Separation of Cisplatin and Its Hydrolysis Products Using Electrospray Ionization High-Field Asymmetric Waveform Ion Mobility Spectrometry Coupled with Ion Trap Mass Spectrometry

Cui, Meng; Ding, Luyi; Mester, Zoltán

doi:10.1021/ac0344182

Cited by 57 publications

(66 citation statements)

References 39 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…The hemispherical section of "dome" FAIMS that collects ions separated in the cylindrical part provides a natural MS interface, resulting in a broad acceptance of that design. [22][23][24][25][26][27][28][29][30][31][32][33][34][35] In a planar analytical gap, ions freely spread laterally to the gas flow and only a minor fraction enters a small orifice leading to MS. This has compelled virtually all FAIMS/MS systems to adopt c-FAIMS, regardless of its intrinsic merits vs. p-FAIMS.…”

Section: Introductionmentioning

confidence: 99%

High-Resolution Field Asymmetric Waveform Ion Mobility Spectrometry Using New Planar Geometry Analyzers

2006

View full text Add to dashboard Cite

Field asymmetric waveform ion mobility spectrometry (FAIMS) has emerged as a powerful tool of broad utility for separation and characterization of gas-phase ions, especially in conjunction with mass spectrometry (MS). In FAIMS, ions are filtered by the dependence of mobility on electric field while carried by gas flow through the analytical gap between two electrodes of either planar (p-) or cylindrical (c-) geometry. Most FAIMS/MS systems employ c-FAIMS because of its ease of coupling to MS, yet the merits of two geometries have not been compared in detail. Here, a priori simulations reveal that reducing the FAIMS curvature always improves resolution at equal sensitivity. In particular, the resolving power of p-FAIMS exceeds that of c-FAIMS, typically by a factor of 2 -4 depending on the ion species and carrier gas. We have constructed a new planar FAIMS incorporating a curtain plate interface for effective operation with an ESI ion source and joined to MS using an ion funnel interface with a novel slit aperture. The resolution increases up to 4-fold over existing c-FAIMS, even though the analysis is ∼2 times faster. This allows separation of species not feasible in previous FAIMS studies, e.g., protonated leucine and isoleucine or new bradykinin isomers. The improvement for protein conformers (of ubiquitin) is less significant, possibly because of multiple unresolved geometries.

show abstract

Section: Introductionmentioning

confidence: 99%

High-Resolution Field Asymmetric Waveform Ion Mobility Spectrometry Using New Planar Geometry Analyzers

2006

View full text Add to dashboard Cite

show abstract

“…[4][5][6][7][8][9][10] Recent commercial introduction of such systems [11][12][13][14] is expanding interest in ion mobility/MS, particularly for analyses of complex biological samples such as proteolytic digests and lipids, nucleotides, and metabolites. [15][16][17][18][19][20][21][22][23][24] Single-stage ion mobility spectrometry (IMS) was investigated since the 1970s, [25][26][27] with a noteworthy development of ESI/IMS in 1980s. 28 In IMS, ions drift through a non-reactive buffer gas under the influence of a modest electric field.…”

mentioning

confidence: 99%

Feasibility of Higher-Order Differential Ion Mobility Separations Using New Asymmetric Waveforms

2006

View full text Add to dashboard Cite

Technologies for separating and characterizing ions based on their transport properties in gases have been around for three decades. The early method of ion mobility spectrometry (IMS) distinguished ions by absolute mobility that depends on the collision cross section with buffer gas atoms. The more recent technique of field asymmetric waveform IMS (FAIMS) measures the difference between mobilities at high and low electric fields. Coupling IMS and FAIMS to soft ionization sources and mass spectrometry (MS) has greatly expanded their utility, enabling new applications in biomedical and nanomaterials research. Here, we show that time-dependent electric fields comprising more than two intensity levels could, in principle, effect an infinite number of distinct differential separations based on the higher-order terms of expression for ion mobility. These analyses could employ the hardware and operational procedures similar to those utilized in FAIMS. Methods up to the 4 th or 5 th order (where conventional IMS is 1 st order and FAIMS is 2 nd order) should be practical at field intensities accessible in ambient air, with still higher orders potentially achievable in insulating gases. Available experimental data suggest that higher-order separations should be largely orthogonal to each other and to FAIMS, IMS, and MS.Approaches to separation of ion mixtures and characterization of ions in the gas phase based on ion mobility are becoming commonplace in analytical chemistry. The key advantage of gas-phase separations over condensed phase methods is the exceptional speed enabled by rapid molecular motion in gases. This inherent benefit is made increasingly topical by the growing focus of analytical technology on higher throughput. Since their first demonstration a decade ago, 1-3 instrumental platforms combining electrospray ionization (ESI) or matrixassisted laser desorption ionization (MALDI) sources with ion mobility separations and mass-spectrometry (MS) have undergone a sustained development that has improved their resolution and sensitivity to the levels demanded by practical applications. 4-10 Recent commercial introduction of such systems 11-14 is expanding interest in ion mobility/MS, particularly for analyses of complex biological samples such as proteolytic digests and lipids, nucleotides, and metabolites. [15][16][17][18][19][20][21][22][23][24] Single-stage ion mobility spectrometry (IMS) was investigated since the 1970s, 25-27 with a noteworthy development of ESI/IMS in 1980s. 28 In IMS, ions drift through a non-reactive buffer gas under the influence of a modest electric field. The drift velocity (v) in the field of intensity E is determined by ion mobility (K):(1)For consistency, measured mobilities are normally converted to reduced values K 0 by adjusting the buffer gas temperature (T, Kelvin) and pressure (P, Torr) to standard (STP) conditions:NIH Public Access

