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| 1 | Heterogeneous oxidation of cyclohexanone catalyzed by TS-1:Combined experimental and DFT studies显示文摘 | Changjiu Xia Long Ju Yi Zhao Hongyi Xu Bin Zhu Feifei Gao Min Lin Zhenyu Dai Xiaodong Zou Xingtian Shu | 2015 | 催化学报2015，36，6： | 11 |
| 2 | A “Green” Cyclohexanone Oxidation Route Catalyzed by Hollow Titanium Silicate Zeolite for Preparing ε-Caprolactone,6-Hydroxyhexanoic Acid and Adipic Acid显示文摘Hollow titanium silicalite (HTS) molecular sieve has been synthesized, and information on its structure, physico-chemical characterization, as well as surface property was investigated by a host of analytical methods, such as XRF, XRD, low-temperature N2 adsorption/desorption, TEM, FT-IR, UV-Vis, 29Si MAS NMR, and XPS techniques. The characterization results suggest that HTS zeolite has a special hollow crystal structure and its mesopore volume is larger than that of TS-1 zeolite. The titanium species in this zeolite are composed of the framework tetrahedral Ti (IV) ions and extra-framework octahedral Ti (IV) ions, which tend to disperse into its bulk phase. This zeolite material also has been applied to catalyze the cyclohexanone oxidation process, and the products are not completely consistent with those results obtained by using TS-1 zeolite, which might be caused by their difference in pore structure and pore volume, especially the mesopore volume. Cyclohexanone oxidation catalyzed by HTS zeolite is a representative consecutive reaction, the main target products of which are e-caprolactone, 6-hydroxyhexanoic acid and adipic acid. The effect of H2O2/cyclohexanone mole ratio on the cyclohexanone conversion, the total target product selectivity, the distribution of three target products selectivity and their variations along with reaction time is also researched and analyzed, which indicate that HTS zeolite shows a high performance for the Baeyer-Villiger reaction of cyclohexanone and catalytic oxidation of 6-hydroxyhexanoic acid under mild conditions, and the quantity of active surface titanium species as well as the pore structure and mesopore volume controlling the mass diffusion rate are the key factors determining the catalytic activity of HTS zeolite and product selectivity. | Xia Changjiu Zhu Bin Lin Min Shu Xingtian | 2012 | China Petroleum Processing & Petrochemical Technology2012，14，4： | 5 |
| 3 | Study on the Mechanisms for Baeyer-Villiger Oxidation of Cyclohexanone with Hydrogen Peroxide in Different Systems显示文摘The green and effective Baeyer-Villiger oxidation reaction of cyclohexanone for preparing ε-caprolactone is of particular importance in the synthesis of new polymer materials. We have discussed here several mechanism types of Baeyer-Villiger oxidation of cyclohexanone with H2O2 in different reaction systems. Five main types have been addressed, i. e.: (1) the non-catalyzed reaction type, where the C=O of ketones is activated by H+, which is electrolytically dissociated from H2O2 and H2O, to improve the capability of C=O group for accepting the electron pairs; (2) the thermally activated radical reaction type, where the Criegee intermediate is produced via two steps of radical reaction with ·OH attack, with much more hydroxyl radicals being excited in the presence of TS-1 zeolite; (3) the Brnsted acid catalysis reaction type, where both O-O moiety and C=O group could be activated by Brnsted acid; (4) the solid Lewis acid catalyzed C=O of the substrate activation reaction type through enhancing the donor-acceptor interaction between the antibonding π*C=O orbital of cyclohexanone and HOMO of Sn-containing zeolites; and (5) the solid Lewis acid catalyzed H2O2 to form Me-OOH oxidative species by