Thermodynamic evaluation and experimental investigation of CaO-assisted Fe-based chemical looping reforming process for syngas production
Thermodynamic evaluation and experimental investigation of CaO-assisted Fe-based chemical looping reforming process for syngas production
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CaO辅助铁基化学循环重整合成气工艺热力学评价及实验研究
DOI：
10.1016/j.apenergy.2021.116614
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发表时间：
2021-04
期刊：
影响因子：
11.2
通讯作者：
Zhiwu Liang
中科院分区：
文献类型：
--
作者：
Yunlei Zhao;Bo Jin;Xiao Luo;Zhiwu Liang
铁基载氧体在化学链部分氧化重整过程中的反应活性和价态转变是国内外研究的热点。但是，以CaO作为CO2载体，实现CO2捕集与利用的同时，其重整性能及操作因素的影响尚不清楚。在这项工作中，热力学平衡计算，反应性测试和材料表征进行优化的过程特性。考察了进料条件（Fe/Al质量比、甲烷量、Ca/Fe摩尔比和装填方式）对反应活性的影响，揭示了CaO和Fe 2 O3之间的相互作用。气体产物分布表明，积碳和氧化程度与CH 4含量密切相关。CaCO 3和Fe 2 O3重整反应之间的空间构型对获得理想的重整产物至关重要。实验和理论相组成上FeO存在的差异说明反应程度受还原剂用量的影响。通过比较CaCO 3、Fe 2 O3及其混合物的甲烷程序升温反应，认为CaCO 3的存在有利于促进铁基甲烷重整反应。该研究为提高化学链重整反应程度和优化过程特性提供了一条途径。
Many works have focused on the reactivity and valence transition of Fe-based oxygen carriers in chemical looping partial oxidation reforming process. However, the reforming performance and impacts of operating factors are unclear with the co-feeding of CaO being CO2carrier to realize simultaneous CO2capture and utilization. In this work, thermodynamic equilibrium calculation, reactivity test and material characterization are carried out to optimize the process characteristics. The impacts of feeding conditions (Fe/Al weight ratio, methane amount, Ca/Fe mole ratio and packing manner) on the reforming reactivity are obtained to reveal the interaction between CaO and Fe2O3. The gas product distribution indicates that the carbon deposition and oxidation degree is closely related to CH4amount. The spatial configuration between CaCO3and Fe2O3reforming is essential to obtain the desirable reforming products. The difference of FeO existence on the theoretical and experimental phase components illustrates that reaction degree is affected by the reduction agent amount. By comparing the methane temperature-programmed reaction of CaCO3, Fe2O3and their mixture, it is suggested that the existence of CaCO3is beneficial for accelerating iron-based methane reforming. This study provides a way to improve reaction degree and optimize process characteristic for chemical looping reforming process.
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