Interfacial electron shuttling processes across Kolliphor®EL monolayer grafted electrodes

Khadijeh Nekoueian; Christopher E Hotchen; Mandana Amiri; Mika Sillanpää; Geoffrey W Nelson; John S Foord; Philip Holdway; Antoine Buchard; Stephen C Parker; Frank Marken

doi:10.1021/acsami.5b03654

Interfacial electron shuttling processes across Kolliphor®EL monolayer grafted electrodes

Khadijeh Nekoueian, Christopher E Hotchen, Mandana Amiri, Mika Sillanpää, Geoffrey W Nelson, John S Foord, Philip Holdway, Antoine Buchard, Stephen C Parker, Frank Marken

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Abstract

Covalently grafted Kolliphor®EL (a poly-ethylene-glycol based "transporter molecule" for hydrophobic water-insoluble drugs; MW ca. 2486; diameter ca. 3-5 nm) at the surface of a glassy carbon electrode strongly affects the rate of electron transfer for aqueous redox systems such as Fe(CN)63-/4-. XPS data confirm mono-layer grafting after electrochemical anodisation in pure Kolliphor®EL. Based on voltammetry and impedance measurements, the charge transfer process for the Fe(CN)63-/4- probe molecule is completely blocked after Kolliphor®EL grafting and in the absence of a "guest". However, in the presence of low concentrations of suitable ferrocene derivatives as "guests", mediated electron transfer across the mono-layer via a "shuttle mechanism" is observed. The resulting amplification of the ferrocene electroanalytical signal is investigated systematically and compared for 5 ferrocene derivatives. The low concentration electron shuttle efficiency decreases in the sequence dimethylaminomethyl-ferrocene > n-butyl-ferrocene > ferrocene-dimethanol > ferrocene-acetonitrile > ferrocene-acetic acid.

Original language	English
Pages (from-to)	15458-15465
Journal	ACS Applied Materials and Interfaces
Volume	7
Issue number	28
Early online date	9 Jul 2015
DOIs	https://doi.org/10.1021/acsami.5b03654
Publication status	Published - 22 Jul 2015

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Kolliphor_Manuscript_Feb2015_f_revision_nh
This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials and Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/acsami.5b03654
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@article{7efacdea5afe4609a0dc180bf1efb08d,

title = "Interfacial electron shuttling processes across Kolliphor{\textregistered}EL monolayer grafted electrodes",

abstract = "Covalently grafted Kolliphor{\textregistered}EL (a poly-ethylene-glycol based {"}transporter molecule{"} for hydrophobic water-insoluble drugs; MW ca. 2486; diameter ca. 3-5 nm) at the surface of a glassy carbon electrode strongly affects the rate of electron transfer for aqueous redox systems such as Fe(CN)63-/4-. XPS data confirm mono-layer grafting after electrochemical anodisation in pure Kolliphor{\textregistered}EL. Based on voltammetry and impedance measurements, the charge transfer process for the Fe(CN)63-/4- probe molecule is completely blocked after Kolliphor{\textregistered}EL grafting and in the absence of a {"}guest{"}. However, in the presence of low concentrations of suitable ferrocene derivatives as {"}guests{"}, mediated electron transfer across the mono-layer via a {"}shuttle mechanism{"} is observed. The resulting amplification of the ferrocene electroanalytical signal is investigated systematically and compared for 5 ferrocene derivatives. The low concentration electron shuttle efficiency decreases in the sequence dimethylaminomethyl-ferrocene > n-butyl-ferrocene > ferrocene-dimethanol > ferrocene-acetonitrile > ferrocene-acetic acid.",

author = "Khadijeh Nekoueian and Hotchen, {Christopher E} and Mandana Amiri and Mika Sillanp{\"a}{\"a} and Nelson, {Geoffrey W} and Foord, {John S} and Philip Holdway and Antoine Buchard and Parker, {Stephen C} and Frank Marken",

year = "2015",

month = jul,

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doi = "10.1021/acsami.5b03654",

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journal = "ACS Applied Materials and Interfaces",

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T1 - Interfacial electron shuttling processes across Kolliphor®EL monolayer grafted electrodes

AU - Nekoueian, Khadijeh

AU - Hotchen, Christopher E

AU - Amiri, Mandana

AU - Sillanpää, Mika

AU - Nelson, Geoffrey W

AU - Foord, John S

AU - Holdway, Philip

AU - Buchard, Antoine

AU - Parker, Stephen C

AU - Marken, Frank

PY - 2015/7/22

Y1 - 2015/7/22

N2 - Covalently grafted Kolliphor®EL (a poly-ethylene-glycol based "transporter molecule" for hydrophobic water-insoluble drugs; MW ca. 2486; diameter ca. 3-5 nm) at the surface of a glassy carbon electrode strongly affects the rate of electron transfer for aqueous redox systems such as Fe(CN)63-/4-. XPS data confirm mono-layer grafting after electrochemical anodisation in pure Kolliphor®EL. Based on voltammetry and impedance measurements, the charge transfer process for the Fe(CN)63-/4- probe molecule is completely blocked after Kolliphor®EL grafting and in the absence of a "guest". However, in the presence of low concentrations of suitable ferrocene derivatives as "guests", mediated electron transfer across the mono-layer via a "shuttle mechanism" is observed. The resulting amplification of the ferrocene electroanalytical signal is investigated systematically and compared for 5 ferrocene derivatives. The low concentration electron shuttle efficiency decreases in the sequence dimethylaminomethyl-ferrocene > n-butyl-ferrocene > ferrocene-dimethanol > ferrocene-acetonitrile > ferrocene-acetic acid.

AB - Covalently grafted Kolliphor®EL (a poly-ethylene-glycol based "transporter molecule" for hydrophobic water-insoluble drugs; MW ca. 2486; diameter ca. 3-5 nm) at the surface of a glassy carbon electrode strongly affects the rate of electron transfer for aqueous redox systems such as Fe(CN)63-/4-. XPS data confirm mono-layer grafting after electrochemical anodisation in pure Kolliphor®EL. Based on voltammetry and impedance measurements, the charge transfer process for the Fe(CN)63-/4- probe molecule is completely blocked after Kolliphor®EL grafting and in the absence of a "guest". However, in the presence of low concentrations of suitable ferrocene derivatives as "guests", mediated electron transfer across the mono-layer via a "shuttle mechanism" is observed. The resulting amplification of the ferrocene electroanalytical signal is investigated systematically and compared for 5 ferrocene derivatives. The low concentration electron shuttle efficiency decreases in the sequence dimethylaminomethyl-ferrocene > n-butyl-ferrocene > ferrocene-dimethanol > ferrocene-acetonitrile > ferrocene-acetic acid.

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DO - 10.1021/acsami.5b03654

M3 - Article

C2 - 26104182

SN - 1944-8244

VL - 7

SP - 15458

EP - 15465

JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

IS - 28

ER -

Interfacial electron shuttling processes across Kolliphor®EL monolayer grafted electrodes

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Frank Marken

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Interfacial electron shuttling processes across Kolliphor®EL monolayer grafted electrodes

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