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Microdroplet fusion mass spectrometry: Accelerated kinetics of acid-induced chlorophyll demetallation

Title
Microdroplet fusion mass spectrometry: Accelerated kinetics of acid-induced chlorophyll demetallation
Authors
Lee, Jae KyooNam, Hong GilZare, Richard N.
DGIST Authors
Nam, Hong Gil
Issue Date
2017-02
Citation
Quarterly Reviews of Biophysics, 50, 1-7
Type
Article
Article Type
Review
Keywords
Charged MicrodropletsElectrosprayNeat WaterWater Surface
ISSN
0033-5835
Abstract
Kinetics of acid-induced chlorophyll demetallation was recorded in microdroplets by fusing a stream of microdroplets containing 40 μM chlorophyll a or b dissolved in methanol with a stream of aqueous microdroplets containing 35 mM hydrochloric acid (pH = 1-46). The kinetics of the demetallation of chlorophyll in the fused microdroplets (14 ± 6 μm diameter; 84 ± 18 m s-1 velocity) was recorded by controlling the traveling distance of the fused microdroplets between the fusion region and the inlet of a mass spectrometer. The rate of acid-induced chlorophyll demetallation was about 960 ± 120 times faster in the charged microdroplets compared with that reported in bulk solution. If no voltage was applied to the sprayed microdroplets, then the acceleration factor was about 580 ± 90, suggesting that the applied voltage is not a major factor determining the acceleration. Chlorophyll a was more rapidly demetallated than chlorophyll b by a factor of ∼26 in bulk solution and ∼5 in charged microdroplets. The demetallation kinetics was second order in the H+ concentration, but the acceleration factor of microdroplets compared with bulk solution appeared to be unchanged in going from pH = 1-3 to 7-0. The water:methanol ratio of the fused microdroplets was varied from 7:3 to 3:7 causing an increase in the reaction rate of chlorophyll a demetallation by 20%. This observation demonstrates that the solvent composition, which has different evaporation rates, does not significantly affect the acceleration. We believe that a major portion of the acceleration can be attributed to confinement effects involving surface reactions rather than either to evaporation of solvents or to the introduction of charges to the microdroplets. © Cambridge University Press 2017.
URI
http://hdl.handle.net/20.500.11750/4240
DOI
10.1017/S0033583517000014
Publisher
Cambridge University Press
Related Researcher
Files:
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Collection:
New BiologyCBRG(Complex Biology Research Group)1. Journal Articles


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