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pH操作窗口影响沉淀铁催化剂费托合成性能的研究

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以Na2CO3为沉淀剂, 在pH值介于6~8的条件下, 采用并流沉淀法制备了费托 (F-T) 合成沉淀铁Fe-Cu-K-SiO2催化剂.利用X射线衍射 (XRD) 、N2吸附/脱附、氢气程序升温还原 (H2-TPR) 及穆斯堡尔谱 (MES) 对催化剂的晶型结构、晶粒尺寸、孔结构、还原性能及碳化程度进行了表征, 并在工业测试条件下考察了沉淀铁制备pH值对其催化费托合成反应性能的影响.结果表明, 该操作窗口内pH值的变化对催化剂物化性能影响显著, 提高沉淀pH值所制催化剂的晶粒增大, 比表面积降低, 从而增加了其还原和碳化的难度, 使得相应催化剂的CO转化率和CH4选择性降低, 而CO2和C5+选择性增加.将MES表征结果与催化性能关联, 发现CO转化率与Fe5C2相密切相关, 而CO2的选择性主要与Fe3O4相相关.
Effect of pH on the catalytic properties of precipitated iron for Fischer-Tropsch synthesis
A serial of Fischer-Tropsch synthesis catalysts (Fe-Cu-K-SiO2) was prepared by the coprecipitation method with varied pH of 6~8.The properties of the catalysts, i.e.crystal phase, particle size, pore structure, reducibility and carburization, were studied by XRD, N2adsorption, H2-TPR, and M9ssbauer spectroscopy.The catalysts were evaluated for Fischer-Tropsch synthesis under typical industrial conditions.The results indicate that the increase of pH values increases the particle size and decreases the surface area, which inhibit the reduction and carburization of the catalysts.As a result, a lower CO conversion and a lower selectivity of CH4but a higher selectivity of CO2and C5+products were obtained in Fischer-Tropsch synthesis.By correlating the M9ssbauer characterization with catalytic results, the CO conversion is revealed to be dependent on the Fe5C2phase while CO2selectivity is related to Fe3O4phase over the catalyst.

precipitated ironFischer-Tropsch synthesispHparticle sizeactive phase

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北京低碳清洁能源研究院,北京 102211

沉淀铁催化剂 费托合成 pH值 晶粒 活性相

国家重点研发计划

2017YFB0602500

2019

陕西师范大学学报(自然科学版)
陕西师范大学

陕西师范大学学报(自然科学版)

CSTPCDCSCD北大核心
影响因子:0.563
ISSN:1672-4291
年,卷(期):2019.47(1)
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