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Enhancing hydrothermal stability of framework Al in ZSM-5:From the view on the transformation between P and Al species by solid-state NMR spectroscopy

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Chinese Journal of Chemical Engineering 2020年第12期28卷 3052-3060页

作者： Lei Han Ying Ouyang Enhui Xing Yibin Luo zhijian da State Key Laboratory of Catalytic Materials and Reaction Engineering Research Institute of Petroleum ProcessingSinopecBeijing 100083China

HZSM-5,with good surface acidity and shape selectivity,was reported as hydrocarbon cracking catalyst for multiple decades,however the hydrothermal stability,especially dealumination of tetrahedrally coordinated framework aluminum(TFAl),has been proved extensively as one of the major challenges during reactionregeneration *** was proposed to stabilize TFAl and indeed it enhanced the hydrothermal ***,most of the phosphorus species would remain outside of the zeolite pore,mainly as polyphosphate species,and block the micropore severely,with only a limited portion introduced into the channel being able to interact with *** the pore size by alkali treatment(desilication)is one of the most convinced methods,but the details about specific P species during alkali treatment and its transformation upon hydrothermal activation is not acquired,thus the mechanism has not been fully ***,the P-containing species and its transformation during direct P modification and acid/alkali treatment followed by Pmodification have been studied,and the mechanism on the interaction between P and Al species has been investigated,using several analytical methods,especially Solid-state nuclear magnetic resonance(SSNMR)*** was found that the combination of desilication and subsequent phosphorus modification can enhance the activity of the ZSM-5 for the cracking of ethylcyclohexane,due to the better hydrothermal stabilization of acid sites by the enhanced interaction between phosphorus and TFAl,resulting from the improved accessibility of TFAl because of the successful generation of *** the acid treatment followed by phosphorus modification,with declined retention of crystallinity and P/Al ratio,monoclinic/orthorhombic transition during steam activation,and the failed generation of mesopores,would cause obvious aggregation of the phosphorus species and could not improve the hydrothermal stability of the ZSM-5 ef

关键词： Phosphorus modification TFAl NaOH/alkali treatment Interaction ZSM-5

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Hydrogenation Conversion of Phenanthrene over Dispersed Mo-based Catalysts

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China Petroleum Processing & Petrochemical Technology 2015年第3期17卷 7-14页

作者： Hu Yiwen da zhijian Wang Zijun SINOPEC Research Institute of Petroleum Processing

With oil-soluble molybdenum compound and sublimed sulfur serving as raw materials, two dispersed Mo-based catalysts were prepared, characterized and then applied to the hydrogenation conversion of phenanthrene. The test results showed that under the conditions specified by this study, the catalyst prepared in a higher sulfiding atmosphere was more catalytically active due to its higher content of MoS2 and stronger intrinsic catalytic activity of MoS2 unit, which demonstrated that the sulfiding atmosphere for the preparation of catalysts not only could influence the yield of MoS2 but also the structure of *** analysis on the selectivity of octahydrophenanthrene isomers revealed that the catalyst prepared in a lower sulfiding atmosphere had a relatively higher catalytic selectivity to the hydrogenation of outer aromatic ring and the structure of catalysts could be modified under the specific reaction conditions. Moreover, the selectivity between the isomers of as-octahydrophenanthrene at different reaction time and temperature was analyzed and, based on the results, a hydrogenation mechanism over dispersed Mo-based catalysts was suggested, with monatomic hydrogen transfer and catalytic surface desorption of the half-addition intermediates functioning as the key points. In addition, it is concluded that the catalyst prepared in a lower sulfiding atmosphere was more capable of adsorption than the other one.

关键词： dispersed Mo-based catalysts phenanthrene conversion MoS2 structure product selectivity hydrogenationmechanism

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Phosphorous-Modified Carbon Nanotube-Supported Pt Nanoparticles for Propane Dehydrogenation Reaction

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China Petroleum Processing & Petrochemical Technology 2019年第1期21卷 7-14页

作者： Liu Jie Liu Changcheng da zhijian Zheng Huidong College of Chemical Engineering Fuzhou University SINOPEC Research Institute of Petroleum Processing

The sintering of Pt nanoparticles is one of the main reasons for catalyst deactivation during the high-temperature propane dehydrogenation(PDH) reaction. Promoters and supports have been introduced to prolong the catalyst ***, it is still necessary to develop novel catalysts with robust stability. Herein, the phosphorus-modified carbon nanotube-supported Pt nanoparticles were employed for the PDH process. Phosphorus modification improves the Pt dispersion, effectively promoting the activity of Pt/P-CNTs. Additionally, the phosphorus-modified CNTs can interact strongly with Pt nanoparticles by improving the electron transfer or hybridization, stabilizing Pt nanoparticles from agglomeration, and significantly enhancing the catalyst stability.

