Department of Chemistry, University of Warwick, Coventry CV4 7AL, United Kingdom.
Anal Chem. 2012 Mar 6;84(5):2585-91. doi: 10.1021/ac203493p. Epub 2012 Feb 15.
Evanescent wave cavity ringdown spectroscopy (EW-CRDS) is advocated as an approach for monitoring the formation of supported lipid bilayers (SLBs) on quartz substrates in situ and for the quantitative study of fast molecular adsorption kinetics at the resulting modified biomimetic surface. This approach is illustrated using SLBs of 1,2-dioleoyl-3-trimethylammonium-propane (DOTAP). Complementary atomic force microscopy (AFM) and quartz crystal microbalance with dissipation (QCM-D) measurements confirm the formation of bilayers on quartz. The subsequent interaction of the porphyrin, 5,10,15,20-tetraphenyl-21H,23H-porphine-p,p',p'',p'''-tetrasulfonic acid tetrasodium hydrate (TPPS) with the cationic bilayer-modified silica surface has been studied using EW-CRDS combined with an impinging-jet to deliver analyte to the surface in a well-defined manner. The adsorption of TPPS to the bilayer was kinetically controlled and the adsorption rate constant was found to be 1.7 (±0.6) × 10(-4) cm s(-1) from finite element modeling of the jet hydrodynamics and associated convective-diffusion equation, coupled to a first-order surface process describing adsorption. These proof-of-concept studies provide a platform for the investigation of molecular processes at biomembranes using EW-CRDS for chemical species showing optical absorbance in the visible and ultraviolet range.
消逝波腔衰荡光谱(EW-CRDS)被提倡作为一种原位监测石英基底上支撑脂质双层(SLB)形成的方法,以及用于研究在由此产生的仿生改性表面上快速分子吸附动力学的定量研究方法。该方法使用 1,2-二油酰基-3-三甲铵丙烷(DOTAP)的 SLB 进行说明。互补的原子力显微镜(AFM)和石英晶体微天平与耗散(QCM-D)测量证实了在石英上形成双层。随后,卟啉,5,10,15,20-四苯基-21H,23H-卟啉-p,p',p'',p''' -四磺酸四钠盐水合物(TPPS)与阳离子双层改性硅表面的相互作用已使用 EW-CRDS 结合冲击射流进行研究,以明确的方式将分析物输送到表面。TPPS 对双层的吸附是动力学控制的,并且吸附速率常数通过射流流体动力学的有限元建模以及与描述吸附的一阶表面过程相关的对流扩散方程发现为 1.7(±0.6)×10(-4)cm s(-1)。这些概念验证研究为使用 EW-CRDS 研究具有可见和紫外光范围内光学吸收的化学物质在生物膜上的分子过程提供了一个平台。