Preparation of DNA-immobilized magnetic particles and their utilization as an accumulative material of metal ions

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Eiji Hosono Research Institute for Energy Conservation, National Institute of Advanced Industrial Science and Technology, Tsukuba 305-8568, Japan (Received 1 September 2015; accepted 5 January 2016)

DNA-immobilized Fe3O4 particles (DNA–Fe-particles) were prepared by mixing DNA, magnetic Fe3O4 particles, and the silane coupling reagent, bis[3-(trimethoxysilyl)propyl]amine. The DNA–inorganic hybrid material was uniformly immobilized onto magnetic Fe3O4 particles with the diameters of approximately 450 nm. These DNA–Fe-particles were stable in water. Additionally, we could simply collect the DNA–Fe-particles by a magnet from an aqueous solution. Therefore, we demonstrated the accumulation of various metal ions, such as heavy and rare-earth metal ions, by the DNA–Fe-particles. As a result, although these DNA–Fe-particles could selectively accumulate heavy and rare-earth metal ions, these materials could not accumulate the light metal ions, such as Mg(II) and Ca(II) ions. Furthermore, the metal ion-accumulated DNA–Fe-particles could be recycled by washing them with an aqueous ethylenediaminetetraacetic acid solution.

I. INTRODUCTION

Double-stranded DNA, one of the most important biopolymers in living organisms, has many functions, such as the intercalation of planar-structure containing compounds,1,2 the groove binding of cancer drugs,1,2 the complementary interaction between nucleic acid bases,3,4 and the selective binding of metal ions.1–4 Therefore, double-stranded DNA has been used as a functional material, such as the accumulations of harmful compounds,5,6 electric devices,7,8 optical materials,9–11 ion conducting materials,12,13 bio- and medical materials,14,15 nanomaterials,16–19 and environmental materials.3,4,7,8 Recently, we reported the preparation of the DNA–inorganic hybrid film20 and DNA-immobilized glass beads21 by mixing the double-stranded DNA and silane coupling reagents. These DNA materials could selectively accumulate harmful compounds, such as dioxin derivatives, polychlorinated biphenyl derivatives, benzo[a]pyrene, and heavy metal ions.20–22 Additionally, these harmful compound-accumulated DNA materials could be reused by washing with ethanol or chelating reagents. However, it is difficult to collect these DNA materials, such as the DNA–inorganic hybrid film and DNA-immobilized glass beads, from an aqueous

Contributing Editor: Adrian B. Mann a) Address all correspondence to this author. e-mail: [email protected] DOI: 10.1557/jmr.2016.14 360

J. Mater. Res., Vol. 31, No. 3, Feb 15, 2016

solution. Therefore, for utilization of the DNA as an environmental material, the development of effective and simple collection methods of DNA material from an aqueous solution is very important. Metal oxide particles have many functions, such as optical properties,23,24 catalytic activities,25 antimicrobial activities,26 and the absorption properties.27 Therefore, the metal oxide particles have been used as engineering materials, catalysts, absorbents, and biomedical materials.28 Additionally, composite mate