Department of Chemical Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, USA.
Langmuir. 2010 Apr 6;26(7):4725-31. doi: 10.1021/la903616p.
For bottom-up particle fabrication, separation of complex particle assemblies from their precursor colloidal building blocks is critical to producing useable quantities of materials. The separations are often done using a density gradient sedimentation due to its simplicity and scalability. When loading density gradients at volume fractions greater than 0.001, however, an inherent convective instability arises. By translating the Rayleigh-Benard instability from the heat-transfer literature into an analogous mass-transfer problem, the variables affecting the critical stability limit were effectively catalogued and examined. Experiments using submicrometer particles loaded onto sucrose and Ficoll density gradients matched theoretical trends and led to a series of useful heuristics for prolonging density gradient stability. Higher particle loading heights, lower volume fractions, and smaller gradient material diffusion coefficients were found to improve stability. Centrifugation was useful at short times, as particles were removed from top of the gradient where the stable density profile degrades to unstable, and the resulting density inversion arises as the sucrose diffuses upward.
对于自下而上的颗粒制造,从其前体胶体构建块中分离复杂的颗粒组装体对于生产可用数量的材料至关重要。由于其简单性和可扩展性,通常使用密度梯度沉降进行分离。然而,当在体积分数大于 0.001 的情况下加载密度梯度时,会出现固有的对流不稳定性。通过将热传递文献中的瑞利-贝纳德不稳定性转化为类似的质量传递问题,可以有效地对影响临界稳定性极限的变量进行分类和检查。使用加载到蔗糖和 Ficoll 密度梯度上的亚微米颗粒进行的实验与理论趋势相匹配,并得出了一系列有用的启发式方法来延长密度梯度稳定性。发现更高的颗粒装载高度、更低的体积分数和更小的梯度材料扩散系数可提高稳定性。离心在短时间内很有用,因为颗粒从密度稳定轮廓降解为不稳定的梯度顶部被移除,并且随着蔗糖向上扩散,会出现密度反转。