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Monolithic oxygen carrier applied to fixed bed methane chemical chain steam reforming and preparation method of monolithic oxygen carrier
The invention relates to a preparation method of a monolithic oxygen carrier applied to fixed bed methane chemical chain steam reforming. The monolithic oxygen carrier has a layered structure, the surface layer is perovskite type LaFe0.3Mn0.7O<3+delta>, and the mass ratio of the perovskite type LaFe0.3Mn0.7O<3+delta> is 10-15wt%; and the internal part is CeO2-Fe2O3-Al2O3 foamed ceramic, and the mass ratio of CeO2 to Fe2O3 to Al2O3 is (2-9): (4-18): 1. According to the invention, a direct foaming method and a pore-forming agent method are combined to obtain high-porosity CeO2-Fe2O3-Al2O3 open-cell foamed ceramic, and then LaFe0.3Mn0.7O<3+delta> is loaded on the surface of the foamed ceramic by adopting a citric acid complexing impregnation method to obtain the monolithic oxygen carrier. The prepared monolithic oxygen carrier couples the good reforming performance of perovskite type LaFe0.3Mn0.7O<3+delta>, the rapid oxygen migration ability of CeO2 and the economical efficiency and oxygen carrying ability of Fe2O3/Fe3O4, the oxygen carrier is high in cycling stability, high in carbon deposition resistance and good in synthesis gas selectivity, and the monolithic oxygen carrier is suitable for the methane chemical chain steam reforming process. The preparation process is relatively simple, conditions are easy to control, and the monolithic oxygen carrier has the characteristics of high specific surface area and high activity component dispersity.
本发明涉及一种应用于固定床甲烷化学链水蒸气重整的整体式载氧体的制备方法。所述整体式载氧体具有分层结构，表面层为钙钛矿型的LaFe0.3Mn0.7O3+δ，其质量占比为10~15 wt.%；内部为CeO2‑Fe2O3‑Al2O3泡沫陶瓷，CeO2:Fe2O3:Al2O3质量比为2~9:4~18:1。本发明通过直接发泡法与造孔剂法相结合，得到高孔隙率CeO2‑Fe2O3‑Al2O3开孔泡沫陶瓷，随后采用柠檬酸络合浸渍法将LaFe0.3Mn0.7O3+δ负载于泡沫陶瓷表面，得到整体式载氧体。所制整体式载氧体耦合了钙钛矿型LaFe0.3Mn0.7O3+δ良好的重整性能、CeO2快速氧迁移能力与Fe2O3/Fe3O4的经济性和载氧能力，载氧体循环稳定性高、抗积碳能力强、合成气选择性好，适用于甲烷化学链水蒸气重整过程。本发明制备工艺相对简单，条件容易控制，具有高比表面积、高活性组分分散度的特点。
Monolithic oxygen carrier applied to fixed bed methane chemical chain steam reforming and preparation method of monolithic oxygen carrier
The invention relates to a preparation method of a monolithic oxygen carrier applied to fixed bed methane chemical chain steam reforming. The monolithic oxygen carrier has a layered structure, the surface layer is perovskite type LaFe0.3Mn0.7O<3+delta>, and the mass ratio of the perovskite type LaFe0.3Mn0.7O<3+delta> is 10-15wt%; and the internal part is CeO2-Fe2O3-Al2O3 foamed ceramic, and the mass ratio of CeO2 to Fe2O3 to Al2O3 is (2-9): (4-18): 1. According to the invention, a direct foaming method and a pore-forming agent method are combined to obtain high-porosity CeO2-Fe2O3-Al2O3 open-cell foamed ceramic, and then LaFe0.3Mn0.7O<3+delta> is loaded on the surface of the foamed ceramic by adopting a citric acid complexing impregnation method to obtain the monolithic oxygen carrier. The prepared monolithic oxygen carrier couples the good reforming performance of perovskite type LaFe0.3Mn0.7O<3+delta>, the rapid oxygen migration ability of CeO2 and the economical efficiency and oxygen carrying ability of Fe2O3/Fe3O4, the oxygen carrier is high in cycling stability, high in carbon deposition resistance and good in synthesis gas selectivity, and the monolithic oxygen carrier is suitable for the methane chemical chain steam reforming process. The preparation process is relatively simple, conditions are easy to control, and the monolithic oxygen carrier has the characteristics of high specific surface area and high activity component dispersity.
本发明涉及一种应用于固定床甲烷化学链水蒸气重整的整体式载氧体的制备方法。所述整体式载氧体具有分层结构，表面层为钙钛矿型的LaFe0.3Mn0.7O3+δ，其质量占比为10~15 wt.%；内部为CeO2‑Fe2O3‑Al2O3泡沫陶瓷，CeO2:Fe2O3:Al2O3质量比为2~9:4~18:1。本发明通过直接发泡法与造孔剂法相结合，得到高孔隙率CeO2‑Fe2O3‑Al2O3开孔泡沫陶瓷，随后采用柠檬酸络合浸渍法将LaFe0.3Mn0.7O3+δ负载于泡沫陶瓷表面，得到整体式载氧体。所制整体式载氧体耦合了钙钛矿型LaFe0.3Mn0.7O3+δ良好的重整性能、CeO2快速氧迁移能力与Fe2O3/Fe3O4的经济性和载氧能力，载氧体循环稳定性高、抗积碳能力强、合成气选择性好，适用于甲烷化学链水蒸气重整过程。本发明制备工艺相对简单，条件容易控制，具有高比表面积、高活性组分分散度的特点。
Monolithic oxygen carrier applied to fixed bed methane chemical chain steam reforming and preparation method of monolithic oxygen carrier
一种应用于固定床甲烷化学链水蒸气重整的整体式载氧体及其制备方法
XIAO YAN (author) / YIN XIANGLEI (author) / YAN JINGCHUN (author) / SHEN LAIHONG (author)
2021-09-24
Patent
Electronic Resource
Chinese
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