关键词： propane dehydrogenation phosphorus-modified carbon nanotubes platinum catalyst strong metal-support interactions

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Influence of Dechlorination Temperature on Propane Dehydrogenation over Pt-θ-Al2O3

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China Petroleum Processing & Petrochemical Technology 2018年第4期20卷 1-7页

作者： Liu Jie Liu Changcheng Ma Aizeng da zhijian Zheng Huidong College of Chemical Engineering Fuzhou UniversityFuzhou 350116 SINOPEC Research Institute of Petroleum Processing Beijing 100083

Several Pt-θ-Al_2O_3 catalysts with similar ultra-low Cl contents were used to investigate the influence of dechlorination temperature on propane dehydrogenation reaction. The Pt-θ-Al_2O_3 catalyst treated at a highest dechlorination temperature showed a lowest propane rate and propylene selectivity. The scanning transmission electron microscopy showed that the dispersions of Pt nanoparticles decreased with an increasing dechlorination temperature. The temperature-programmed reduction analysis showed that higher dechlorination temperature could lead to strong interactions between the metal and support, making it difficult to reduce Pt nanoparticles. The temperature-programmed oxidation analysis implied that more coke was deposited on the metal for catalyst treated at higher dechlorination temperature. The Raman spectra and the H/C ratio showed that more side-reactions, such as cracking and severe deep dehydrogenation reactions, occurred on catalysts treated at higher dechlorination temperatures. Therefore, the lower the dispersion of Pt nanoparticles was, the stronger the metal-support interactions and increased side-reactions would be, resulting in lower catalytic activity for Pt-θ-Al_2O_3 treated with higher dechlorination temperature.

关键词： dechlorination temperature metal-support interactions θ-Al2O3 Pt nanoparticles propane dehydrogenation reaction

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Hydrocarbon Composition of Different VGO Feedstocks and Its Correlation with FCC Product Distribution

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China Petroleum Processing & Petrochemical Technology 2013年第1期15卷 32-39页

作者： Song Haitao Jiao Guofeng Zhu Xinyi Zhou Xiang Zhu Yuxia da zhijian Research Institute of Petroleum Processing SINOPECBeijing 100083

Three different types of VGO were selected and cut into various distillates by true boiling-point distillation （TBD）, and the distillates were further separated into different components （saturates, aromatics and resins） via solid phase extrac- tion （SPE）. The hydrocarbon components in saturates and aromatics were characterized on the quasi-molecular level by GC/ MS and CJC/TOF MS. Cracking reactions of VGO, their distillates, and hydrocarbon components （saturates and aromatics） were performed on an ACE （model AP） unit. Nine correlation parameters （mainly based on the previous assumption of basic structure Units, BSU） which could better reflect the structures and compositions of hydrocarbons were put forward based on the quasi-molecular level analysis data, and correlated with FCC product distribution by multi-regression method. A series of correlation formulas were obtained. The formulas were further verified by comparing experimental and calculated FCC yields emanated from two other VGO feedstocks.

关键词： fluid catalytic cracking VGO product distribution hydrocarbon composition correlation

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The Effect of Non-Framework Aluminum on the Stability and Activity of REY Zeolite

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China Petroleum Processing & Petrochemical Technology 2005年第2期7卷 47-51页

作者： Chen Beiyan Shen Ningyuan He Mingyuan Tian Huiping da zhijian Research Institute of Petroleum Processing Beijing 100083

The present study is focused on the influence of a routine step, washing, following the preparation of calcined rare earth exchanged Y zeolite, on its hydrothermal stability. The hydrothermal stability of REY products, which were washed by different reagents, was observed and characterized by XRD, ICP, NMR, etc. The results reveal that the amount and the chemical type of the acidic media used for washing can significantly influence the content of remaining non-framework aluminum (NFA) and consequently further affect the hydrothermal stability of the washed REY products. The content of remaining non-framework aluminum can be well correlated with the crystallinity of REY products.

关键词： rear earth Y zeolite hydrothermal stability non-framework aluminum

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Selective Hydrogen Transfer Reaction in FCC Process:Characterization and Application

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China Petroleum Processing & Petrochemical Technology 2003年第3期5卷 45-48页

作者： Chen Beiyan He Mingyuan da zhijian(Research Institute of Petroleum Processing, Beijing, 100083) Res. Inst. of Petroleum Processing Beijing 100083 China

The product distribution and gasoline quality of FCC process, especially the olefin content,heavily depends on the catalyst performance in terms of selective/non-selective hydrogen transfer reaction selectivity. A reliable experimental protocol has been established by using n-dodecane as a probe molecule to characterize the selective hydrogen transfer ability of catalytic materials. The results obtained have been correlated with the performance of the practical catalysts.

