Single Molecule Force Spectroscopy of Smart Poly(ferrocenylsilane) Macromolecules: Towards Highly Controlled Redox-Driven Single Chain Motors

S(han) Zou; I. Korczagin; Mark A. Hempenius; Holger Schönherr; Gyula J. Vancso

doi:10.1016/j.polymer.2005.12.091

Single Molecule Force Spectroscopy of Smart Poly(ferrocenylsilane) Macromolecules: Towards Highly Controlled Redox-Driven Single Chain Motors

S(han) Zou, I. Korczagin, Mark A. Hempenius, Holger Schönherr, Gyula J. Vancso

Research output: Contribution to journal › Article › Academic › peer-review

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Abstract

We investigated various stimuli-responsive poly(ferrocenylsilane) (PFS) polymers as model systems for the realization of molecular motors powered by a redox process. Covalently end-grafted PFS on gold, as well as PFS homopolymers and block copolymers in ultrathin films, were studied by AFM-based single molecule force spectroscopy (SMFS). Surface confined PFS macromolecules were chemically oxidized by addition of tetracyanoethylene or were completely and reversibly oxidized (and reduced) in situ by applying an electrochemical potential. Chemical oxidation was successful only for the block copolymers. The entropic elasticity of neutral PFS chains (Kuhn length IK0.40 nm) was found to be larger than that of oxidized PFS chains (IK0.65 nm) in the lower force regime. The elasticities could be reversibly controlled in situ by adjusting the applied potential in electrochemical SMFS experiments. For a single PFS macromolecule (DP=80) operating cycle, a work output and an efficiency of 3.4×10−19 J and 5%, respectively, were estimated based on the single chain experimental data.

Original language	Undefined
Pages (from-to)	2483-2492
Number of pages	10
Journal	Polymer
Volume	47
Issue number	7
DOIs	https://doi.org/10.1016/j.polymer.2005.12.091
Publication status	Published - 2006

Keywords

METIS-231149
IR-74281

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10.1016/j.polymer.2005.12.091

Cite this

@article{a8b976a9a6f948a88a4aaf7800b02ea3,

title = "Single Molecule Force Spectroscopy of Smart Poly(ferrocenylsilane) Macromolecules: Towards Highly Controlled Redox-Driven Single Chain Motors",

abstract = "We investigated various stimuli-responsive poly(ferrocenylsilane) (PFS) polymers as model systems for the realization of molecular motors powered by a redox process. Covalently end-grafted PFS on gold, as well as PFS homopolymers and block copolymers in ultrathin films, were studied by AFM-based single molecule force spectroscopy (SMFS). Surface confined PFS macromolecules were chemically oxidized by addition of tetracyanoethylene or were completely and reversibly oxidized (and reduced) in situ by applying an electrochemical potential. Chemical oxidation was successful only for the block copolymers. The entropic elasticity of neutral PFS chains (Kuhn length IK0.40 nm) was found to be larger than that of oxidized PFS chains (IK0.65 nm) in the lower force regime. The elasticities could be reversibly controlled in situ by adjusting the applied potential in electrochemical SMFS experiments. For a single PFS macromolecule (DP=80) operating cycle, a work output and an efficiency of 3.4×10−19 J and 5%, respectively, were estimated based on the single chain experimental data.",

keywords = "METIS-231149, IR-74281",

author = "S(han) Zou and I. Korczagin and Hempenius, {Mark A.} and Holger Sch{\"o}nherr and Vancso, {Gyula J.}",

note = "Special issue on single chain polymers ",

year = "2006",

doi = "10.1016/j.polymer.2005.12.091",

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T1 - Single Molecule Force Spectroscopy of Smart Poly(ferrocenylsilane) Macromolecules: Towards Highly Controlled Redox-Driven Single Chain Motors

AU - Zou, S(han)

AU - Korczagin, I.

AU - Hempenius, Mark A.

AU - Schönherr, Holger

AU - Vancso, Gyula J.

N1 - Special issue on single chain polymers

PY - 2006

Y1 - 2006

N2 - We investigated various stimuli-responsive poly(ferrocenylsilane) (PFS) polymers as model systems for the realization of molecular motors powered by a redox process. Covalently end-grafted PFS on gold, as well as PFS homopolymers and block copolymers in ultrathin films, were studied by AFM-based single molecule force spectroscopy (SMFS). Surface confined PFS macromolecules were chemically oxidized by addition of tetracyanoethylene or were completely and reversibly oxidized (and reduced) in situ by applying an electrochemical potential. Chemical oxidation was successful only for the block copolymers. The entropic elasticity of neutral PFS chains (Kuhn length IK0.40 nm) was found to be larger than that of oxidized PFS chains (IK0.65 nm) in the lower force regime. The elasticities could be reversibly controlled in situ by adjusting the applied potential in electrochemical SMFS experiments. For a single PFS macromolecule (DP=80) operating cycle, a work output and an efficiency of 3.4×10−19 J and 5%, respectively, were estimated based on the single chain experimental data.

AB - We investigated various stimuli-responsive poly(ferrocenylsilane) (PFS) polymers as model systems for the realization of molecular motors powered by a redox process. Covalently end-grafted PFS on gold, as well as PFS homopolymers and block copolymers in ultrathin films, were studied by AFM-based single molecule force spectroscopy (SMFS). Surface confined PFS macromolecules were chemically oxidized by addition of tetracyanoethylene or were completely and reversibly oxidized (and reduced) in situ by applying an electrochemical potential. Chemical oxidation was successful only for the block copolymers. The entropic elasticity of neutral PFS chains (Kuhn length IK0.40 nm) was found to be larger than that of oxidized PFS chains (IK0.65 nm) in the lower force regime. The elasticities could be reversibly controlled in situ by adjusting the applied potential in electrochemical SMFS experiments. For a single PFS macromolecule (DP=80) operating cycle, a work output and an efficiency of 3.4×10−19 J and 5%, respectively, were estimated based on the single chain experimental data.

KW - METIS-231149

KW - IR-74281

U2 - 10.1016/j.polymer.2005.12.091

DO - 10.1016/j.polymer.2005.12.091

M3 - Article

VL - 47

SP - 2483

EP - 2492

JO - Polymer

JF - Polymer

SN - 0032-3861

IS - 7

ER -