项目名称： 煤直接化学链制氢工艺中煤焦与钾修饰铁基氧载体的催化反应机理探索

项目编号： No.21506241

项目类型： 青年科学基金项目

立项/批准年度： 2016

项目学科： 有机化学

项目作者： 余钟亮

作者单位： 中国科学院山西煤炭化学研究所

项目金额： 21万元

中文摘要： 与传统煤气化制氢工艺相比，煤直接化学链制氢工艺可省去空分、CO变换、CO2/H2分离和H2精制工序，具有显著提高产氢效率的潜力。FeO/Fe的生成是基于铁基氧载体的煤直接化学链制氢工艺的关键和前提，然而，氧化铁与煤焦直接反应生成FeO/Fe的速率很慢。通过添加碳酸钾可显著增大该反应的速率，前期机理研究发现反应过程中存在明显的钾迁移及自催化现象，但是对其产生机制还缺乏进一步的了解。为此，本项目拟首先详细研究不同碳转化率下反应速率与氧载体物相、钾分布与含量的对应关系；然后进行氧化铁-煤焦之间钾迁移特性的影响因素考察；在考察氧化铁与碳酸钾的反应特性之后，比较氧化铁、碳酸钾及二者反应产物对煤焦气化反应的催化作用；最后总结规律研究钾存在下氧化铁的自催化机制。项目的研究实施有助于揭示钾修饰铁基氧载体与煤焦的催化反应机理和氧载体活性保持机制，为煤直接化学链制氢工艺的研究开发奠定理论基础。

中文关键词： 煤；氢气；铁基氧载体；化学链；催化机理

英文摘要： Compared to the traditional process of coal to hydrogen via gasification, the efficiency of coal direct chemical looping hydrogen is expected to be remarkably increased due to the requirements of air separation, CO shift, CO2-H2 separation, and H2 purification are avoided. The production of FeO/Fe is the precondition of coal direct chemical looping hydrogen with iron based oxygen carrier. However, the reduction rate of Fe2O3 to FeO/Fe by coal char is very slow. This reduction rate can be significantly enhanced by K2CO3 addition. The previous catalytic mechanism studies have found the remarkable potassium migration and autocatalysis. However, the mechanism is not clear. Therefore，this project will detailedly analyze the following aspects: the relationship of reduction rate with the phase of iron oxide, potassium distribution and content; the effects on the potassium migration between iron oxide and coal char; the reaction characteristics of iron oxide and K2CO3; the catalytic effects of iron oxide, K2CO3 and their products on the gasification of coal char; the autocatalysis by iron oxide in the presence of potassium. The implementations of this project could help to understand the catalytic reaction mechanism and the mechanism of activity conserving, and provide a theoretical basis for the research and development of coal direct chemical looping hydrogen process.

英文关键词： coal;hydrogen;iron-based oxygen carrier;chemical looping ;catalytic mechanism