converting the highest occupied molecular orbital (HOMO) of Ti-OOH into a singly occupied molecular orbital (SOMO), making the O-O group highly electrophilic to attack the C=O of cyclohexanone during the Baeyer-Villiger oxidation process. In the end, we have also compared the different mechanisms and put forward our opinions on the development direction of catalytic materials aiming at eco-friendly Baeyer-Villiger oxidation of cyclohexanone in the years to come. | Xia Changjiu Lin Min Zhu Bin Shu Xingtian | 2012 | China Petroleum Processing & Petrochemical Technology2012，14，2： | 4 |
| 4 | The Function of β Zeolite for Enhancing the Propylene Yield in FCC Process显示文摘The ultra-stable Y zeolite, modified β zeolite, and modified ZSM-5 zeolite were characterized by NH3-TPD analysis. The results showed that the acidic substance of modified β zeolite is between that of the Y zeolite and the ZSM-5 zeolite. These three kinds of zeolites were evaluated by using hexane, decane and light diesel serving as feedstocks with different molecular size. The results showed that these three kinds of zeolites had different cracking capability and product distribution obtained for cracking hydrocarbons with different molecular sizes as a result of the difference in pore structure and acidic substances. The modified β zeolite can produce much more C_5~= —C_8~= olefins, which are excellent precursors of propylene. Then the mixed samples of these three kinds of zeolites were tested in the VGO microreactor unit, and the test results showed that the modified β zeolite played a ‘relay role' between the ultra-stable Y zeolite and the modified ZSM-5 zeolite, so that the composite made of the ultra-stable Y zeolite, the modified β zeolite, and the modified ZSM-5 zeolite showed a highest propylene yield and selectivity. | Ouyang Ying Luo Yibin Shu Xingtian | 2017 | China Petroleum Processing & Petrochemical Technology2017，19，4： | 4 |
| 5 | Hydrothermal Synthesis and Properties of Y-zeolite-containing Composite Material with Micro/mesoporous Structure显示文摘有 micro/mesoporous 结构的 Y-zeolite-containing 合成材料从白陶土被综合了借助于在原处结晶化方法。获得的样品被 XRD 调查并且赌了方法。商业 Y 沸石和新奇 Y-zeolite-containing 的催化活动的评估合成材料在脉搏被执行有不同分子的尺寸的二个探查分子的微层析的站台:VGO 化工物品和 1,3,5 tri-isopropyl 苯。Y-zeolite-containing 合成材料富于外部表面和 meso-/macro-pores,这被发现;Y-zeolite-containing 合成材料与商业 Y 沸石相比表明了释放的更小的率。 | Zhou Jihong Min Enze Shu Xingtian Zong Baoning Yang Haiying Luo Yibin (State Key Laboratory of Catalytic Material and Reaction Engineering,Research Institute of Petroleum Processing,SINOPEC,Beijing 100083) | 2010 | China Petroleum Processing & Petrochemical Technology2010，12，1： | 3 |
| 6 | Regeneration of Simulated Deactivated Hollow Titanium Silicate Zeolite by Secondary Crystallization in the TPAOH Solution显示文摘It is of paramount importance to improve the utilization efficiency of hollow titanium silicate(HTS) zeolite catalyst used in the cyclohexanone ammoxidation process. To achieve this aim, the regeneration of simulated deactivated HTS zeolite by post-synthesis was carried out in an aqueous TPAOH solution under hydrothermal conditions. It was found that the catalytic performance for phenol hydroxylation over regenerated HTS zeolite was as high as that of fresh one.Judging from the BET measurements, electron micrography and XRD analysis results, it was confirmed that the topological and morphological structure was repaired. The chemical state of Ti species was detected by the UV-Vis and ^(29)Si MAS NMR spectroscopy. No acidic amorphous TiO_2-SiO_2 oxide was formed, and the extraframework Ti species could be reincorporated into the framework of HTS zeolite thanks to the tetrahedral coordination by the condensation between Ti-OH and Si-OH groups. In order