Figueroa-Cosme Legna, Gilroy Kyle D, Yang Tung-Han, Vara Madeline, Park Jinho, Bao Shixiong, da Silva Anderson G M, Xia Younan
School of Chemistry and Biochemistry, Georgia Institute of Technology, Atlanta, Georgia, 30332, USA.
The Wallace H. Coulter Department of Biomedical Engineering, Georgia Institute of Technology and Emory University, Atlanta, Georgia, 30332, USA.
Chemistry. 2018 Apr 20;24(23):6133-6139. doi: 10.1002/chem.201705720. Epub 2018 Mar 25.
Shape-controlled synthesis of colloidal metal nanocrystals has traditionally relied on the use of an approach that involves the reduction of a metal precursor by a single reductant. Once the concentration of atoms surpasses supersaturation, they will undergo homogeneous nucleation to generate nuclei and then seeds, followed by further growth into nanocrystals. In general, it is a grand challenge to optimize such an approach because the kinetic requirement for nucleation tends to be drastically different from what is needed to guide the growth process. In this work, we overcome this difficulty by switching to a dual-reductant approach, in which both strong and weak reductants are added into the same reaction solution. By controlling their amounts to program the reduction kinetics, the strong reductant only regulates the homogeneous nucleation process to generate the desired seeds, and once consumed, the weak reductant takes over to control the growth pattern and thereby the shape of the resulting nanocrystals.
传统上,胶体金属纳米晶体的形状控制合成依赖于一种通过单一还原剂还原金属前驱体的方法。一旦原子浓度超过过饱和度,它们将经历均相成核以产生核,然后形成晶种,随后进一步生长成纳米晶体。一般来说,优化这种方法是一个巨大的挑战,因为成核的动力学要求往往与引导生长过程所需的条件截然不同。在这项工作中,我们通过转向双还原剂方法克服了这一困难,即将强还原剂和弱还原剂都加入到同一反应溶液中。通过控制它们的用量来编程还原动力学,强还原剂仅调节均相成核过程以产生所需的晶种,一旦消耗完毕,弱还原剂就接管以控制生长模式,从而控制所得纳米晶体的形状。