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Kinetics of porphyrin adsorption and DNA-assisted desorption at the silica-water interface
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Zhang, Meiqin, Powell, Hayley V., Mackenzie, Stuart R. and Unwin, Patrick R. (2010) Kinetics of porphyrin adsorption and DNA-assisted desorption at the silica-water interface. Langmuir, Vol.26 (No.6). pp. 4004-4012. doi:10.1021/la903438p ISSN 0743-7463.
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Official URL: http://dx.doi.org/10.1021/la903438p
Abstract
Evanescent wave cavity ring-down spectroscopy (EW-CRDS) has been used to study in situ the kinetics of the adsorption of 5,10,15,20-tetrakis(4-N-methylpyridiniumyl)porphyin (TMPyP) from pH 7.4 phosphate buffer solution (PBS) to the silica-water interface and the interaction of calf thymus DNA (CT-DNA) with the resulting TMPyP-functionalized Surface. TMPyP was delivered to the silica surface using an impinging jet technique to allow relatively fast surface kinetics to be accessed. Adsorption was first-order in TM PyP, and the initial adsorption rate constant at the bare surface was found to be k = (4.1 +/- 0.6) x 10(-2) cm s(-1). A deceleration in the adsorption kinetics was observed at longer times that could be described semiquantitatively using an Elovich-type kinetic expression. The limiting value of the absorbance corresponded approximately to monolayer coverage (6.2 x 10(13) molecules cm(-2)). Exposure of the TMPyP-modified silica surface to CT-DNA, achieved by flowing CT-DNA solution over the functionalizcd surface, resulted in efficient desorption of the TMPyP. The desorption process was driven by the interaction of TMPyP with CT-DNA, which UV-vis spectroscopy indicated involved intercalative binding. The desorption kinetics were also simulated using complementary finite element modeling of convection-diffusion coupled to a surface process.
| Item Type: | Journal Article | ||||
|---|---|---|---|---|---|
| Subjects: | Q Science > QD Chemistry T Technology > TA Engineering (General). Civil engineering (General) |
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| Divisions: | Faculty of Science, Engineering and Medicine > Science > Chemistry | ||||
| Journal or Publication Title: | Langmuir | ||||
| Publisher: | American Chemical Society | ||||
| ISSN: | 0743-7463 | ||||
| Official Date: | 16 March 2010 | ||||
| Dates: |
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| Volume: | Vol.26 | ||||
| Number: | No.6 | ||||
| Number of Pages: | 9 | ||||
| Page Range: | pp. 4004-4012 | ||||
| DOI: | 10.1021/la903438p | ||||
| Status: | Peer Reviewed | ||||
| Publication Status: | Published | ||||
| Access rights to Published version: | Restricted or Subscription Access | ||||
| Funder: | Marie Curie Incoming International Fellowship, European Commission, Engineering and Physical Sciences Research Council (EPSRC), Advanced Research Fellowship, European Regional Development Fund (ERDF) | ||||
| Grant number: | 040126: "SECM-CRDS", EP/C00907X (EPSRC) |
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