Influence of the Preparation Procedure on the State of Platinum and on the Isomerizing Ability of Catalysts for Isodewaxing of High-Molecular-Mass Hydrocarbon Feedstock

IF 1.1 4区 工程技术 Q3 CHEMISTRY, ORGANIC
Roman A. Maslenkin, Irina A. Shamanaeva, Ekaterina E. Vorob’eva, Anastasiya A. Chemes, Andrei V. Volik, Roman E. Yakovenko, Pavel A. Simonov, Vsevolod A. Vdovichenko, Ekaterina V. Parkhomchuk
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Abstract

Granulated catalytic materials based on Al2O3 + SAPO-11 with Pt deposited either onto Al2O3 with the subsequent mixing with SAPO-11 or onto granulated composite support Al2O3 + SAPO-11 were prepared. The catalyst supports were prepared with the addition of polystyrene template to the mixture of support precursors or without template. The materials were characterized by Fourier IR spectroscopy of adsorbed pyridine, mercury and nitrogen porosimetry, X-ray diffraction analysis, inductively coupled plasma atomic emission spectroscopy, electron microscopy, and CO chemisorption. In all the samples, platinum was uniformly distributed over the granule cross section. The most pronounced platinum aggregation was observed in supports prepared without template and in those prepared by admixing SAPO-11 to Pt/Al2O3 (compared to the deposition onto the composite support). The template catalysts are characterized by increased CO/Pt stoichiometry (according to the СО chemisorption data) and larger particle size (according to electron microscopy data), which is due to high surface defectiveness and formation of Pt particles of unusual flat morphology. Strong metal–support interaction in these samples was confirmed by the presence of high-temperature H2 uptake peaks (above 750°С) in the temperature-programmed reduction (TPR) experiments; such peaks were absent in the TPR spectra of the analogs prepared without template. The template samples have also high total specific pore volume (0.6–0.8 cm3/g). Catalytic trials have shown that, under the conditions of the С18+ feed dewaxing, the target liquid product is formed exclusively in the presence of catalysts prepared by the template procedure, which demonstrates essential advantage of this approach and apparent shift of the process toward isomerization.

制备工艺对铂态及高分子质量烃原料异脱蜡催化剂异构化能力的影响
制备了基于Al2O3 + SAPO-11的颗粒状催化材料,将Pt沉积在Al2O3上,再与SAPO-11混合,或沉积在颗粒状复合载体Al2O3 + SAPO-11上。在载体前体混合物中加入聚苯乙烯模板或不加入模板制备催化剂载体。采用吸附吡啶的傅立叶红外光谱、汞氮孔隙度、x射线衍射、电感耦合等离子体原子发射光谱、电子显微镜和CO化学吸附对材料进行了表征。在所有样品中,铂均匀分布在颗粒截面上。与沉积在复合支架上相比,在没有模板制备的支架和将SAPO-11与Pt/Al2O3混合制备的支架中观察到最明显的铂聚集。模板催化剂的特点是CO/Pt化学计量增加(根据СО化学吸附数据)和更大的颗粒尺寸(根据电子显微镜数据),这是由于高表面缺陷和形成异常扁平形态的Pt颗粒。在程序升温还原(TPR)实验中,高温H2吸收峰(750°С以上)的存在证实了这些样品中存在强的金属-载体相互作用;无模板制备的类似物在TPR光谱中不存在这些峰。模板样品也具有较高的总比孔容(0.6-0.8 cm3/g)。催化实验表明,在С18+进料脱蜡条件下,目标液体产物只在模板法制备的催化剂存在下形成,这表明了该方法的本质优势,并明显向异构化转变。
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来源期刊
Petroleum Chemistry
Petroleum Chemistry 工程技术-工程:化工
CiteScore
2.50
自引率
21.40%
发文量
102
审稿时长
6-12 weeks
期刊介绍: Petroleum Chemistry (Neftekhimiya), founded in 1961, offers original papers on and reviews of theoretical and experimental studies concerned with current problems of petroleum chemistry and processing such as chemical composition of crude oils and natural gas liquids; petroleum refining (cracking, hydrocracking, and catalytic reforming); catalysts for petrochemical processes (hydrogenation, isomerization, oxidation, hydroformylation, etc.); activation and catalytic transformation of hydrocarbons and other components of petroleum, natural gas, and other complex organic mixtures; new petrochemicals including lubricants and additives; environmental problems; and information on scientific meetings relevant to these areas. Petroleum Chemistry publishes articles on these topics from members of the scientific community of the former Soviet Union.
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