Chemical looping hydrogen generation of coal with oxygen carrier of Mg-modified Fe/Al

doi:10.16085/j.issn.1000-6613.2021-0561

Abstract

Abstract:

Fe₂O₃/Al₂O₃ oxygen carrier used in chemical looping process will form FeAl₂O₄, which is difficult to react with water to produce hydrogen due to thermodynamic limitations. In order to solve this problem, Mg was added to Fe/Al oxygen carrier for coal chemical looping hydrogen generation, and the action mechanism of Mg was deeply analyzed and its influence on the experimental results was explored. The XRD results show that when the Mg content increases from 1% to 26.5%, the characteristic peak of MgAl₂O₄ increases, and the characteristic peak of FeAl₂O₄ gradually disappears, indicating that Mg weakens the interaction between Fe and Al. SEM shows that the size of oxygen carrier particles decrease after adding Mg, and the sintering resistance is excellent. Based on the experiments of different coal/oxygen-carrier mass ratio, the carbon conversion and hydrogen production were the highest when the mass ratio was 0.5/15. Among the oxygen carriers with different Mg contents, Fe40Mg20Al40 has the best reaction performance, and the carbon conversion and hydrogen production are 81.75% and 1.7182L/g, which increase by 10.2% and 58.5% compared with Fe40Al60, respectively. After 10 cycles, the surface of Fe40Mg20Al40 is only slightly sintered, and the carbon conversion and hydrogen production are above 78% and 1.52L/g, respectively, showing good cycling performance. The addition of Mg can effectively inhibit the formation of FeAl₂O₄, significantly enhance the reactivity of steam oxidation process, and greatly increase the yield of hydrogen, which is very suitable for coal chemical looping hydrogen generation.

Key words: Fe-based oxygen carrier, FeAl₂O₄, MgAl₂O₄, chemical looping hydrogen generation, coal

摘要：

目前化学链过程常用的Fe₂O₃/Al₂O₃载氧体会形成FeAl₂O₄，因热力学限制很难与水反应制氢。为了抑制FeAl₂O₄的形成，本文向Fe/Al载氧体中添加Mg，在固定床上进行煤化学链制氢（CLHG），深入分析Mg的作用机理并探究其对实验结果的影响。XRD结果表明，Mg质量分数从1%增加到26.5%时，MgAl₂O₄特征峰增强，FeAl₂O₄特征峰逐渐消失，说明Mg减弱了Fe和Al之间的相互作用。SEM显示Mg添加后载氧体颗粒减小，耐烧结性能优异。对比不同煤/载氧体质量比的实验，质量比为0.5/15时碳转化率和产氢量最高。在不同Mg含量的载氧体中，Fe40Mg20Al40具备最好的反应性能，碳转化率和产氢量为81.75%和1.7182L/g，比Fe40Al60分别增加10.2%和58.5%。Fe40Mg20Al40经10次循环，表面仅有轻微烧结，碳转化率和产氢量均在78%和1.52L/g以上，循环性能良好。添加Mg可以有效抑制FeAl₂O₄的生成，显著增强蒸汽氧化过程的反应活性，大幅提高氢气产量，十分适用于煤化学链制氢。

关键词: Fe基载氧体, FeAl₂O₄, MgAl₂O₄, 化学链制氢, 煤

CLC Number:

TQ116.2

AN Yang, YUAN Sijie, GAO Zhendong, WU Man, WANG Lingyun, GUO Qingjie. Chemical looping hydrogen generation of coal with oxygen carrier of Mg-modified Fe/Al[J]. Chemical Industry and Engineering Progress, 2022, 41(2): 648-654.

安阳, 袁思杰, 高振东, 吴曼, 王凌云, 郭庆杰. Mg修饰Fe/Al载氧体煤化学链制氢[J]. 化工进展, 2022, 41(2): 648-654.

Figures/Tables 12

References 24

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工业分析/%					元素分析/%
M_ad	A_ad	V_ad	FC_ad		C_ad	H_ad	N_ad	S_ad	O_ad
11.18	4.56	31.95	63.50		77.60	5.16	1.46	0.46	10.77

工业分析/%					元素分析/%
M_ad	A_ad	V_ad	FC_ad		C_ad	H_ad	N_ad	S_ad	O_ad
11.18	4.56	31.95	63.50		77.60	5.16	1.46	0.46	10.77

循环次数	Mg质量分数/%
新鲜载氧体	12.02
5次循环	11.97
10次循环	11.89

循环次数	Mg质量分数/%
新鲜载氧体	12.02
5次循环	11.97
10次循环	11.89

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