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Rapid Hydrogen-Deuterium Exchange in Liquid Droplets
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - BMC, Analytical Chemistry. Stanford Univ, Dept Chem, Stanford, CA 94305 USA..ORCID iD: 0000-0002-0675-3412
Stanford Univ, Dept Chem, Stanford, CA 94305 USA..
Stanford Univ, Dept Mech Engn, Stanford, CA 94305 USA..
Stanford Univ, Dept Chem, Stanford, CA 94305 USA..
2017 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 139, no 20, p. 6851-6854Article in journal (Refereed) Published
Abstract [en]

The rate of hydrogen-deuterium exchange (HDX) in aqueous droplets of phenethylamine has been determined with submillisecond temporal resolution by mass spectrometry using nanoelectrospray ionization with a theta-capillary. The average speed of the micro droplets is measured using microparticle image velocimetry. The droplet travel time is varied from 20 to 320 mu s by changing the distance between the emitter and the heated inlet to the mass spectrometer and the voltage applied to the emitter source. The droplets were found to accelerate by similar to 30% during their observable travel time. Our droplet imaging shows that the theta-capillary produces two Taylor cone-jets (one per channel), causing mixing to take place from droplet fusion in the Taylor spray zone. Phenethylamine (phi CH2CH2NH2) was chosen to study because it has only one functional group (-NH2) that undergoes rapid HDX. We model the HDX with a system of ordinary differential equations. The rate constant for the formation of -NH2D+ from -NH3+ is 3660 +/- 290 s(-1), and the rate constant for the formation of -NHD2+ from -NH2D+ is 3330 +/- 270 s(-1). The observed rates are about 3 times faster than what has been reported for rapidly exchangeable peptide side-chain groups in bulk measurements using stopped-flow kinetics and NMR spectroscopy. We also applied this technique to determine the HDX rates for a small 10-residue peptide, angiotensin I, in aqueous droplets, from which we found a 7-fold acceleration of HDX in the droplet compared to that in bulk solution.

Place, publisher, year, edition, pages
2017. Vol. 139, no 20, p. 6851-6854
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:uu:diva-328178DOI: 10.1021/jacs.7b03541ISI: 000402498500018PubMedID: 28481522OAI: oai:DiVA.org:uu-328178DiVA, id: diva2:1134736
Funder
Swedish Research Council, 2015-00406Available from: 2017-08-21 Created: 2017-08-21 Last updated: 2017-08-21Bibliographically approved

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