to confirm this conclusion, the fresh HTS zeolite was treated under the NH_3·H_2O hydrothermal and thermal conditions for several times. The catalytic activity of both uncalcined and calcined simulated deactivated HTS zeolite samples could be regenerated without the formation of Br?nsted acid sites. It was concluded that the highly dispersed Ti species could be reincorporated into the framework of zeolite by hydrated condensation of Si-OH and Ti-OH groups after secondary hydrothermal synthesis. | Xia Changjiu Lin Min Peng Xinxin Zhu Bin Xu Guangtong Shu Xingtian | 2017 | China Petroleum Processing & Petrochemical Technology2017，19，1： | 3 |
| 7 | Investigation on Organic Solvent Free Toluene Oxidative Bromination Reaction Catalyzed by HTS Zeolite显示文摘The toluene oxidative bromination reaction catalyzed by hollow titanium silicalite(HTS)zeolite in aqueous medium was investigated by employing H2O2 and HBr under mild conditions without the need for organic solvent.A high toluene conversion(90.7%)and high selectivity of mono-bromotoluene(99.0%)was achieved under the optimal reaction conditions.The UV-Raman spectroscopy was applied for the mechanism study and the result reveals that HTS is efficient for catalyzing the oxidation reaction of HBr with H2O2 to produce abundant active bromine species,which can further facilitate the toluene electrophilic bromination reaction.A two-step toluene bromination reaction mechanism involving the HTS catalyzed active bromine species“generation-conversion-utilization”process is proposed based on the UV-Raman spectroscopy analysis. | Peng Xinxin Xia Changjiu Lin Min Zhu Bin Luo Yibin Shu Xingtian | 2020 | China Petroleum Processing & Petrochemical Technology2020，22，4： | 2 |
| 8 | Environmentally-Friendly Catalytic Oxidation of Cyclohexanone with 30% H_2O_2 Solution: A Comparison Study between Hollow Titanium Silicate and Dealuminated HBEA Zeolites显示文摘Two clean liquid–phase cyclohexanone oxidation routes catalyzed by DHBEA and HTS zeolites, in the absence of organic solvents, have been developed for producing high value-added chemical intermediates. Under optimized conditions,the cyclohexanone conversion reaches up to 60%, and the selectivity of total target products(ε-caprolactone, 6-hydroxyhexanoic acid and adipic acid) is over 90% achieved by the HTS zeolite; while both cyclohexanone conversion and the 6-hydroxyhexanoic acid selectivity are over 95% obtained on the DHBEA zeolite. Both the Lewis and Br鰊sted acid sites of DHBEA zeolite can preferentially activate the carbonyl group of cyclohexanone without any impact on H_2O_2 molecules.Meanwhile, the HTS zeolite can predominantly make H_2O_2 more reactive, which agrees well with the molecular calculation results. Hence, two different Baeyer-Villiger oxidation mechanisms based on the activation of H_2O_2 and cyclohexanone are proposed. Then, 6-hydroxyhexanoic acid is formed via the ring-opening of ε-caprolactone. However, C-OH groups cannot be reactivated by DHBEA zeolite, leading to insignificant adipic acid formation, while the selectivity of adipic acid is 28.5% obtained on the HTS zeolite. Consequently, the higher catalytic performance of the DHBEA zeolite is ascribed to its larger amount of active sites and greater diffusion features than those of HTS zeolite. | Xia Changjiu Zhao Yi Zhu Bin Lin Min Peng Xinxin Dai Zhenyu Shu Xingtian | 2018 | China Petroleum Processing & Petrochemical Technology2018，20，4： | 2 |
