Lee Jae-Seung, Stoeva Savka I, Mirkin Chad A
Department of Chemistry and International Institute for Nanotechnology, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA.
J Am Chem Soc. 2006 Jul 12;128(27):8899-903. doi: 10.1021/ja061651j.
We present a novel method for size-selectively separating mixtures of nanoparticles in aqueous media utilizing the inherent chemical recognition properties of DNA and the cooperative binding properties of DNA-functionalized gold nanoparticles. We have determined that the melting temperatures (T(m)s) of aggregates formed from nanoparticles interconnected by duplex DNA are dependent upon particle size. This effect is proposed to derive from larger contact areas between the larger particles and therefore increased cooperativity, leading to higher T(m)s. The separation protocol involves taking two aliquots of a mixture of particles that vary in size and functionalizing them with complementary DNA. These aliquots are mixed at a temperature above the T(m) for aggregates formed from the smaller particles but below the T(m) for aggregates formed from the larger particles. Therefore, the aggregates that form consist almost exclusively of the larger particles and can be easily separated by sedimentation and centrifugation from the smaller dispersed particles. This unusual size-dependent behavior and separation protocol are demonstrated for three binary mixtures of particles and one ternary mixture.
我们提出了一种在水性介质中对纳米颗粒混合物进行尺寸选择性分离的新方法,该方法利用了DNA固有的化学识别特性以及DNA功能化金纳米颗粒的协同结合特性。我们已经确定,由双链DNA相互连接的纳米颗粒形成的聚集体的解链温度(T(m))取决于颗粒大小。这种效应被认为源于较大颗粒之间更大的接触面积,从而导致更高的协同性,进而产生更高的T(m)。分离方案包括取两份不同大小的颗粒混合物等分试样,并用互补DNA对它们进行功能化。这些等分试样在高于较小颗粒形成的聚集体的T(m)但低于较大颗粒形成的聚集体的T(m)的温度下混合。因此,形成的聚集体几乎完全由较大颗粒组成,可以通过沉淀和离心轻松地与较小的分散颗粒分离。这种不寻常的尺寸依赖性行为和分离方案在三种颗粒二元混合物和一种三元混合物中得到了证明。