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基于等转化法及多元非线性拟合的高岭石非等温脱羟基动力学分析

KINETIC ANALYSIS OF NON-ISOTHERMAL DEHYDROXYLATION OF KAOLINITE BASED ON ISOCONVERSIONAL AND MULTIVARIATE NON-LINEAR REGRESSION METHODS

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【作者】 张湘辉钟玉馨汪灵廖广志王如燕李忠权李家燕

【Author】 ZHANG Xianghui;ZHONG Yuxing;WANG Ling;LIAO Guangzhi;WANG Ruyan;LI Zhongquan;LI Jiayan;College of Materials and Chemistry and Chemical Engineering,Chengdu University of Technology;Petro China Exploration & Production Company;Xinjiang Oilfield Company,PetroChina;State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation,Chengdu University of Technology;Key Laboratory of Tectonic Controls on Mineralization and Hydrocarbon Accumulation,Ministry of Natural Resources,Chengdu University of Technology;

【通讯作者】 汪灵;

【机构】 成都理工大学材料与化学化工学院中国石油勘探与生产公司中国石油新疆油田分公司油气藏地质及开发工程国家重点实验室成都理工大学自然资源部构造成矿成藏重点实验室成都理工大学

【摘要】 采用Netzsch STA409PC同步热分析仪研究了苏州高岭石(KW125)在30℃~1 200℃间的热分解过程。采用"Netzsch Thermokinetics software"软件对其脱羟基机理进行了非等温动力学研究。基于等转化法评价了反应活化能及反应进程的依存关系。基于多元非线性拟合确定了最可能反应机理及动力学参数。研究结果表明:苏州高岭石在30℃~1 200℃温度范围的热分解为脱羟基与相转变等两个阶段。其脱羟基(30℃~800℃)过程中活化能呈现三个变化:197.68 kJ/mol±12.95 kJ/mol→181.04 kJ/mol±18.98 kJ/mol→269.7 kJ/mol±14.64 kJ/mol。脱羟基反应遵循三步连续反应模型t:f,f;(D3-Fn-Fn),一个三维扩散(D3)反应,然后是两个n序列(Fn)反应。第一步,f(α)=3(1-α)2/3/(2(1-(1-α)1/3),E1=185.27 kJ/mol,logA=10.83 s-1;第二步,f(α)=(1-α)n,n=1.75,E2=187.81 kJ/mol,logA=10.32 s-1;第三步,f(α)=(1-α)n,n=4.4,E3=262.70 kJ/mol,logA=13.26 s-1

【Abstract】 The thermal decomposition of Suzhou kaolinite below 1 200 ℃was investigated by simultaneous thermal analyzer.Non-isothermal kinetic analysis was employed to study the dehydroxylation mechanism by using Netzsch Thermokinetics software.The dependence of activation energy on the reaction process was evaluated based on the isoconversional method,and the probable mechanism as well as the corresponding kinetic parameters was determined on the basis of multivariate non-linear regression program. It was showed that the thermal decomposition of Suzhou kaolinite was divided into two stages of dehydroxylation and phase transformation. During kaolinite dehydroxylation,three activation energy changes were recognized as 197.68→181.04→269.7 kJ/mol.The dehydroxylation reaction was controlled by three consecutive mechanisms t:f,f;(D3-Fn-Fn),a three-dimensional diffusion(D3 mode) reaction followed by two n-order(Fn mode) reactions. The first step was f(α)=(3(1-α)2/3/(2(1-(1-α)1/3)),E1=185.27 kJ/mol, logA=10.83 s-1;the second step f(α)=(1-α)n,n=1.75,E2=187.81 kJ/mol,logA=10.32 s-1 and the third step was f(α)=(1-α)n,n=4.4,E3=262.70 kJ/mol,logA=13.26 s-1.

【基金】 国家自然科学基金(41672196,41741004,41572038);地质灾害防治与地质环境保护国家重点实验室开放基金(SKLGP2018K022);国家科技重大专项(2016ZX05004-005-02,2017ZX05008-001);中国石油新疆油田分公司项目(XJYT-gcjsyjy-2017-JS-612);四川省教育厅资助科研项目(16ZA0081,12ZB006,16TD0011,13TD0007)
  • 【文献出处】 矿物岩石 ,Mineralogy and Petrology , 编辑部邮箱 ,2019年02期
  • 【分类号】P578.94
  • 【被引频次】2
  • 【下载频次】140
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