| 9 | Effects of Metal Oxide in ZSM-5 Zeolite on Its Catalytic Performance in FCC Process显示文摘Effects of metal oxide in ZSM-5 zeolite on its catalytic performance in fluid catalytic cracking reaction were studied via characterization by XRD and FT-IR spectroscopy using pyridine and collidine as molecular probes,and the modified ZSM-5 zeolite was evaluated in a micro reactor using standard light diesel fraction as the feedstock.Test results indicate that the metal species introduced into the ZSM-5 zeolite had led to the formation of Lewis acid centers.When the modified ZSM-5 zeolite with the metal species on its surface was used as the catalyst in FCC reaction,both the propylene yield and the propylene concentration in the liquefied petroleum gas increased,but in the meantime,more hydrogen and coke were formed at high conversion rate under the joint action of nonselective cracking of Lewis acid centers and dehydrogenation at metal centers on its outside surface. | Qin Jinlai Ouyang Ying Li Minggang Luo Yibin Shu Xingtian(SINOPEC Research Institute of Petroleum Processing,Beijing 100083) | 2011 | China Petroleum Processing & Petrochemical Technology2011，13，2： | 2 |
| 10 | Deactivation Behavior of Hollow Titanium Silicalite Zeolite in Aqueous Ammonia Solution under Simulated Industrial Cyclohexanone Ammoximation Conditions显示文摘For simulating the real deactivation of hollow titanium silicalite(HTS) zeolite in commercial ammoximation process, HTS was treated by 10% NH_3·H_2O solution at 120 ℃ in stirred autoclave. It is found that a part of HTS zeolite crystals dissolved in the hot NH_3·H_2O solution, and the specific surface area and pore volume continuously decreased with the increase in NH_3 hydrothermal treatment time. Meanwhile, the transformation of framework Ti species into extraframework Ti species was detected by the spectroscopic methods. However, the extraframework Ti species were still in a highly dispersed state after the hydrothermal and thermal treatments as shown by TEM images, while the formation of new acid sites was not detected. Upon combining the results of characterization with catalytic performance of HTS, the main deactivation reason for this material had been determined, which might be attributed to the reduction of specific surface area and active centers after basic treatment and calcination of HTS samples. And then the possible mechanism of simulated deactivation of HTS zeolite was proposed, which could describe the elemental reaction steps much more visually and directly. | Xia Changjiu Lin Min Peng Xinxin Zhu Bin Xu Guangtong Shu Xingtian | 2016 | China Petroleum Processing & Petrochemical Technology2016，18，4： | 2 |
| 11 | Synthesis of Nanosized SSZ-13 Zeolite and Performance of Its Mixed Matrix Membrane for CO2/CH4 Separation显示文摘Nanosized SSZ-13 zeolite was synthesized by traditional hydrothermal method using N,N,N-trimethyl-1-adamantanaminium hydroxide as the structure-directing agent (SDA). The influence of different preparative conditions of nanosized SSZ-13 was investigated systematically. The synthetic zeolites were characterized by X-ray powder diffraction (XRD), nitrogen physisorption, and scanning electron microscopy (SEM). By means of the self-assembled method, the thin SSZ-13/polyvinyl alcohol nanocomposite membranes were obtained by incorporating the nanosized SSZ-13 zeolite into the polymeric precursor (polyvinyl alcohol (PVA)). The permeation properties of pure CO2 and CH4 through the mixed matrix membranes (MMMs) were measured. The results showed that the highly crystalline SSZ-13 zeolite in a dispersed nanocrystal form with a controllable particle size of 100 nm could be hydrothermally synthesized by optimizing the synthetic parameters and the selectivity of CO2/CH4 of the MMMs could reach a value of 40 by changing the amount of nanosized SSZ-13 zeolite. | Liu Jianqiang Luo Yibin Li Minggang Shu Xingtian | 2019 | China Petroleum Processing & Petrochemical Technology2019，21，2： | 2 |
