氧化铁石墨固相还原非等温反应动力学

doi:10.3969/j.issn.0438-1157.2013.06.024

化工学报 ›› 2013, Vol. 64 ›› Issue (6): 2072-2079.DOI: 10.3969/j.issn.0438-1157.2013.06.024

• 催化、动力学与反应器 • 上一篇下一篇

氧化铁石墨固相还原非等温反应动力学

姚梅琴^1,2, 余剑¹, 郭凤^1,3, 许光文¹

1. 中国科学院过程工程研究所多相复杂系统国家重点实验室,北京 100190;
2. 中国科学院研究生院,北京 100039;
3. 中国矿业大学(北京)化学与环境工程学院,北京 100083

收稿日期:2012-09-18 修回日期:2012-12-24 出版日期:2013-06-05 发布日期:2013-06-05
通讯作者: 余剑,许光文
作者简介:姚梅琴(1988—),女,硕士研究生。
基金资助:
国家自然科学基金项目(21106156, 21006114);国家重大仪器专项(2011YQ120039)。

Non-isotherm kinetics of iron oxide reduction by graphite

YAO Meiqin^1,2, YU Jian¹, GUO Feng^1,3, XU Guangwen¹

1. State Key Laboratory of Multi-phase Complex Systems, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
2. Graduate University of Chinese Academy of Sciences, Beijing 100039, China;
3. School of Chemical and Environmental Engineering, China University of Mining and TechnologyBeijing, Beijing 100083, China

Received:2012-09-18 Revised:2012-12-24 Online:2013-06-05 Published:2013-06-05
Supported by:
supported by the National Natural Science Foundation of China(21106156,21006114)and the National Instrumentation Grant(2011YQ120039).

摘要/Abstract

摘要： 准确测试固固反应,如铁矿炭还原反应的动力学在科学研究和实际应用中均具有重要意义。利用热重程序升温的方法研究了氧化铁石墨还原的固固反应特性,在惰性气氛下分别考察了研磨与浸渍混合后焙烧制得的Fe₂O₃/C样品的失重曲线,采用Flynn-Wall-Ozawa公式和Coats-Redfern公式相结合的方法分别求算了两种混合样品的固固反应动力学参数,研究发现氧化铁在炭表面的聚集形态与其活化能变化规律直接相关,且浸渍焙烧法所得样品的活化能符合强吸热反应活化能变化规律。结合固体原位XRD表征与气体产物在线分析手段,发现在初始阶段Fe₂O₃即可与C直接反应生成Fe₃O₄和CO₂。该反应的活化能约为530 kJ·mol^-1,反应机理为二级化学反应模型。

关键词: 固固反应, 铁矿还原, 石墨, 非等温, 反应动力学

Abstract: The accurate measurement of solid-solid reaction kinetics, such as reduction of iron oxide by carbon, is of great significance in scientific research and practical applications.In this paper solid-solid reaction characteristics between iron oxide and graphite was studied using thermogravimeter (TG) measurement for both samples prepared respectively by directly mixing and grinding graphite and Fe₂O₃ as well as by impregnating Fe₂O₃ on the graphite.Their reaction kinetic parameters were calculated using the Flynn-Wall-Ozawa and Coats-Redfern equations.The variation trends of activation energy are related with the aggregation morphology of Fe₂O₃ on the surface of carbon.The reduction kinetics for impregnated sample is of the characteristics of strong endothermic reaction.Combining the results of XRD characterization and online gas determination, in the initial stage of Fe₂O₃ reduction the products are Fe₃O₄ and CO₂, reaction follows second order reaction mechanism and activation energy is about 530 kJ·mol^-1.

Key words: solid-solid reaction, reduction of iron oxide, graphite, non-isothermal, reaction kinetics

中图分类号:

O643
TQ138.1

姚梅琴, 余剑, 郭凤, 许光文. 氧化铁石墨固相还原非等温反应动力学[J]. 化工学报, 2013, 64(6): 2072-2079.

YAO Meiqin, YU Jian, GUO Feng, XU Guangwen. Non-isotherm kinetics of iron oxide reduction by graphite[J]. CIESC Journal, 2013, 64(6): 2072-2079.

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氧化铁石墨固相还原非等温反应动力学

Non-isotherm kinetics of iron oxide reduction by graphite

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