Hydrodeoxygenation of fatty acid methyl esters and isomerization of products over NiP/SAPO-11 catalysts
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摘要: 采用过量浸渍法制备了不同镍负载量的NiP/SAPO-11催化剂，并用N2吸附-脱附、吡啶红外光谱、NH3-TPD、H2-TPR等技术对催化剂的物理化学性能进行了测试。脂肪酸甲酯催化加氢脱氧及产物异构化反应在固定床反应器上进行，液体产品分别用GC-MS和GC进行定性和定量分析。结果表明，在温度为340℃，压力为2.0 MPa，氢气流量为60 mL/min，重时空速为2.5 h-1的操作条件下，当Ni负载量为3%（质量分数）时，原料转化率可以达到97.8%，C15-18的收率84.5%，异构化率14.0%。
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关键词:
- 脂肪酸甲酯 /
- NiP/SAPO-11 /
- 加氢脱氧 /
- 异构化
Abstract: NiP/SAPO-11 catalysts with various nickle loading amounts were prepared by the impregnation method, and their properties were determined by means of N2 adsorption-desorption, DRIFTS of adsorbed pyridine, NH3-TPD and H2-TPR. The catalytic hydrodeoxygenation of fatty acid methyl esters (FAME) and isomerization of consecutive paraffin products were carried out in a fixed-bed continuous-flow reactor. Liquid products were qualitatively and quantitatively identified by GC-MS and GC respectively. Under the operation conditions of 340℃, 2.0 MPa, WHSV of 2.5 h-1, H2 of 60 mL/min, the catalyst with 3% nickel loading (mass content) attained the high conversion of FAME (97.8%), C15-18 yield (84.5%) and isomerization rate (14.0%).-
Key words:
- FAME /
- NiP/SAPO-11 /
- hydrodeoxygenation /
- isomerization
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图 1 不同Ni负载量的催化剂的N2吸附等温线
Figure 1 N2 adsorption-desorption isotherms of catalysts with various nickel contents
图 2 不同Ni负载量的H2-TPR谱图
Figure 2 H2-TPR profiles of catalysts with various nickel contents
a: 13%; b: 10%; c: 8%; d: 5%; e: 3%; f: 1%
图 3 3%NiP(1/1) /SAPO-11的吸附吡啶红外光谱谱图
Figure 3 DRIFTS spectra of pyridine adsorbed on 3%NiP(1/1) /SAPO-11
图 4 不同Ni负载量的催化剂的NH3-TPD谱图
Figure 4 NH3-TPD profiles of catalysts with different nickel contents
a: 13%; b: 10%; c: 8%; d: 5%; e: 3%; f: 1%
图 5 Ni负载量对原料的转化率和C15-18收率的影响
Figure 5 Conversion rates of FAME and yields of C15-18 over catalysts with various Ni contents
图 6 异构化率随Ni负载量的变化
Figure 6 Isomerization rates over catalysts with different Ni contents
表 1 不同Ni负载量的催化剂的孔容和平均孔径和比表面积
Table 1 Pore volume, average pore diameter, and specific surface areas of catalysts with various nickel contents
Catalyst Pore volume v/(cm3·g-1) Average pore diameter d/nm Specific surface area A/(m2·g-1) SAPO-11 0.250 6.51 176.53 1%NiP(1/1) /SAPO-11 0.234 7.72 155.74 3%NiP(1/1) /SAPO-11 0.184 6.51 120.09 5%NiP(1/1) /SAPO-11 0.169 3.82 117.97 8%NiP(1/1) /SAPO-11 0.116 3.83 90.49 10%NiP(1/1) /SAPO-11 0.086 3.82 80.77 13%NiP(1/1) /SAPO-11 0.089 3.83 56.84 
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