3-Dimensional graphene/Cu/Fe 3 O 4 composites: Immobilized laccase electrodes for detecting bisphenol A

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School of Chemistry and Chemical Engineering, Qiqihar University, Qiqihar, Heilongjiang Province 161000, China School of Materials Science and Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China 3 Key Laboratory of Materials Processing and Mold (Zhengzhou University), Ministry of Education, National Engineering Research Center for Advanced Polymer Processing Technology, Zhengzhou University, Zhengzhou 450001, China 4 Integrated Composites Laboratory (ICL), Department of Chemical & Biomolecular Engineering, University of Tennessee, Knoxville, Tennessee 37996, USA; and School of Materials Science and Engineering, North University of China, Taiyuan 030051, China 5 College of Materials Science and Engineering, Changsha University of Science and Technology, Changsha 410114, China 6 Integrated Composites Laboratory (ICL), Department of Chemical & Biomolecular Engineering, University of Tennessee, Knoxville, Tennessee 37996, USA a) Address all correspondence to these authors. e-mail: [email protected] b) e-mail: [email protected] c) e-mail: [email protected] d) e-mail: [email protected] 2

Received: 29 April 2019; accepted: 17 July 2019

Three-dimensional graphene (3D-GN)/Cu/Fe3O4 composite support materials were synthesized by a modified chemical reduction method using graphene oxide precursor. A 3D-GN/Cu/Fe3O4 biosensor was prepared by coating the electrode with laccase. The electrochemical properties of the biosensor were investigated by cyclic voltammetry (CV) and differential pulse voltammetry using potassium ferricyanide, phosphate-buffered saline (PBS) solution, and bisphenol A (BPA) solution. The current response of 3D-GN/Cu/Fe3O4 biosensors presents a remarkable sensitivity based on CV. The linear range of BPA is 7.2–18 lM using differential pulse voltammetry in PBS solution (pH = 4.0). A linear fitting equation of the laccase biosensor was observed for the current response as a function of BPA concentration. The detection limit was decreased to 1.7 lM. The detection approach herein turns out to be highly sensitive, has a wide linear range, and exhibits excellent stability.

Introduction With the continuous progress of industrialization and increasing demands of new materials [1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13] and energy [14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30], serious pollution of environment is caused by the release of many chemicals such as heavy metals [31, 32, 33, 34, 35], organics [36, 37, 38], gases [39, 40], and oils that are harmful to animals and plants [41, 42, 43, 44, 45]. Environmental estrogen or endocrine disruptor (EDC) is an important pollutant [46]. After entering the human body, it has two main effects on human beings. Firstly, it competes with the body’s own estrogen to bind serum protein, affecting the normal functions of its own estrogen. Secondly, its binding to nuclear receptors affects the hormonal homeostasis [46]. Bisphenol A (BPA), namely, 2,2-bis(4-hydroxyphenyl)propane, as the endocrine disruptor, has been

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