等离子体强化制备镍基催化剂过程机理研究

项目名称： 等离子体强化制备镍基催化剂过程机理研究

项目编号： No.21476157

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 有机化学

项目作者： 刘昌俊

作者单位： 天津大学

项目金额： 100万元

中文摘要： 镍基催化剂已被广泛用于合成气生产、煤制天然气等工业过程，并在页岩气、沼气、煤层气、焦炉气等利用方面将有重要应用。镍基催化剂上述应用涉及高温反应，均存在高温烧结、积炭严重和耐硫性差等问题，而催化剂尺度和结构对催化剂性能影响很大，但相关尺度和结构控制存在很大困难。本项目组在前期研究中已发现采用非氢等离子体法影响镍催化剂前驱体分解，可实现催化剂尺度、结构、表界面控制制备，并由此获得抗烧结、抗积炭和耐硫性能的改进。由于方法的新颖性和复杂性，等离子体强化催化剂制备过程控制机理还有待于研究。本项目围绕上述过程控制机理问题，研究等离子体活性物质（包括电子、激发态物质、离子等）影响催化剂前驱体分解相关能量、质量传递控制机理，研究等离子体影响下晶体成核与生长相关热力学和动力学特性，并通过甲烷水汽重整、CO2重整和CO甲烷化评价催化剂，建立相关非平衡传递过程理论与实验体系，为工业镍基催化剂改进制备打下基础。

中文关键词： 过程强化；催化剂；等离子体；晶体成核；晶体生长

英文摘要： Nickel based catalysts have been extensively applied for syngas production from natural gas and methanation of syngas (from coal and other resources). They are also promising for the potential application of shale gas, biogas, coal mine methane and coal oven gas. All the related reactions are carried out at high temperature. The nickle catalysts suffer from deactivation due to sintering, coking and sulfur poison. It has been confirmed that the catalyst size and structure show significant influence on the catalyst performance. However, the size and structure control of the nickel catalysts is a big challenge. We previously demonstrated that the nucleation and crystal growth under the influence of plasmas during the decomposition of the nickel precursor lead to a control for the catalyst size and structure and catalyst-support interface.By this way, the anti-sintering property, coke resistence and surfur tolerence of the Ni catalysts are significantly improved. Because of the nolvety and complex issue of the plasma preparation, the process mechanism is still not clear and needs to be investigated immediately. In this proposed work, we aim to study the process mechanism of the plasma catalyst preparation. The effect of various active species in the plasma (including electrons, excited species and ions) on the energy and mass transportation of the decomposition of the catalyst precursors will be investigated. The thermodynamic and kinetic of the nucleation and crystal growth under the influence of the plasma will be studied too. Steam reforming, CO reforming and CO methanation will be employed for the evaluation of the catalysts obtained. The theoretical and experimental system of the plasma catalyst preparation will be established. The results of the proposed study will be very helpful for the further improvement in the industrialized Ni catalysts.

英文关键词： process intensification;catalyst;plasma;nucleation;crystal growth