联系生产实际对西门子法三氯氢硅氢还原反应体系的反应做了归类分析,选用可靠适用的热力学基础数据,设计合理计算方案,计算分析16个反应在反应温度区及附近温度区的吉布斯自由能和标准平衡常数数值,利用反应耦合理论提供了将SiHCl3(g)+H2(g)=Si(s)+3HCl(g)作为主反应的热力学依据,确认该主反应与关键组分SiHCl3(g)的两个热分解生成有Si(s)和SiCl4(g)的反应构成的平行反应为生成Si-CVD的主要反应.在此基础上,应用L-H均匀表面吸附理论,借助非均相气-固相催化反应模型方法,导出该还原Si-CVD过程的本征速率方程-rAs=ksc1cA +ksc2cA2+ksc3cA4,进而线性化变换为等价的拟一级不可逆反应动力学模型-RAS=ksc,djcA,dj(简写为-RAss=kscccA),便于动力学参数测定和后续建立宏观动力学模型.
In order to identify the main reactions that effect the formation of silicon in the hydrogen reduction reaction system of Trichlorosilane by the Siemens method and derive the intrinsic-kinetics equation,some classified analysis of all the possible reactions by choosing the appropriate and reliable thermal chemical data were made,the reasonable calculation plan was designed,and the Gibbs free energy and Standard equilibrium constant between the reaction temperature zone and the nearby temperature zone were contrasted.Coupling reaction theory being used and coupling effect through related reactions being analyzed,the theoretic confusion about the lack of basis in the main reaction of SiHCl3(g)+H2(g)=Si(s)+3HCl(g) is confirmed as the main reaction,and also determined that these two thermal reactions which break down and produce Si(s) and SiCl4(g) shouldn't be ignored and should be regarded as significant reactions.On the basis of this,the intrinsic-kinetics equation (-rAs =ksc1cA +ksc2cA2 +ksc3cA4) of reduction-CVD was derived by applying the L-H uniform surface adsorption theory and heterogeneous gas-solid-phase catalytic reaction model approach.This linearized transformation is simplified into equivalent irreversible kinetic model (-RAs =ksc,djcA,dj,Simple plan writing (-RAs =ksccA),which is not only good for the determination of kinetic parameters,but also for the subsequent establishment of the macro-dynamics model.
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