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Ce改性Ni/SAPO-11催化剂对烃基生物柴油制备的影响OA

Effect of Ce Modification on Ni/SAPO-11 Catalysts for the Preparation of Hydrocarbon-based Biodiesel

中文摘要英文摘要

以自主合成的SAPO-11分子筛为载体,Ce(NO3)3为Ce源,采用等体积浸渍法制备了不同Ce负载量(以催化剂总质量中Ce质量分数计,1%~7%)的Ni-xCe/SAPO-11催化剂,通过多种表征技术对催化剂进行表征,并评价其对脂肪酸甲酯(FAME)一步加氢脱氧异构制备烃基生物柴油的催化性能及循环稳定性.研究结果表明:Ce的引入未破坏分子筛构型,提高了催化剂比表面积,降低了酸强度,增加了载体表面碱性位和Ni活性位点分散度.其中Ni-5Ce/SAPO-11的比表面积达173 m2/g、孔容达0.13 cm3/g,扩孔作用明显,而过量Ce的负载会使催化剂比表面积有所下降.Ni-5Ce/SAPO-11催化剂在300℃反应4 h时,FAME的转化率达100%,C15~C18选择性为98.4%,异构率达24.9%,催化性能最优.此外,Ce的添加提升了催化剂的循环稳定性,其中Ni-7Ce/SAPO-11经4次循环后长链烷烃C15~C18选择性仍可达83.4%.

Self-synthesized SAPO-11 molecular sieve was used as the carrier and Ce(NO3)3 as the Ce source to prepare a series of Ni-xCe/SAPO-11 catalysts with different Ce loadings(the mass fraction of Ce element in the total catalyst mass,1%-7%)by the incipient wetness impregnation method.The catalysts were characterized by various techniques,and their catalytic performance and cyclic stability were evaluated for the one-step hydro-deoxygenation and isomerization of fatty acid methyl ester(FAME)to produce hydrocarbon-based biodiesel.The results indicated that the introduction of Ce increased the specific surface area of the catalyst,enhanced the surface basic sites and improved the dispersion of Ni active sites,without reducing the acid strength and destroying the molecular sieve configuration.Among the catalysts,Ni-5Ce/SAPO-11 exhibited a specific surface area of 173 m2/g and a pore volume of 0.13 cm3/g,indicating a clear pore-expansion effect,whereas excessive Ce loading would lead to a decrease in specific surface area.The optimal performance was observed over Ni-5Ce/SAPO-11 at 300 ℃ for 4 h,giving 100%FAME conversion,98.4%C15-C18 alkane selectivity and a 24.9%isomerization rate.Furthermore,the addition of Ce improved the cyclic stability of the catalyst,and the selectivity to long-chain alkanes(C15-C18)over Ni-7Ce/SAPO-11 remained as high as 83.4%after four reaction cycles.

林昕;王德超;姚权;林健;李水荣;郑志锋

厦门大学能源学院,福建厦门 361102厦门大学能源学院,福建厦门 361102厦门大学能源学院,福建厦门 361102厦门大学能源学院,福建厦门 361102厦门大学能源学院,福建厦门 361102厦门大学能源学院,福建厦门 361102

化学化工

烃基生物柴油加氢异构Ni/SAPO-11稀土金属Ce

hydrocarbon-based biodieselhydrogenation isomerizationNi/SAPO-11rare earth metal Ce

《林产化学与工业》 2026 (3)

47-53,7

国家自然科学基金资助项目(32271799,325B2071)福建省自然科学基金资助项目(2024J08017)厦门市自然科学基金资助项目(3502Z202371008)

10.20195/j.issn.0253-2417.2024223

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