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Title: Biofouling affects the redox kinetics of outer and inner sphere probes on carbon surfaces drastically differently – implications to biosensing

Abstract

Biofouling imposes a significant threat for sensing probes used in vivo. Antifouling strategies commonly utilize a protective layer on top of the electrode but this may compromise performance of the electrode. Here, we investigated the effect of surface topography and chemistry on fouling without additional protective layers. We have utilized two different carbon materials; tetrahedral amorphous carbon (ta-C) and SU-8 based pyrolytic carbon (PyC) in their typical smooth thin film structure as well as with a nanopillar topography templated from black silicon. The near edge X-ray absorption fine structure (NEXAFS) spectrum revealed striking differences in chemical functionalities of the surfaces. PyC contained equal amounts of ketone, hydroxyl and ether/epoxide groups, while ta-C contained significant amounts of carbonyl groups. Overall, oxygen functionalities were significantly increased on nanograss surfaces compared to the flat counterparts. Neither bovine serum albumin (BSA) or fetal bovine serum (FBS) fouling caused major effects on electron transfer kinetics of outer sphere redox (OSR) probe Ru(NH3)63+ on any of the materials. In contrast, negatively charged OSR probe IrCl62– kinetics were clearly affected by fouling, possibly due to the electrostatic repulsion between redox species and the anionically-charged proteins adsorbed on the electrode and/or stronger interaction of the proteins and positivelymore » charged surface. The OSR probe kinetics were less affected by fouling on PyC, probably due to conformational changes of proteins on the surface. Dopamine (DA) was tested as an inner sphere redox (ISR) probe and as expected, the kinetics were heavily dependent on the material; PyC had very fast electron transfer kinetics, while ta-C had sluggish kinetics. DA electron transfer kinetics were heavily affected on all surfaces by fouling (ΔEp increase 30–451%). The effect was stronger on PyC, possibly due to the more strongly adhered protein layer limiting the access of the probe to the inner sphere.« less

Authors:
ORCiD logo [1];  [1];  [2]; ORCiD logo [3];  [3]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [1]
  1. Department of Electrical Engineering and Automation, School of Electrical Engineering, Aalto University, Espoo, Finland
  2. Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, USA, Microelectronics Research Unit
  3. Department of Chemistry and Materials Science, School of Chemical Technology, Aalto University, Espoo, Finland
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Academy of Finland; Business Finland; European Union (EU)
OSTI Identifier:
1638527
Alternate Identifier(s):
OSTI ID: 1656549
Grant/Contract Number:  
AC02-76SF00515; 321996; 328854; 2117731; 841621
Resource Type:
Published Article
Journal Name:
Physical Chemistry Chemical Physics. PCCP
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Volume: 22 Journal Issue: 29; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Peltola, Emilia, Aarva, Anja, Sainio, Sami, Heikkinen, Joonas J., Wester, Niklas, Jokinen, Ville, Koskinen, Jari, and Laurila, Tomi. Biofouling affects the redox kinetics of outer and inner sphere probes on carbon surfaces drastically differently – implications to biosensing. United Kingdom: N. p., 2020. Web. doi:10.1039/D0CP02251A.
Peltola, Emilia, Aarva, Anja, Sainio, Sami, Heikkinen, Joonas J., Wester, Niklas, Jokinen, Ville, Koskinen, Jari, & Laurila, Tomi. Biofouling affects the redox kinetics of outer and inner sphere probes on carbon surfaces drastically differently – implications to biosensing. United Kingdom. https://doi.org/10.1039/D0CP02251A
Peltola, Emilia, Aarva, Anja, Sainio, Sami, Heikkinen, Joonas J., Wester, Niklas, Jokinen, Ville, Koskinen, Jari, and Laurila, Tomi. Wed . "Biofouling affects the redox kinetics of outer and inner sphere probes on carbon surfaces drastically differently – implications to biosensing". United Kingdom. https://doi.org/10.1039/D0CP02251A.
@article{osti_1638527,
title = {Biofouling affects the redox kinetics of outer and inner sphere probes on carbon surfaces drastically differently – implications to biosensing},
author = {Peltola, Emilia and Aarva, Anja and Sainio, Sami and Heikkinen, Joonas J. and Wester, Niklas and Jokinen, Ville and Koskinen, Jari and Laurila, Tomi},
abstractNote = {Biofouling imposes a significant threat for sensing probes used in vivo. Antifouling strategies commonly utilize a protective layer on top of the electrode but this may compromise performance of the electrode. Here, we investigated the effect of surface topography and chemistry on fouling without additional protective layers. We have utilized two different carbon materials; tetrahedral amorphous carbon (ta-C) and SU-8 based pyrolytic carbon (PyC) in their typical smooth thin film structure as well as with a nanopillar topography templated from black silicon. The near edge X-ray absorption fine structure (NEXAFS) spectrum revealed striking differences in chemical functionalities of the surfaces. PyC contained equal amounts of ketone, hydroxyl and ether/epoxide groups, while ta-C contained significant amounts of carbonyl groups. Overall, oxygen functionalities were significantly increased on nanograss surfaces compared to the flat counterparts. Neither bovine serum albumin (BSA) or fetal bovine serum (FBS) fouling caused major effects on electron transfer kinetics of outer sphere redox (OSR) probe Ru(NH3)63+ on any of the materials. In contrast, negatively charged OSR probe IrCl62– kinetics were clearly affected by fouling, possibly due to the electrostatic repulsion between redox species and the anionically-charged proteins adsorbed on the electrode and/or stronger interaction of the proteins and positively charged surface. The OSR probe kinetics were less affected by fouling on PyC, probably due to conformational changes of proteins on the surface. Dopamine (DA) was tested as an inner sphere redox (ISR) probe and as expected, the kinetics were heavily dependent on the material; PyC had very fast electron transfer kinetics, while ta-C had sluggish kinetics. DA electron transfer kinetics were heavily affected on all surfaces by fouling (ΔEp increase 30–451%). The effect was stronger on PyC, possibly due to the more strongly adhered protein layer limiting the access of the probe to the inner sphere.},
doi = {10.1039/D0CP02251A},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 29,
volume = 22,
place = {United Kingdom},
year = {Wed Jul 29 00:00:00 EDT 2020},
month = {Wed Jul 29 00:00:00 EDT 2020}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/D0CP02251A

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Cited by: 7 works
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