Jerzy Haber Institute of Catalysis and Surface Chemistry, Polish Academy of Sciences, Niezapominajek 8, 30-239 Krakow, Poland.
Anal Chem. 2020 Nov 17;92(22):15087-15095. doi: 10.1021/acs.analchem.0c03115. Epub 2020 Nov 6.
A new theoretical model is formulated for the quantitative analysis of quartz crystal microbalance (QCM) response for heterogeneous loads consisting of nano- and microparticles. The influence of particle coverage and structure is described using a universal correction function in an manner. Explicit analytical expressions for the frequency and dissipation shifts are derived for the entire range of particle size under the rigid contact regime. The solvent coupling functions are also calculated to determine the dry coverage using the QCM measurements. These expressions furnish the upper limit of the QCM signal, which can be attained for a sensor providing perfect adhesion of particles. Correction functions accounting for the finite adhesion strength (soft contact regime) are also derived. The theoretical results are confronted with QCM and atomic force microscopy measurements of positively charged polymer particle deposition on silica sensors. The main features of the theoretical model are confirmed, especially the abrupt decrease in the QCM wet mass with the particle coverage and the overtone number. The latter effect is especially pronounced for microparticles under the soft contact regime, where the higher-number overtones produce a negligible QCM signal. These results represent a useful reference data for the interpretation of protein and bioparticles, for example, virus and bacteria attachment processes to various substrates.
提出了一种新的理论模型,用于定量分析由纳米和微米颗粒组成的不均匀负载的石英晶体微天平(QCM)响应。采用通用修正函数以统一的方式描述了颗粒覆盖率和结构的影响。在刚性接触状态下,导出了整个颗粒尺寸范围内的频率和耗散位移的显式解析表达式。还计算了溶剂耦合函数,以使用 QCM 测量确定干覆盖。这些表达式提供了 QCM 信号的上限,对于提供颗粒完美粘附的传感器可以达到该上限。还推导了考虑有限粘附强度(软接触状态)的修正函数。理论结果与 QCM 和原子力显微镜测量正电荷聚合物颗粒在二氧化硅传感器上的沉积进行了对比。证实了理论模型的主要特征,特别是颗粒覆盖率和倍频数对 QCM 湿质量的急剧下降。在软接触状态下,后者对微颗粒的影响尤其明显,其中更高倍频数产生可忽略不计的 QCM 信号。这些结果为解释蛋白质和生物颗粒(例如病毒和细菌)在各种基质上的附着过程提供了有用的参考数据。