Single-molecule chemical reaction reveals molecular reaction kinetics and dynamics

Zhang, Yuwei; Song, Ping; Fu, Qiang; Ruan, Mingbo; Xu, Weilin

doi:10.1038/ncomms5238

Cited by 32 publications

(44 citation statements)

References 48 publications

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“…In the conditions implemented in this article, it can be shown that the first term D r Á @C @r could be neglected. Equation 18 was further reduced to:…”

Section: Modeling Methodsmentioning

confidence: 99%

“…Based on the literature background, 17,18 one can assume that this colorimetric reaction is of a global order 2, with respect to the oxygen and to the dihydroresorufin. The rate of consumption of dihydroresorufin, r B (or the rate of consumption of oxygen r O2 ) is then expressed as:…”

Section: About the Kinetics Of The Colorimetric Reactionmentioning

confidence: 99%

“…Based on the literature background, one can assume that this colorimetric reaction is of a global order 2, with respect to the oxygen and to the dihydroresorufin. The rate of consumption of dihydroresorufin,

r_{B}

(or the rate of consumption of oxygen

r_{O_{2}}

) is then expressed as:

r_{B} = - ν \cdot k_{2} \cdot C_{O_{2}} \cdot C_{B} = ν \cdot r_{O_{2}} .

where

k_{2}

is the reaction rate constant (m 3 ·mol −1 ·s −1 ) and

ν

the stoichiometric coefficient equal to 2.…”

Section: Introductionmentioning

confidence: 99%

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Optical methods to investigate the enhancement factor of an oxygen‐sensitive colorimetric reaction using microreactors

et al. 2016

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OATAO is an open access repository that collects the work of Toulouse researchers and makes it freely available over the web where possible. This is an author-deposited version published in : http://oatao. Abstract: Visualization of mass transfer is a powerful tool to improve understanding of local phenomenon. The use of an oxygen-sensitive dye (colorimetric technique 1 ) has showed its relevancy for locally visualizing and characterizing gas-liquid mass transfer at different scales 2,3 . At present, the occurrence of a possible enhancement of the gas-liquid mass transfer by this reaction has not been yet demonstrated. This paper aims at filling this gap by evaluating the Hatta number Ha and the enhancement factor E associated with the oxygen colorimetric reaction when implementing in milli/micro channels. For that, as data on the kinetic of the colorimetric reaction are seldom in the literature, the reaction characteristic time was firstly estimated by carrying out experiments in a microchannel equipped with a micromixer. The diffusion coefficients of dihydroresorufin and O 2 were then determined by implementing two original optical methods in a specific coflow microchannel device, coupled with theoretical modelling. The knowledge of these parameters enabled at last to demonstrate that no enhancement of the gas-liquid mass transfer by this colorimetric reaction existed.Complementary information about the reliability of the colorimetric technique to characterize the gasliquid mass transfer in milli/micro systems was also given.

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“…In the conditions implemented in this article, it can be shown that the first term D r Á @C @r could be neglected. Equation 18 was further reduced to:…”

Section: Modeling Methodsmentioning

confidence: 99%

Section: About the Kinetics Of The Colorimetric Reactionmentioning

confidence: 99%

r_{B}

(or the rate of consumption of oxygen

r_{O_{2}}

) is then expressed as:

r_{B} = - ν \cdot k_{2} \cdot C_{O_{2}} \cdot C_{B} = ν \cdot r_{O_{2}} .

where

k_{2}

is the reaction rate constant (m 3 ·mol −1 ·s −1 ) and

ν

the stoichiometric coefficient equal to 2.…”

Section: Introductionmentioning

confidence: 99%

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Optical methods to investigate the enhancement factor of an oxygen‐sensitive colorimetric reaction using microreactors

et al. 2016

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“…Understanding the elementary process of chemical reactions in condensed phase is significant for improvement of efficiencies in industries. Recently, in our lab, by combining with quantum chemical calculation, single-molecule fluorescence microscopy was adopted successfully to gain new insights into elementary reactions in condensed phase [57]. This work was done based on an observation of a highly reversible redox process: a fluorescent Resorufin molecule can be reduced to non-fluorescent dihydro-Resorufin by reductant of sodium borohydride (NaBH 4 ), while the dihydro-Resorufin can be oxidized back to fluorescent Resorufin easily by oxygen (Fig.…”

