期刊
ACS APPLIED POLYMER MATERIALS
卷 3, 期 1, 页码 329-341出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsapm.0c01120
关键词
poly(N-isopropylacrylamide); stimuli-responsive; molecular imprinting; electrochemical sensing; nitrophenol; conformation change; templated polymer; RAFT
资金
- NIH COBRE Center of Integrated Biomedical and Bioengineering Research from the National Institute of General Medical Sciences [CIBBR] [P20 GM113131]
- National Science Foundation [ECCS] [1847152]
- Collaborative Research Excellence (CoRE) Pilot Research Partnership from the University of New Hampshire
- Directorate For Engineering
- Div Of Electrical, Commun & Cyber Sys [1847152] Funding Source: National Science Foundation
The development of a single-chain stimuli-responsive templated polymer without covalent interchain cross-linkers shows promise as a target recognition element for a label-free electrochemical sensing platform.
The use of highly cross-linked molecularly imprinted polymers as a synthetic target receptor has the limitations of restricted accessibility to the binding sites, resulting in a slow response time. Moreover, such artificial receptors often require additional transduction mechanisms to translate target binding events into measurable signals. Here, we propose the development of a single-chain stimuli-responsive templated polymer, without using any covalent interchain cross-linkers, as a target recognition element. The synthesized polymer chain exhibits preferential binding with the target molecule with which the polymer is templated. Moreover, upon specific target recognition, the polymer undergoes conformation change induced by its particular stimuli responsiveness, namely, the target binding event. Such templated single-chain polymers can be attached to the electrode surface to implement a label-free electrochemical sensing platform. A target analyte, 4-nitrophenol (4-NP), was used as a template to synthesize a poly(N-isopropylacrylamide) (PNIPAM)-based copolymer chain which was anchored to the electrode to be used as a selective receptor for 4-NP. The electrode surface chemistry analysis and the electrochemical impedance study reveal that the polymer concentration, the interchain interactions, and the Hofmeister effect play a major role in influencing the rate of polymer grafting as well as the morphology of the polymers grafted to the electrode. We also show that the specific binding between 4-NP and the copolymer results in a substantial change in the charge transfer kinetics at the electrode signifying the polymer conformation change.
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