Pulsed Nanoelectrospray Ionization Boosts Ion Signal in Whole Protein Mass Spectrometry

Electrospray ionisation (ESI) is renowned for its ability to ionise intact proteins for sensitive detection by mass spectrometry (MS). However, the use of a conventional direct current ESI voltage can result in the formation of relatively large initial droplet sizes, which can limit efficient ion de...

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Autores principales:	Qinwen Liu, Ezaz Ahmed, K. M. Mohibul Kabir, Xiaojing Huang, Dan Xiao, John Fletcher, William A. Donald
Formato:	article
Lenguaje:	EN
Publicado:	MDPI AG 2021
Materias:	electrospray ionisation nanoelectrospray proteins alternating current top-down Technology T Engineering (General). Civil engineering (General) TA1-2040 Biology (General) QH301-705.5 Physics QC1-999 Chemistry QD1-999
Acceso en línea:	https://doaj.org/article/d45ea3fe47ff4c2290949a0095962ced
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spelling	oai:doaj.org-article:d45ea3fe47ff4c2290949a0095962ced2021-11-25T16:39:58ZPulsed Nanoelectrospray Ionization Boosts Ion Signal in Whole Protein Mass Spectrometry10.3390/app1122108832076-3417https://doaj.org/article/d45ea3fe47ff4c2290949a0095962ced2021-11-01T00:00:00Zhttps://www.mdpi.com/2076-3417/11/22/10883https://doaj.org/toc/2076-3417Electrospray ionisation (ESI) is renowned for its ability to ionise intact proteins for sensitive detection by mass spectrometry (MS). However, the use of a conventional direct current ESI voltage can result in the formation of relatively large initial droplet sizes, which can limit efficient ion desolvation and sensitivity. Here, pulsed nanoESI (nESI) MS using nanoscale emitters with inner diameters of ~250 nm is reported. In this approach, the nESI voltage is rapidly pulsed from 0 to ~1.5 kV with sub-nanosecond rise times, duty cycles from 10 to 90%, and repetition rates of 10 to 350 kHz. Using pulsed nESI, the performance of MS for the detection of intact proteins can be improved in terms of increased ion abundances and decreased noise. The absolute ion abundances and signal-to-noise levels of protonated ubiquitin, cytochrome C, myoglobin, and carbonic anhydrase II formed from standard denaturing solutions can be increased by up to 82% and 154% using an optimal repetition rate of ~200 kHz compared to conventional nESI-MS. Applying pulsed nESI-MS to a mixture of four proteins resulted in the signal for each protein increasing by up to 184% compared to the more conventional nESI-MS. For smaller ions (≤1032 <i>m</i>/<i>z</i>), the signal can also be increased by the use of high repetition rates (200–250 kHz), which is consistent with the enhanced performance depending more on general factors associated with the ESI process (e.g., smaller initial droplet sizes and reduced Coulombic repulsion in the spray plume) rather than analyte-specific effects (e.g., electrophoretic mobility). The enhanced sensitivity of pulsed nESI is anticipated to be beneficial for many different types of tandem mass spectrometry measurements.Qinwen LiuEzaz AhmedK. M. Mohibul KabirXiaojing HuangDan XiaoJohn FletcherWilliam A. DonaldMDPI AGarticleelectrospray ionisationnanoelectrosprayproteinsalternating currenttop-downTechnologyTEngineering (General). Civil engineering (General)TA1-2040Biology (General)QH301-705.5PhysicsQC1-999ChemistryQD1-999ENApplied Sciences, Vol 11, Iss 10883, p 10883 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	electrospray ionisation nanoelectrospray proteins alternating current top-down Technology T Engineering (General). Civil engineering (General) TA1-2040 Biology (General) QH301-705.5 Physics QC1-999 Chemistry QD1-999
spellingShingle	electrospray ionisation nanoelectrospray proteins alternating current top-down Technology T Engineering (General). Civil engineering (General) TA1-2040 Biology (General) QH301-705.5 Physics QC1-999 Chemistry QD1-999 Qinwen Liu Ezaz Ahmed K. M. Mohibul Kabir Xiaojing Huang Dan Xiao John Fletcher William A. Donald Pulsed Nanoelectrospray Ionization Boosts Ion Signal in Whole Protein Mass Spectrometry
description	Electrospray ionisation (ESI) is renowned for its ability to ionise intact proteins for sensitive detection by mass spectrometry (MS). However, the use of a conventional direct current ESI voltage can result in the formation of relatively large initial droplet sizes, which can limit efficient ion desolvation and sensitivity. Here, pulsed nanoESI (nESI) MS using nanoscale emitters with inner diameters of ~250 nm is reported. In this approach, the nESI voltage is rapidly pulsed from 0 to ~1.5 kV with sub-nanosecond rise times, duty cycles from 10 to 90%, and repetition rates of 10 to 350 kHz. Using pulsed nESI, the performance of MS for the detection of intact proteins can be improved in terms of increased ion abundances and decreased noise. The absolute ion abundances and signal-to-noise levels of protonated ubiquitin, cytochrome C, myoglobin, and carbonic anhydrase II formed from standard denaturing solutions can be increased by up to 82% and 154% using an optimal repetition rate of ~200 kHz compared to conventional nESI-MS. Applying pulsed nESI-MS to a mixture of four proteins resulted in the signal for each protein increasing by up to 184% compared to the more conventional nESI-MS. For smaller ions (≤1032 <i>m</i>/<i>z</i>), the signal can also be increased by the use of high repetition rates (200–250 kHz), which is consistent with the enhanced performance depending more on general factors associated with the ESI process (e.g., smaller initial droplet sizes and reduced Coulombic repulsion in the spray plume) rather than analyte-specific effects (e.g., electrophoretic mobility). The enhanced sensitivity of pulsed nESI is anticipated to be beneficial for many different types of tandem mass spectrometry measurements.
format	article
author	Qinwen Liu Ezaz Ahmed K. M. Mohibul Kabir Xiaojing Huang Dan Xiao John Fletcher William A. Donald
author_facet	Qinwen Liu Ezaz Ahmed K. M. Mohibul Kabir Xiaojing Huang Dan Xiao John Fletcher William A. Donald
author_sort	Qinwen Liu
title	Pulsed Nanoelectrospray Ionization Boosts Ion Signal in Whole Protein Mass Spectrometry
title_short	Pulsed Nanoelectrospray Ionization Boosts Ion Signal in Whole Protein Mass Spectrometry
title_full	Pulsed Nanoelectrospray Ionization Boosts Ion Signal in Whole Protein Mass Spectrometry
title_fullStr	Pulsed Nanoelectrospray Ionization Boosts Ion Signal in Whole Protein Mass Spectrometry
title_full_unstemmed	Pulsed Nanoelectrospray Ionization Boosts Ion Signal in Whole Protein Mass Spectrometry
title_sort	pulsed nanoelectrospray ionization boosts ion signal in whole protein mass spectrometry
publisher	MDPI AG
publishDate	2021
url	https://doaj.org/article/d45ea3fe47ff4c2290949a0095962ced
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_version_	1718413106012487680

Pulsed Nanoelectrospray Ionization Boosts Ion Signal in Whole Protein Mass Spectrometry

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