安 阳，袁思杰，吴 曼，王凌云，郭庆杰

(青岛科技大学 化工学院，山东 青岛 266042)

DOI:10.13732/j.issn.1008-5548.2022.01.010

收稿日期： 2021-04-19，修回日期：2021-10-12，在线出版时间：2021-12-01。

基金项目：国家自然科学基金联合基金重点项目，编号：U20A20124；国家重点研发计划项目，编号：2018YFB0605401；宁夏回族自治区重点研发计划(重大科技)项目，编号：2018BCE01002。

第一作者简介：安阳(1996—)，男，硕士研究生，研究方向为煤炭清洁利用。E-mail：ayaaa@126.com。

通信作者简介：郭庆杰(1967—)，男，教授，博士，博士生导师，研究方向为煤炭清洁利用。E-mail：qj_guo@yahoo.com。

摘要：为促进铁基载氧体的深度还原提高氢气产量，通过优化反应过程形成强化煤化学链制氢(强化煤CLHG)工艺。采用浸渍法制备铁基载氧体；以梅花井烟煤为原料，在固定床上研究煤与铁基载氧体的质量比对强化煤CLHG的影响；对比了三反应器煤CLHG和强化煤CLHG的制氢过程，对不同阶段的铁基载氧体进行XRD表征；对比二反应器、三反应器以及强化煤CLHG在6次循环实验中的碳转化率和氢气产量。结果表明：当煤与载氧体质量比为1:15时，氢气产量最高达1.74 L/g;强化煤CLHG中的铁基载氧体更多地被还原为FeO或Fe,还原程度加深，同时还原阶段的残炭在蒸汽氧化阶段进一步反应，使得氢气产量比三反应器煤CLHG的高18.4%;在6次循环实验中，强化煤CLHG的碳转化率与三反应器煤CLHG的相差不大，远高于二反应器煤CLHG的；强化煤CLHG的氢气产量始终高于二反应器煤CLHG和三反应器煤CLHG的；强化煤CLHG的单次最高氢气产量为1.76 L/g,循环累计氢气产量为9.54 L。强化煤CLHG缩短制氢时间，制氢能力更优异。

关键词：铁基载氧体；强化煤；化学链制氢；二反应器；三反应器

Abstract：In order to promote the deep reduction of Fe-based oxygen carrier and increase the yield of hydrogen, an enhanced coal chemical looping hydrogen generation(enhanced coal CLHG)was proposed by optimizing the reaction process. Fe-based oxygen carrier was prepared by impregnation method. Using Meihuajing bituminous coal as raw material, the effect of the mass ratio of coal and Fe-based oxygen carrier on the enhanced coal CLHG was studied on a fixed bed.The hydrogen generation of two-reactor, three-reactor and enhanced chemical looping hydrogen generation processes in six cycles of experiments were compared. The results show that when the mass ratio of coal to oxygen carrier is 1∶15, the maximum hydrogen yield is 1.74 L/g.The Fe-based oxygen carrier in the enhanced coal CLHG is more reduced to FeO or Fe, and the degree of reduction is deepened. At the same time, the carbon residue in the reduction stage is further reacted in the steam oxidation stage, making the hydrogen production 18.4% higher than that of the three-reactor coal CLHG. In the 6-cycle experiment, the carbon conversion rate of the enhanced coal CLHG is not much different from that of the three-reactor coal CLHG, which is much higher than that of the two-reactor coal CLHG.The hydrogen production of the enhanced coal CLHG is always higher than that of the two-reactor coal CLHG and the three-reactor coal CLHG. The maximum hydrogen output in a single cycle of the enhanced coal CLHG is 1.76 L/g, and the cumulative hydrogen output of the cycle is 9.54 L.The enhanced coal CLHG shortens the hydrogen production time, and the hydrogen production capacity is more excellent.

Keywords：Fe-based oxygen carrier; enhanced coal; chemical looping hydrogen generation; two-reactor; three-reactor

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