论文部分内容阅读
Carbonate-bearing fluids widely exist in different geological settings, and play important roles in transporting some elements such as the rare earth elements. They may be trapped as large or small fluid inclusions (with the size down to <1 μm sometimes), and record critical physical-chemical signals for the formations of their host minerals. Spectroscopic methods like Raman spectroscopy and infrared spectroscopy have been proposed as effective methods to quantify the carbonate concentrations of these fluid inclusions. Although they have some great technical advantages over the conventional microthermometry method, there are still some technical dif-ficulties to overcome before they can be routinely used to solve relevant geological problems. The typical limi-tations include their interlaboratory difference and poor performance on micro fluid inclusions. This study prepared standard ion-distilled water and K2CO3 aqueous solutions at different molarities (from 0.5 to 5.5 mol/L), measured densities, collected Raman and infrared spectra, and explored correlations between the K2CO3 molarity and the spectroscopic features at ambient P-T conditions. The result confirms that the Raman O–H stretching mode can be used as an internal standard to determine the carbonate concentrations despite some significant differences among the correlations, established in different laboratories, between the relative Raman intensity of the C–O symmetric stretching mode and that of the O–H stretching mode. It further reveals that the interlabor-atory difference can be readily removed by performing one high-quality calibration experiment, provided that later quantifying analyses are conducted using the same Raman spectrometer with the same analytical conditions. Our infrared absorption data were collected from thin fluid films (thickness less than～2μm) formed by pressing the prepared solutions in a Microcompression Cell with two diamond-II plates. The data show that both the O–H stretching mode and the O–H bending mode can be used as internal standards to determine the carbonate con-centrations. Since the IR signals of the C–O antisymmetric stretching vibration of the CO32- ion, and the O–H stretching and bending vibrations from our thin films are very strong, their relative IR absorbance intensity, if well calibrated, can be used to investigate the micron-sized carbonate-bearing aqueous fluid inclusions. This study establishes the first calibration of this kind, which may have some applications. Additionally, our spectroscopic data suggest that as the K2CO3 concentration increases the aqueous solution forms more large water molecule clusters via more intense hydrogen-bonding. This process may significantly alter the physical and chemical behavior of the fluids.