Quartz Crystal Microbalance (QCM)in High-Pressure Carbon Dioxide (CO_2):Experimental Aspects of QCM Theory and CO_2 Adsorption

摘要

The quartz crystal microbalance (QCM)technique has been developed into a powerful tool for the study of solid-fluid interfaces.This study focuses on the applications of QCM in high-pressure carbon dioxide (CO2)systems.Frequency responses of six QCM crystals with different electrode materials (silver or gold)and roughness values were determined in helium,nitrogen,and carbon dioxide at 35-40 deg C and at elevated pressures up to 3200 psi.The goal is to experimentally examine the applicability of the traditional QCM theory in high-pressure systems and determine the adsorption of CO2 on the metal surfaces.A new QCM calculation approach was formulated to consider the surface roughness contribution to the frequency shift.It was found that the frequency-roughness correlation factor,C_r,in the new model was critical to the accurate calculation of mass changes on the crystal surface.Experiments and calculations demonstrated that the adsorption (or condensation)of gaseous and supercritical CO_2 onto the silver and gold surfaces was as high as 3.6 mug cm~(-2)at 40 deg C when the CO_2 densities are lower than 0.85 g cm~(-3).The utilization of QCM crystals with different roughness in determining the adsorption of CO2 is also discussed.