Section: Revealing Molecular Reaction Kinetics and Dynamics Of Elemenmentioning

confidence: 99%

Recent progress on single-molecule nanocatalysis based on single-molecule fluorescence microscopy

et al. 2017

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“…[23][24][25][26] While background fluorescence is ac ommon obstacle in single-molecule fluorescence microscopy,asingle fluorescence molecule exhibiting ac ontrolled unique blinking pattern can be readily read out even against ah igh-fluorescence background. Blinking can occur in response to various chemical reactions and is involved in super-resolution microscopy.…”

mentioning

confidence: 99%

Single‐Molecule Monitoring of the Structural Switching Dynamics of Nucleic Acids through Controlling Fluorescence Blinking

et al. 2017

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Single-molecule fluorescence resonance energy transfer (smFRET) is ap owerful tool to investigate the dynamics of biomolecular events in real time.H owever,i t requires two fluorophores and can be applied only to dynamics that accompany large changes in distance between the molecules.Herein, we introduce amethod for kinetic analysis based on control of fluorescence blinking (KACB), ag eneral approach to investigate the dynamics of biomolecules by using as ingle fluorophore.B yc ontrolling the kinetics of the redox reaction the blinking kinetics or pattern can be controlled to be affected by microenvironmental changes around af luorophore (rKACB), therebye nabling real-time single-molecule measurement of the structure-changing dynamics of nucleic acids.Advances in single-molecule fluorescence microscopy in the last two decades have allowed us to reveal many important biochemical and cellular processes. [1][2][3][4][5] Single-molecule fluorescence measurement is especially effective for investigating the dynamic reaction and motion of biomolecules. [6][7][8][9][10] One of the most successful approaches is the observation of fluorescence resonance energy transfer between as ingle pair of fluorophores (smFRET). [11][12][13][14] Thed ynamics of distance changes between two sites on biomolecules or between two different molecules can be measured by monitoring timedependent fluctuation in the donor and acceptor fluorescence signals.T his information is usually inaccessible in ensemble measurements due to al ack of synchronization of dynamic motions or of the reactions of biomolecules.While smFRET is ap owerful tool and offers fruitful information on various dynamic reactions and the motions of biomolecules,itnevertheless has two disadvantages.O ne is that it can be applied only to dynamics that accompany large distance changes between two fluorophores (> 2nm). Theother is the need to label biomolecules with two fluorophores.T hus the development of am ethod that requires the labeling of only as ingle fluorophore to provide dynamic information on biomolecules is highly desired.To date,c hemists have developed various environmentsensitive fluorophores. [15][16][17][18][19][20] These fluorophores undergo fluorescence intensity and lifetime changes or spectral shifts related to microenvironmental changes around the fluorophore.E nvironment-sensitive changes in the fluorescence intensity and lifetime of Cy3 have been successfully applied to the observation of the dynamics of protein-nucleic acid interactions. [21,22] However, it is still often challenging to achieve sufficient time resolution in single-molecule dynamic analysis based on environment-sensitive fluorophores.Fluorescent signals from asingle fluorophore often blink, reflecting time-dependent fluctuations between bright (ON) and dark (OFF) states. [23][24][25][26] While background fluorescence is ac ommon obstacle in single-molecule fluorescence microscopy,asingle fluorescence molecule exhibiting ac ontrolled unique blinking pattern can be readily read ...

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Single-molecule chemical reaction reveals molecular reaction kinetics and dynamics

Cited by 32 publications

References 48 publications

Optical methods to investigate the enhancement factor of an oxygen‐sensitive colorimetric reaction using microreactors

Optical methods to investigate the enhancement factor of an oxygen‐sensitive colorimetric reaction using microreactors

Recent progress on single-molecule nanocatalysis based on single-molecule fluorescence microscopy

Single‐Molecule Monitoring of the Structural Switching Dynamics of Nucleic Acids through Controlling Fluorescence Blinking

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