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Microdroplet fusion mass spectrometry for fast reaction kinetics

Title
Microdroplet fusion mass spectrometry for fast reaction kinetics
Authors
Lee, JK[Lee, Jae Kyoo]Kim, S[Kim, Samuel]Nam, HG[Nam, Hong Gil]Zare, RN[Zare, Richard N.]
DGIST Authors
Nam, HG[Nam, Hong Gil]
Issue Date
2015-03-31
Citation
Proceedings of the National Academy of Sciences of the United States of America, 112(13), 3898-3903
Type
Article
Article Type
Article
Keywords
2,6 DichlorophenolindophenolAbsorption SpectroscopyAscorbic AcidBradykininCameraChemical Reaction KineticsCytochrome CDeuteriumEvaporationHydrogenHydrogen-Deuterium Isotope ExchangeIon CurrentLiquid MicrodropletsMass SpectrometerMass SpectrometryMicrodroplet Fusion Mass SpectrometrypHPriority JournalProtein FoldingProtein UnfoldingReaction KineticsReaction TimeWater
ISSN
0027-8424
Abstract
We investigated the fusion of high-speed liquid droplets as a way to record the kinetics of liquid-phase chemical reactions on the order of microseconds. Two streams of micrometer-size droplets collide with one another. The droplets that fused (13 μm in diameter) at the intersection of the two streams entered the heated capillary inlet of a mass spectrometer. The mass spectrum was recorded as a function of the distance x between the mass spectrometer inlet and the droplet fusion center. Fused droplet trajectories were imaged with a high-speed camera, revealing that the droplet fusion occurred approximately within a 500-μm radius from the droplet fusion center and both the size and the speed of the fused droplets remained relatively constant as they traveled from the droplet fusion center to the mass spectrometer inlet. Evidence is presented that the reaction effectively stops upon entering the heated inlet of the mass spectrometer. Thus, the reaction time was proportional to x and could be measured and manipulated by controlling the distance x. Kinetic studies were carried out in fused water droplets for acid-induced unfolding of cytochrome c and hydrogen-deuterium exchange in bradykinin. The kinetics of the former revealed the slowing of the unfolding rates at the early stage of the reaction within 50 μs. The hydrogen- deuterium exchange revealed the existence of two distinct populations with fast and slow exchange rates. These studies demonstrated the power of this technique to detect reaction intermediates in fused liquid droplets with microsecond temporal resolution.
URI
http://hdl.handle.net/20.500.11750/1664
DOI
10.1073/pnas.1503689112
Publisher
National Academy of Sciences
Related Researcher
Files:
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Collection:
New BiologyETC1. Journal Articles


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