| 12 | Exploratory study on upgrading 1-butene using spent FCC catalyst/additive undcr simulated conditions of FCCU' s stripper显示文摘 | Lu Yong He Mingyuan Shu Xingtian | 2003 | Applied Catalysis A : General2003，255，： | 1 |
| 13 | Research on Bipolar Membrane Electrodialysis for Ion Exchange of Molecular Sieves显示文摘In view of the problems associated with large amount of discharged wastewater and serious pollution in the existing technology for removing sodium species from molecular sieves,this research work introduces the bipolar membrane electrodialysis into the process of removing sodium species from molecular sieves,and proposes a novel method of cleanly removing sodium from molecular sieves.The results show that the technology for removing sodium ions from the molecular sieves with an indirect electrodialysis process is feasible,and can recover Na OH solution.The bipolar membrane electrodialysis is especially suitable for treating the USY,ZSM-5 and Beta molecular sieves with high acid-resistance,and the physicochemical properties and catalytic performance of the prepared molecular sieves are roughly equivalent to those of the ammonium ion-exchange method.In comparison with the ammonium ion-exchange method,the process is clean and environmentally friendly,which consumes less water,and does not discharge wastewater to exhibit a rosy prospect of industrial application. | Chen Beiyan Liu Zhongqing Zhou Lina Luo Yibin Shu Xingtian | 2018 | China Petroleum Processing & Petrochemical Technology2018，20，2： | 1 |
| 14 | Rational construction of multiple hollow silicalite-1 zeolite with enhanced quasi acidity for robust vapor-phase Beckmann rearrangement显示文摘Developing efficient and stable zeolites for vapor-phase Beckmann rearrangement of cyclohexanone oxime is still a great challenge to realizeε-caprolactam(CPL)green production.In this work,the hierarchical porous silicalite-1 zeolites with multiple hollow structure(S-1-M)are explored by in-situ desilication−recrystallization post-treatment of spongy highway-like zeolites(S-1-S),which are synthesized through silanization synthesis of conventional bulky silicalite-1(S-1).Compared to S-1,S-1-M achieves superior catalytic performance,with improving the CPL selectivity from 85.7%to 94.1%and prolonging the catalyst lifetime from 74 to 126 h at a weight hourly space velocity(WHSV)of 6 h^(−1).Comprehensive physiochemical studies demonstrate that the highly dispersed intracrystalline cavities within S-1-M endow greater mass diffusion and better quasi acidity inducing by the enhanced H-bonds among abundant H-bonded silanols,which is cooperatively responsible for its superior catalytic performance. | Peng Zhang Xianfeng Yi Changjiu Xia Xinxin Peng Shuai Zhang Chengxiang Li Anmin Zheng Xiaoxin Zhang Yibin Luo Lifeng Cui Fuhong Yu Xingtian Shu | 2023 | Nano Research2023，16，5： | 1 |
| 15 | Insights into the Reaction Network and Mechanism of Green Aerobic Oxidative Esterification of Methacrolein over Different Heterogeneous Catalysts显示文摘The oxidative esterification of methacrolein(MAL)is an important way to prepare high-valued methyl methacrylate(MMA),but this process is ultra-complex due to the high reactivity of both C=O and C=C bonds in MAL molecule.In order to further improve MMA selectivity,the reaction network and relevant mechanisms have been proposed and profoundly investigated in this paper.Five kinds of fundamental reactions are involved in this process,including(a)the acetal reaction;(b)the aerobic oxidation of hemiacetal;(c)the alkoxylation of C=C double bond;(d)the Diels-Alder reaction;and(e)the hydrogenation reaction of unsaturated double bond.Among them,the Diels-Alder reaction of MAL is non-catalyzed,and the Brönsted acid sites or