An In Situ Decarbonation Kinetic Study of Calcite Using Synchrotron Radiation XRD

Chuan-jiang Liu, Kenan Han, Duojun Wang
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引用次数: 1

Abstract

In situ decarbonation kinetics of calcite were investigated at high temperatures, up to 900 °C, using synchrotron radiation powder X-ray diffraction. The sequence of X-ray diffraction spectra reveals that calcite begins to thermally decompose into lime (CaO) and CO2 at 800 °C and ambient pressure. The decarbonation degree gradually increases with temperature, and calcite completely transforms into lime at 900 °C. The kinetic analysis of the isothermal data using an Avrami model involving nucleation and growth yields the values for the decarbonation rate and reaction order. Our results indicate that the decarbonation rate increases from 2.89 × 10–4s–1 to 3.48 × 10–3s–1 with elevated temperature from 840 to 880 °C, showing a positive temperature dependence on the reaction rate. The calculated Avrami exponent (n) values between 1.35 and 2.38 suggest that the thermal decomposition of calcite should be mainly dominated by homogeneous nucleation and CO2 diffusion-controlled growth. In natural carbonate fault rocks, the decarbonation of CaCO3 caused by frictional heating may be strengthened by the action of high shear velocity. In addition, the resulting ultrafine powder and CO2 pressurization can remarkably reduce the friction coefficient between two fault planes, which further leads to carbonate fault weakening. The yielding result will be conductive to better understanding the role of decarbonation of calcite in some active fault zones.
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方解石原位脱碳动力学的同步辐射XRD研究
利用同步辐射粉末x射线衍射研究了方解石在900℃高温下的原位脱碳动力学。x射线衍射谱序列表明,方解石在800℃和环境压力下开始热分解为石灰(CaO)和CO2。脱碳程度随温度升高而逐渐增大,在900℃时方解石完全转变为石灰。用Avrami模型对等温数据进行了动力学分析,得到了脱碳速率和反应级数。结果表明,当温度从840°C升高到880°C时,脱碳速率从2.89 × 10-4s-1增加到3.48 × 10-3s-1,反应速率与温度呈正相关。计算得到的Avrami指数(n)在1.35 ~ 2.38之间,说明方解石的热分解主要以均匀成核和CO2扩散控制生长为主。在天然碳酸盐岩断层岩中,摩擦加热引起的CaCO3脱碳可能在高剪切速度的作用下得到加强。此外,由此产生的超细粉末和CO2加压可以显著降低两个断层面的摩擦系数,从而进一步导致碳酸盐岩断层的弱化。研究结果将有助于更好地理解方解石在某些活动断裂带中的脱碳作用。
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