关键词： catalytic cracking hydrogen transfer olefin reduction.

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纳米碳材料催化乙苯脱氢制苯乙烯的研究进展

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石油学报（石油加工） 2018年第2期34卷 398-409页

作者：吴耿煌荣峻峰达志坚中国石化石油化工科学研究院北京100083

乙苯脱氢制苯乙烯是工业上十分重要的反应。以纳米碳材料为催化剂,催化乙苯脱氢制苯乙烯是纳米碳材料领域近年来的研究热点之一。相比于传统的金属氧化物催化剂,纳米碳材料既可以在较低温度下高活性地催化乙苯氧化脱氢,也可以高选择性... 详细信息

乙苯脱氢制苯乙烯是工业上十分重要的反应。以纳米碳材料为催化剂,催化乙苯脱氢制苯乙烯是纳米碳材料领域近年来的研究热点之一。相比于传统的金属氧化物催化剂,纳米碳材料既可以在较低温度下高活性地催化乙苯氧化脱氢,也可以高选择性地催化乙苯直接脱氢,且反应过程中无需通入水蒸气,极大地提高了能源利用效率,具有较大的发展潜力。综述了近年来纳米碳材料催化乙苯脱氢制苯乙烯的研究进展,主要包括纳米碳材料的结构和表面化学性质、纳米碳催化剂的研究进展、催化乙苯脱氢反应机理等方面,同时总结了该领域存在的挑战并对前景进行了展望。

关键词：纳米碳乙苯脱氢苯乙烯纳米金刚石碳纳米管石墨烯

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催化裂化过程中苯并噻吩的转化规律

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石油学报（石油加工） 2013年第1期29卷 6-12页

作者：吴群英达志坚朱玉霞中国石化石油化工科学研究院北京100083

在固定流化床装置上,采用USY-Cat和V-USY-Cat催化剂,考察了苯并噻吩与四氢萘以不同比例混合进料在催化剂作用下的转化路径和硫分布。结果表明,苯并噻吩在催化裂化过程中主要发生氢转移-裂化、缩合、烷基转移和歧化反应。纯苯并噻吩很难... 详细信息

在固定流化床装置上,采用USY-Cat和V-USY-Cat催化剂,考察了苯并噻吩与四氢萘以不同比例混合进料在催化剂作用下的转化路径和硫分布。结果表明,苯并噻吩在催化裂化过程中主要发生氢转移-裂化、缩合、烷基转移和歧化反应。纯苯并噻吩很难开环裂化脱硫,其气体硫、液体硫和焦炭硫的摩尔选择性分别为0.45%、49.71%和49.84%。四氢萘的加入改变了苯并噻吩反应路径的选择性,使气体硫的摩尔选择性略有增加,焦炭硫的摩尔选择性下降到3.18%。催化剂的酸性质对产物硫分布也有影响,酸密度越高,越有利于气体硫的生成;V的加入提高了USY-Cat催化剂的L酸/B酸比,使焦炭硫的选择性上升。

关键词：苯并噻吩催化裂化硫分布钒氢转移

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氢气在二硫化钼上活化机理的研究进展

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石油学报（石油加工） 2015年第3期31卷 812-820页

作者：胡意文达志坚王子军中国石化石油化工科学研究院北京100083

介绍了MoS2的结构和催化性能,从光谱、实验以及理论计算等方面综述氢气在MoS2上活化机理的研究进展。当MoS2的硫化度较高时,氢分子吸附在其边缘处的端基S或桥S上后被均裂成2个SH,并经过氢迁移、H2S释放等过程降低了硫化度;当MoS2硫化度... 详细信息

介绍了MoS2的结构和催化性能,从光谱、实验以及理论计算等方面综述氢气在MoS2上活化机理的研究进展。当MoS2的硫化度较高时,氢分子吸附在其边缘处的端基S或桥S上后被均裂成2个SH,并经过氢迁移、H2S释放等过程降低了硫化度;当MoS2硫化度较低时,氢分子则主要被Mo—S活性位异裂成S—H和M—H。氢分子活化后形成的表面吸附态氢能在相邻原子间迁移,有利于提高MoS2活化氢气的效率。异裂氢分子的活性位Mo—S本质上为一Lewis酸碱对,因此其他分子在其上的竞争吸附不可避免地影响氢分子的活化路径和效率。

关键词：二硫化钼氢气活化解离吸附 Lewis酸碱对竞争吸附

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