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Catalytic Hydrogenation, Hydrocracking and Isomerization Reactions of Biomass Tar Model Compound Mixture over Ni-modified Zeolite Catalysts in Packed Bed Reactor
Renewable Energy ( IF 9.0 ) Pub Date : 2021-04-01 , DOI: 10.1016/j.renene.2020.11.098
Andrii Kostyniuk , David Bajec , Blaž Likozar

Abstract Gas-phase conversion of a model mixture of biomass tar (5 wt.% naphthalene and 95 wt.% of 1-methylnaphthalene) into 2-methylnaphthalene liquid product and ethylene and propane gas mixture was carried out over different zeolites and metal promoted zeolites in a packed-bed reactor for the first time. In the present work, a series of MFI (HZSM-5), BEA (Hβ), FAU (HY, HUSY), and MOR (H-Mordenite) zeolites were investigated. The effect of Ni metal addition on the promotion of parent zeolite catalysts was studied. The most successful catalysts were characterized by BET, ICP-AES, XRD, HRSEM, STEM-HAADF, and STEM-BF with EDXS, NH3-TPD, H2-TPR, TGA, and pyridine-DRIFT techniques. The superior performance in comparison to the other studied catalysts was established over the 5wt.%Ni/HZSM-5 (SiO2/Al2O3 = 30) with 96.2 mol% of selectivity to 2-methylnaphthalene in the liquid phase, 90 mol% total conversion with the highest part (82.9 wt.%) of ethylene and propane in the gas phase after 24 h time-on-stream. This high catalytic performance of the 5wt.%Ni/HZSM-5 catalyst can be attributed to the presence of the high mesopore volume, pore diameter, and high mesopore surface area, the existence of the redox active sites, and the presence of strong Lewis acid sites due to synergetic interaction between Ni metal species and zeolite acid support. Based on the product distributions observed, the reaction scheme of the conversion of biomass tar model mixture of naphthalene and 1-methylnaphthalene over studied catalysts was proposed. Our catalytic results obtained over pristine and Ni-modified zeolite catalysts shed light on the potential use of these catalysts in the biomass tar valorization process under atmospheric pressure.

中文翻译:

填充床反应器中Ni改性沸石催化剂对生物质焦油模型化合物混合物的催化加氢、加氢裂化和异构化反应

摘要 生物质焦油模型混合物(5 wt.% 萘和 95 wt.% 1-甲基萘)在不同的沸石和金属促进沸石上进行气相转化为 2-甲基萘液体产品和乙烯和丙烷气体混合物第一次在填充床反应器中。在目前的工作中,研究了一系列 MFI (HZSM-5)、BEA (Hβ)、FAU (HY、HUSY) 和 MOR (H-丝光沸石) 沸石。研究了Ni金属添加对母体沸石催化剂的促进作用。最成功的催化剂通过 BET、ICP-AES、XRD、HRSEM、STEM-HAADF 和 STEM-BF 与 EDXS、NH3-TPD、H2-TPR、TGA 和吡啶-漂移技术进行表征。与其他研究的催化剂相比,其优越的性能是在 5wt.% Ni/HZSM-5 (SiO2/Al2O3 = 30) 和 96 上建立的。在液相中对 2-甲基萘的选择性为 2 mol%,总转化率为 90 mol%,在运行 24 小时后气相中乙烯和丙烷的最高部分 (82.9 wt.%)。5wt.%Ni/HZSM-5 催化剂的这种高催化性能可归因于高介孔体积、孔径和高介孔表面积的存在、氧化还原活性位点的存在以及强路易斯的存在。由于 Ni 金属物质和沸石酸载体之间的协同相互作用,因此产生了酸性位点。基于观察到的产物分布,提出了在所研究的催化剂上转化生物质焦油模型混合物萘和1-甲基萘的反应方案。
更新日期:2021-04-01
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