Enumeration of Labile Hydrogens in Natural Organic Matter by Use of Hydrogen/Deuterium Exchange Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Kostyukevich, Yury; Kononikhin, Alexey; Popov, Igor; Kharybin, Oleg N.; Perminova, Irina V.; Konstantinov, Andrey I.; Nikolaev, E. N.

doi:10.1021/ac402609x

Cited by 65 publications

(79 citation statements)

References 19 publications

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“…All experiments were repeated at least three times, and the results were found to be reproducible. The effect of the position of the copper plate, ESI needle and the amount of the D 2 O was addressed in our previous papers …”

Section: Methodsmentioning

confidence: 99%

In ESI-source H/D exchange under atmospheric pressure for peptides and proteins of different molecular weights from 1 to 66 kDa: the role of the temperature of the desolvating capillary on H/D exchange

et al. 2015

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Transition of proteins from the solution to the gas phase during electrospray ionization remains a challenging problem despite the large amount of attention it has received during the past few decades. One of the major questions relates to the extent to which proteins in the gas phase retain their condensed phase structures. We have used in-electrospray source hydrogen/deuterium exchange to determine the number of deuterium incorporations as a function of protein mass, charge state and temperature of the desolvating capillary where the reaction occurs. All experiments were performed on a Thermo LTQ FT Ultra equipped with a 7-T superconducting magnet. Ions were generated by an IonMax Electrospray ion source operated in the positive ESI mode. Deuterium exchange was performed by introducing a droplet of D2 O beneath the ESI capillary. We systematically investigated gas phase hydrogen/deuterium (H/D) exchange under atmospheric pressure for peptides and proteins of different molecular weights from 1 to 66 kDa. We observed that almost all proteins demonstrate similar exchange rates for all charge states and that these rates increase exponentially with the temperature of the desolvating capillary. We did not observe any clear correlation of the number of H/D exchanges with the value of the cross section for a corresponding charge state. We have demonstrated the possibility of performing in-ESI source H/D exchange of large proteins under atmospheric pressure. The simplicity of the experimental setup makes it a useful experimental technique that can be applied for the investigation of gas phase conformations of proteins.

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Section: Methodsmentioning

confidence: 99%

In ESI-source H/D exchange under atmospheric pressure for peptides and proteins of different molecular weights from 1 to 66 kDa: the role of the temperature of the desolvating capillary on H/D exchange

et al. 2015

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“…Данная реакция позволяет делать определенные выво-ды о структуре и о конформации ионов в газовой фазе. Ранее методика проведения реакции дейтеро/водород-ного обмена в газовой фазе при атмосферном давлении прямо во время процесса ионизации [13] была успешно применена для структурного исследования широко-го класса различных соединений, таких как пепти-ды, [14,15] белки, сахара, [16,17] малые органические молеку-лы, [18][19][20][21][22] сложные природные субстанции [23,24] и олиго-нуклеотиды. [25] Результаты анализа реакции дейтеро/водородного обмена для комплексов β-циклодекстрина с Ce 3+ приведены в Таблице 1.…”

Section: результаты и обсуждениеunclassified

Investigation of Ion–Molecular Complexes of beta–Cyclodextrin with Proteins and Metals in Gas Phase

Kostyukevich¹,

Kononikhin²,

Бугрова³

et al. 2017

MHC

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“…The first such experiments were performed by using thermospray and electrospray . Later the H/D exchange reaction in the course of ionization process was demonstrated by many other researchers for ESI, APCI, APPI, and other types of ion sources . The performing of the isotope exchange reactions directly during ionization has the advantage of the experimental simplicity, possibility to be carried out on any commercial mass spectrometer and lack of the need of the sample preparation.…”

Section: Introductionmentioning

confidence: 99%

Hydrogen/deuterium exchange in mass spectrometry

Kostyukevich

Acter

Zherebker

et al. 2018

Mass Spectrometry Reviews

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The isotopic exchange approach is in use since the first observation of such reactions in 1933 by Lewis. This approach allows the investigation of the pathways of chemical and biochemical reactions, determination of structure, composition, and conformation of molecules. Mass spectrometry has now become one of the most important analytical tools for the monitoring of the isotopic exchange reactions. Investigation of conformational dynamics of proteins, quantitative measurements, obtaining chemical, and structural information about individual compounds of the complex natural mixtures are mainly based on the use of isotope exchange in combination with high resolution mass spectrometry. The most important reaction is the Hydrogen/Deuterium exchange, which is mainly performed in the solution. Recently we have developed the approach allowing performing of the Hydrogen/Deuterium reaction on-line directly in the ionization source under atmospheric pressure. Such approach simplifies the sample preparation and can accelerate the exchange reaction so that certain hydrogens that are considered as non-labile will also participate in the exchange. The use of in-ionization source H/D exchange in modern mass spectrometry for structural elucidation of molecules serves as the basic theme in this review. We will focus on the mechanisms of the isotopic exchange reactions and on the application of in-ESI, in-APCI, and in-APPI source Hydrogen/Deuterium exchange for the investigation of petroleum, natural organic matter, oligosaccharides, and proteins including protein-protein complexes. The simple scenario for adaptation of H/D exchange reactions into mass spectrometric method is also highlighted along with a couple of examples collected from previous studies.

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Enumeration of Labile Hydrogens in Natural Organic Matter by Use of Hydrogen/Deuterium Exchange Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

Cited by 65 publications

References 19 publications

In ESI-source H/D exchange under atmospheric pressure for peptides and proteins of different molecular weights from 1 to 66 kDa: the role of the temperature of the desolvating capillary on H/D exchange

In ESI-source H/D exchange under atmospheric pressure for peptides and proteins of different molecular weights from 1 to 66 kDa: the role of the temperature of the desolvating capillary on H/D exchange

Investigation of Ion–Molecular Complexes of beta–Cyclodextrin with Proteins and Metals in Gas Phase

Hydrogen/deuterium exchange in mass spectrometry

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