmentioning

confidence: 99%

Big cohort metabolomic profiling of serum for oral squamous cell carcinoma screening and diagnosis

et al. 2021

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The survival rate of oral squamous cell carcinoma (OSCC) can be greatly improved if intervention could be initiated as early as possible. This poses a technical demand for developing a sensitive screening and specific in vitro diagnosis method for OSCC. Herewith, a large cohort consisting of 241 healthy contrast (HC) and 578 OSCC patients were recruited for conducting the rapid metabolic profiling of trace volume serum using conductive polymer spray ionization mass spectrometry (CPSI-MS). Statistical analysis picked out 65 metabolite ions as potential characteristic markers for differentiating OSCC from HC. With the aid of a supporting vector machine (SVM), OSCC can be distinguished from HC with an accuracy of 98.0% by cross-validation in the discovery cohort and 89.6% accuracy in the validation cohort. Furthermore, orthogonal partial least square-discriminant analysis (OPLS-DA) also initially showed the potential for OSCC staging, especially between T1/T2 and T3/T4 stages with an accuracy of 90.1%. CPSI-MS combined with SVM or OPLS-DA can not only quickly distinguish OSCC from HC but also predict the OSCC progression from T1/2 to T3/4 stages in a few minutes, making it a promising tool for both screening and diagnosing high-risk population.

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Polymer substrate with surface solvent reservoir for polymer-spray mass spectrometric analysis of hydrophilic drugs

Cited by 5 publications

References 42 publications

Introducing Nafion for In Situ Desalting and Biofluid Profiling in Spray Mass Spectrometry

Introducing Nafion for In Situ Desalting and Biofluid Profiling in Spray Mass Spectrometry

Distinguishing between Isobaric Ions Using Microdroplet Hydrogen–Deuterium Exchange Mass Spectrometry

Big cohort metabolomic profiling of serum for oral squamous cell carcinoma screening and diagnosis

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