Yusa Shin-ichi, Fukuda Kenichi, Yamamoto Tohei, Iwasaki Yasuhiko, Watanabe Akihiko, Akiyoshi Kazunari, Morishima Yotaro
Department of Materials Science and Chemistry, Graduate School of Engineering, University of Hyogo, 2167 Shosha, Himeji, Hyogo 671-2201, Japan.
Langmuir. 2007 Dec 18;23(26):12842-8. doi: 10.1021/la702741q. Epub 2007 Nov 10.
Poly(N-isopropylacrylamide) (PNIPAM) with a narrow molecular weight distribution was prepared by reversible addition-fragmentation chain transfer (RAFT) radical polymerization. A dithioester group at the chain end of PNIPAM thus prepared was cleaved by treating with 2-ethanolamine to provide thiol-terminated PNIPAM with which gold nanoparticles were coated via reactions of the terminal thiol with gold. The thermoresponsive nature of the maximum wavelength of the surface plasmon band and hydrodynamic radius (Rh) for the PNIPAM-coated gold nanoparticles were found to be sensitively affected by added salt. In pure water, Rh for the PNIPAM-coated gold nanoparticles at 40 degrees C (>lower critical solution temperature (LCST)) was smaller than that at 25 degrees C (<LCST) due to the shrinkage of the PNIPAM chains on the gold surface. The maximum wavelength of the plasmon band in pure water was almost independent of the temperature, the color of the solution remaining pink regardless of temperature. On the other hand, in the presence of 50 mM NaCl, the plasmon band at 40 degrees C was red shifted compared with that at 25 degrees C because of interparticle associations, the pink color at 25 degrees C changing to blue-purple at 40 degrees C. Furthermore, Rh for the PNIPAM-coated gold nanoparticles at 40 degrees C was significantly larger than that at 25 degrees C. Heat-induced association and dissociation for the PNIPAM-coated gold nanoparticles were completely reversible in 50 mM NaCl aqueous solutions, which is responsible for the reversible thermoresponsive color change.
通过可逆加成-断裂链转移(RAFT)自由基聚合制备了具有窄分子量分布的聚(N-异丙基丙烯酰胺)(PNIPAM)。将由此制备的PNIPAM链端的二硫酯基团用2-乙醇胺处理进行裂解,以提供硫醇封端的PNIPAM,通过末端硫醇与金的反应,用其包覆金纳米颗粒。发现PNIPAM包覆的金纳米颗粒的表面等离子体带最大波长和流体力学半径(Rh)的热响应性质受添加盐的敏感影响。在纯水中,由于金表面PNIPAM链的收缩,40℃(>下临界溶液温度(LCST))时PNIPAM包覆的金纳米颗粒的Rh小于25℃(<LCST)时的Rh。纯水中等离子体带的最大波长几乎与温度无关,溶液颜色无论温度如何均保持粉红色。另一方面,在存在50 mM NaCl的情况下,由于颗粒间缔合,40℃时的等离子体带相对于25℃时发生红移,25℃时的粉红色在40℃时变为蓝紫色。此外,40℃时PNIPAM包覆的金纳米颗粒的Rh明显大于25℃时的Rh。PNIPAM包覆的金纳米颗粒的热诱导缔合和解离在50 mM NaCl水溶液中是完全可逆的,这导致了可逆的热响应颜色变化。