化学循环干气重整用Fe基六铝酸盐氧载体的结构及作用机制

项目名称： 化学循环干气重整用Fe基六铝酸盐氧载体的结构及作用机制

项目编号： No.21303137

项目类型： 青年科学基金项目

立项/批准年度： 2014

项目学科： 数理科学和化学

项目作者： 朱燕燕

作者单位： 西北大学

项目金额： 25万元

中文摘要： 化学循环干气重整（CLDR）可同时实现含碳燃料的高效利用、CO2的廉价捕集和定向转化。决定CLDR系统运转的关键是氧载体（实质是氧化还原催化剂），它不仅要能够为燃料提供氧，其还原态还要能够从低化学势的CO2中捕获氧。开发具有高氧化还原活性、强氧传输扩散能力和优异高温稳定性的氧载体以及研究其CLDR作用机制是目前亟需解决的问题。本申请以具有高活性、高温稳定性的Fe基六铝酸盐为前体，通过大阳离子种类和过渡/贵金属离子取代实现氧载体微观结构、氧化还原活性、氧移动性的调控，获得高效CLDR用氧载体。综合利用多种表征技术确定氧载体在CLDR反应过程中的微观结构和化学状态(晶位分布、配位情况、电子状态等)变化规律，结合密度泛函理论计算，研究其作用机制，力图从微观结构、化学状态、氧移动能力多角度揭示Fe基六铝酸盐氧载体在CLDR反应过程中的催化本质，为高效CLDR用氧载体的研究和开发提供理论和实验依据。

中文关键词： 化学循环干气重整；Fe基六铝酸盐；氧载体；构效关系；CO2利用

英文摘要： Chemical looping dry reforming (CLDR) opens a novel pathway to high-efficient utilization of carbon-based fuel, CO2 capture and activation, simultaneously. CLDR uses periodic reduction and oxidation of an oxygen carrier with carbon-based fuel and CO2, respectively, to achieve sequestration-ready CO2 streams and CO, respectively. Oxygen carrier (red-ox catalyst in essence) is the key factor, which dominates the feasibility of CLDR process. Now, It is indispensable to develop a highly red-ox active, high oxygen mobility and high-temperature stable oxygen carrier and to establish the relationship between the structure and reaction performances of CLDR. In this application, we will select Fe-based hexaaluminate to prepare CLDR oxygen carrier, which combined highly red-ox active and remarkable resistance to sintering and thermal shock due to its peculiar layered structure. Furthermore, we will adjust the type and proportion of large cations and the substituted transition/noble metal ions in Fe-based hexaaluminate structure to modify its micro-structure, red-ox active, and oxygen mobility, in order to obtain novel high- efficient CLDR oxygen carrier. After that, the relationship between structure and reaction performance of CLDR will be established. Through characterization technologies (eg. XRD, FTIR, TGA, Rietveld r

英文关键词： Chemical looping dry reforming；Fe-based hexaaluminate；oxygen carrier；relationship between structure and performance；CO2 utilization