show abstract

“…However, FAIMS was not widely used until its coupling to electrospray ionization mass spectrometry [8,9], which has expanded its utility to environmental [10 -13] and biological [14 -18] applications, in addition to traditional detection of airborne volatiles [19 -23]. The recent advent of commercial FAIMS systems (Ionalytics Selectra [17,24] and Sionex DMS [23,25]) is increasing the acceptance of FAIMS and diversifying its applications.While FAIMS analyses have become increasingly common, the fundamentals remain relatively poorly understood [18]. Phenomenologically, ions are separated by the difference between mobilities at high and low electric fields (E) (respectively K H and K L ) that in general differ as ion mobilities in gases depend on the field.…”

mentioning

confidence: 99%

mentioning

confidence: 99%

“…This diffusion may be suppressed in a field that is spatially nonuniform along its direction and has proper polarity (depending on the ion type), such as established in the annular gap between two coaxial cylinders where ions can be focused to the gap median [8]. This configuration (with a hemispherical cap) has been adopted in Ionalytics Selectra [17,24]. In all commercial FAIMS systems, ions are carried through the gap by a gas stream.…”

mentioning

confidence: 99%

See 1 more Smart Citation

FAIMS operation for realistic gas flow profile and asymmetric waveforms including electronic noise and ripple

Shvartsburg

Tang

Smith

2005

J. Am. Soc. Mass Spectrom.

View full text Add to dashboard Cite

The use of field asymmetric waveform ion mobility spectrometry (FAIMS) has rapidly grown with the advent of commercial FAIMS systems coupled to mass spectrometry. However, many fundamental aspects of FAIMS remain obscure, hindering its technological improvement and expansion of analytical utility. Recently, we developed a comprehensive numerical simulation approach to FAIMS that can handle any device geometry and operating conditions. The formalism was originally set up in one dimension for a uniform gas flow and limited to ideal asymmetric voltage waveforms. Here we extend the model to account for a realistic gas flow velocity distribution in the analytical gap, axial ion diffusion, and waveform imperfections (e.g., noise and ripple). The nonuniformity of the gas flow velocity profile has only a minor effect, slightly improving resolution. Waveform perturbations are significant even at very low levels, in some cases ϳ0.01% of the nominal voltage. These perturbations always improve resolution and decrease sensitivity, a trade-off controllable by variation of noise or ripple amplitude. This trade-off is physically inferior to that obtained by adjusting the gap width and/or asymmetric waveform frequency. However, the disadvantage is negligible when the perturbation period is much shorter than the residence time in FAIMS, and ripple adjustment appears to offer a practical method for modifying FAIMS resolution. S eparation of ions in the gas-phase using field asymmetric waveform ion mobility spectrometry (FAIMS) extends back two decades [1][2][3][4][5][6][7]. However, FAIMS was not widely used until its coupling to electrospray ionization mass spectrometry [8,9], which has expanded its utility to environmental [10 -13] and biological [14 -18] applications, in addition to traditional detection of airborne volatiles [19 -23]. The recent advent of commercial FAIMS systems (Ionalytics Selectra [17,24] and Sionex DMS [23,25]) is increasing the acceptance of FAIMS and diversifying its applications.While FAIMS analyses have become increasingly common, the fundamentals remain relatively poorly understood [18]. Phenomenologically, ions are separated by the difference between mobilities at high and low electric fields (E) (respectively K H and K L ) that in general differ as ion mobilities in gases depend on the field. Thus, FAIMS measures the mean derivative of mobility with respect to field ͗ѨK⁄ѨE͘ (over a certain range of E), in contrast to the conventional ion mobility spectrometry [26,27] that determines absolute mobilities (K). The K(E) function can be expressed as a polynomial over even powers of E/N, where N is the buffer gas number density [28,29]:Mobilities tend to significantly deviate from zero-field values K(0) at E/N Ն ϳ30 to 40 Td, which defines the lower limit for electric fields useful in FAIMS operation. The upper limit is given by the onset of electrical breakdown in gas, which depends on the gas identity and number density, and (to a lesser extent) the width and geometry of the gap between electrodes (the...

show abstract

Separation of Cisplatin and Its Hydrolysis Products Using Electrospray Ionization High-Field Asymmetric Waveform Ion Mobility Spectrometry Coupled with Ion Trap Mass Spectrometry

Cited by 57 publications

References 39 publications

High-Resolution Field Asymmetric Waveform Ion Mobility Spectrometry Using New Planar Geometry Analyzers

High-Resolution Field Asymmetric Waveform Ion Mobility Spectrometry Using New Planar Geometry Analyzers

Feasibility of Higher-Order Differential Ion Mobility Separations Using New Asymmetric Waveforms

FAIMS operation for realistic gas flow profile and asymmetric waveforms including electronic noise and ripple

Contact Info

Product

Resources

About