Direct Infusion Electrospray Ionization – Ion Mobility – High Resolution Mass Spectrometry (DIESI-IM-HRMS) for Rapid Characterization of Potential Bioprocess Streams

Munisamy, Sharon M.; Chambliss, C. Kevin; Becker, Christopher H.

doi:10.1007/s13361-012-0382-2

Cited by 13 publications

(7 citation statements)

References 46 publications

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“…Six trisaccharide isomers were also evaluated with ion multiplexing and HRdm, which included melezitose (Mz), kestose (K), raffinose (R), isomaltotriose (I), maltotriose (M), and cellotriose (C). Numerous IMS studies have previously investigated various combinations of these isomers, including Mz/R, ,− Mz/R/I, Mz/R/I/M, Mz/R/I/C, Mz/R/M/C, Mz/I, K/R, I/M, R/I, and R/I/C, but none have explored mixtures of four or more. Here, we evaluate a mixture of all six carbohydrate isomers using HRdm.…”

Section: Resultsmentioning

confidence: 99%

Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique

Knochenmuss²,

et al. 2020

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A combined data acquisition and data processing strategy for improving the sensitivity and resolution of ion mobility measurements is described. This strategy is implemented on a commercially available drift tube ion mobility-mass spectrometry (IM-MS) instrument and utilizes both an existing ion multiplexing strategy to achieve up to an 8-fold gain in ion signal and a new postacquisition data reconstruction technique, termed “high resolution demultiplexing” (HRdm), to improve resolution in the ion mobility dimension. A series of isomeric mixtures were qualitatively investigated with HRdm, including biologically relevant lipids and carbohydrates, which were successfully resolved by HRdm, including two monosaccharide regioisomers which differed in drift time by only 0.8%. For a complex trisaccharide isomer mixture, HRdm was able to resolve 5 out of 6 components. An analysis of two-peak resolution (R pp) and peak-to-peak separation (ΔP) indicated that HRdm performs with an effective resolving power (R p) of between 180 to 250 for the highest deconvolution settings. Overall analysis times and drift time measurement precision were found to be unaffected between standard and HRdm processed data sets, which allowed statistically identical collision cross section values to be directly determined from all ion mobility spectra.

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Section: Resultsmentioning

confidence: 99%

Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique

Knochenmuss²,

et al. 2020

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“…A set of four trisaccharide isomers (melezitose, raffinose, isomaltotriose, and maltotriose), representing various monosaccharide subunit types and linkages, were analyzed individually and as a mixture by both DTIMS and SLIM IM (SLIM settings were 225 m/s and 40 V pp ). These isomers are routinely used by the IM community to benchmark separation performance. − For carbohydrates, the sodiated ion form appears in a high abundance and is investigated here ([M + Na] + , m / z 527). For the mixture of isomers, melezitose exhibits the lowest CCS and appears far-removed from the other trisaccharides.…”

Section: Results and Discussionmentioning

confidence: 99%

Resolving Power and Collision Cross Section Measurement Accuracy of a Prototype High-Resolution Ion Mobility Platform Incorporating Structures for Lossless Ion Manipulation

May

Leaptrot

Rose

et al. 2021

J. Am. Soc. Mass Spectrom.

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A production prototype structures for lossless ion manipulation ion mobility (SLIM IM) platform interfaced to a commercial high-resolution mass spectrometer (MS) is described. The SLIM IM implements the traveling wave ion mobility technique across a ∼13m path length for high-resolution IM (HRIM) separations. The resolving power (CCS/ΔCCS) of the SLIM IM stage was benchmarked across various parameters (traveling wave speeds, amplitudes, and waveforms), and results indicated that resolving powers in excess of 200 can be accessed for a broad range of masses. For several cases, resolving powers greater than 300 were achieved, notably under wave conditions where ions transition from a nonselective "surfing" motion to a mobility-selective ion drift, that corresponded to ion speeds approximately 30−70% of the traveling wave speed. The separation capabilities were evaluated on a series of isomeric and isobaric compounds that cannot be resolved by MS alone, including reversedsequence peptides (SDGRG and GRGDS), triglyceride double-bond positional isomers (TG 3,6, 9 and TG 6,9,12), trisaccharides (melezitose, raffinose, isomaltotriose, and maltotriose), and ganglioside lipids (GD1b and GD1a). The SLIM IM platform resolved the corresponding isomeric mixtures, which were unresolvable using the standard resolution of a drift-tube instrument (∼50). In general, the SLIM IM-MS platform is capable of resolving peaks separated by as little as ∼0.6% without the need to target a specific separation window or drift time. Low CCS measurement biases <0.5% were obtained under high resolving power conditions. Importantly, all the analytes surveyed are able to access high-resolution conditions (>200), demonstrating that this instrument is well-suited for broadband HRIM separations important in global untargeted applications.

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“…The majority of the mass spectra were obtained in the m/z range up to m/z 1000 19–23,26,37 or m/z 1500, 19,24,28,38,39 often with the main goal being to evaluate lignin degradation products 40–42 . However, the MW was mostly left undetermined, 19–24,26,28,37–39 although some studies mentioned the mass range in Daltons in addition to the m/z range, thus recognizing the formation of multiply charged species typical for ESI 15,24,27 . The mass range reported after a presumed deconvolution reached up to 2400, 4500 and 7000 Da 15,24,28 .…”

Section: Esi‐ms Analysis Of Ligninmentioning

confidence: 99%

Atmospheric pressure ionization mass spectrometry as a tool for structural characterization of lignin

Kubátová

Andrianova

Hatton

et al. 2020

Rapid Comm Mass Spectrometry

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Rationale Lignin occurs in a broad range of forms, e.g., native as the main support for plant walls, and processed, for which its structure depends on the nature of the industrial isolation method, such as in paper production or in biorefineries. Due to the variety of lignin sources, there is no unified agreement on the structure of lignin or even its molecular weight (MW). Methods The focus of this review is on the application of atmospheric pressure ionization methods to lignin analysis by mass spectrometry (MS), namely electrospray ionization (ESI) or direct analysis in real‐time (DART). Specific parameters affecting ionization including electrolytes and solvents are discussed. Results The main challenge for MW determination of lignin is its heteropolymer character as well as the mass range limitations of MS instrumentation. To date, only a few studies have successfully used the mass range above m/z 1500. We present the advantage of ESI in generating multiply charged ions, allowing for a further increase in the mass range of deconvoluted mass spectra. While some methods such as DART do not address the mass range problem, they may serve as excellent imaging tools suitable for structural characterization of lignin. Conclusions A literature review presents the recent accomplishments in lignin MS analysis by atmospheric pressure ionization techniques. Although significant breakthroughs have been made, it is essential to further improve the operating conditions and validate the methods for a broader range of feedstocks with the results being confirmed using other methods.

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Direct Infusion Electrospray Ionization – Ion Mobility – High Resolution Mass Spectrometry (DIESI-IM-HRMS) for Rapid Characterization of Potential Bioprocess Streams

Cited by 13 publications

References 46 publications

Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique

Resolution of Isomeric Mixtures in Ion Mobility Using a Combined Demultiplexing and Peak Deconvolution Technique

Resolving Power and Collision Cross Section Measurement Accuracy of a Prototype High-Resolution Ion Mobility Platform Incorporating Structures for Lossless Ion Manipulation

Atmospheric pressure ionization mass spectrometry as a tool for structural characterization of lignin

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