the Lewis acid sites favor promoting acetal reaction of MAL with methanol,while the alkoxylation of C=C bond with methanol is enhanced under alkaline condition.In particular,by employing the Pd-based catalysts,hydrogenation products are formed in alkaline methanol solution,hence with lower than those obtained by the Au-based catalysts.Notably,it is necessary to match the hemiacetal fromation and aerobic oxidation of hemiacetal,which is relevant with the amount and strength of acid and redox sites.Consequently,this work can provide a good guidance for the further design of both catalysts and processes in future. | Li Chenhao Xia Changjiu Liu Yujia Huang Kaimeng Peng Xinxin Liu Jinsheng Lin Min Zhu Bin Luo Yibin Shu Xingtian | 2021 | China Petroleum Processing & Petrochemical Technology2021，23，3： | 1 |
| 16 | Advances in Application of New Catalytic Materials in Petroleum Refining and Petrochemicals Production显示文摘This article introduces the solid acid catalyst for isobutene/butylenes alkylation, the HTS Ti/Si zeolite for ammonoxidation of cyclohexanone and the noncrystalline alloy catalyst and magnetically stabi- lized bed for hydrofining of caprolactam that were developed recently by SINOPEC Research Institute of Petroleum Processing (RIPP). | He Yigong Lin Min Mu Xuhong Shu Xingtian (SINOPEC Research Institute of Petroleum Processing, Beijing 100083) | 2006 | China Petroleum Processing & Petrochemical Technology2006，8，1： | 0 |
| 17 | Hydrothermal Chemistry Involved in Developing Practical Y Type Zeolite Catalysts显示文摘HydrothermalChemistryInvolvedinDevelopingPracticalYTypeZeoliteCatalystsHeMingyuan,ShuXingtian,MinEnze(ResearchInstituteofPetr... | He Mingyuan, Shu Xingtian, Min Enze (Research Institute of Petroleum Processing, Beijing 100083) | 1997 | 石油学报(石油加工)1997，13，S1： | 0 |
| 18 | Synthesis and Characterization of Hollow Titanium Silicalite Zeolite(HTS)显示文摘29Si-NMR 和 1H-NMR 被用来在 tetraethyl orthosilicate (脚趾) 的基本水解作用上面列在后面,结果显示出单体的那种,更暗淡,更整齐,周期并且聚合物硅酸盐被形成。单体并且更暗淡为沸石的高活动是有利的。XRD, 13C CP/MAS 和 29Si NMR 被用来跟踪空钛 silicalite 沸石(HTS ) 的结晶化过程。结果证明 HTS 的正式就职时期是 80 min,并且随后,形成 HTS 和清理毛孔或从 HTS 沸石洗离开杂质的结晶化时期力量功能的留下的时间拿了下 10 min。HTS 沸石的催化氧化表演与 crystallinity 的常规定义不按比例在反映催化氧化活动的沸石的酸活动的不同。综合 HTS 样品被 XRD 描绘,英尺红外,紫外力并且拉曼系列。Ti 被合并到沸石框架,这被证实。综合 HTS 样品为酚的氧化揭示了好重覆性和高活动进 diphenol。 | Lin Min Zhu Bin Shu Xingtian Wang Xieqing | 2008 | China Petroleum Processing & Petrochemical Technology2008，10，3： | 0 |
| 19 | MMC——High Propylene Selectivity DCC Catalyst显示文摘RIPP 开发了催化剂在增加丙烯收益瞄准了的第三根产生小说两重棉包线,作为 MMC 系列催化剂说出。这催化剂具有作为主要活跃部件由 ZSP 沸石组成的 MFIstructure,它为生产低碳的石蜡有更高的能力,特别地丙烯。在 SINOPEC Anqing 石油化学的同伴的这催化剂的商业应用程序表明了 MMC-2 催化剂的采纳导致了百分比以化工物品性质在基本上类似的条件下面在丙烯产量增加的 1.6-4.0 ,进程操作政体在在芳香的内容的汽油石蜡内容和增加结合了减小改进汽油质量。 | Li Zheng Xie Chaogang Luo Yibin Zhao Liuzhou Shu Xingtian | 2007 | China Petroleum Processing & Petrochemical Technology2007，9，1： | 0 |
| 20 | Pore plugging effects on the performance of ZSM-5 catalyst in MTP reaction using a discrete model显示文摘Coke is an important medium for connecting reaction and regeneration of the methanol to propylene process on the ZSM5 catalyst.Coke grows in the meso and macro pores,it gradually worsens the diffusion inside the catalyst particle.Furthermore,pore plugging is inevitable which causes the deactivation of ZSM5 catalyst.However,current continuum model cannot reflect the changes in pore structure with clear physical concepts.A discrete model that is verified by the carbon deposition experiments is introduced to indicate the behavior of pore plugging effects.Results show that the pore plugging has a significant effect on the performance of the catalyst.The time varying profile of effectiveness factor is obtained,indicating a regular reduction with the increase of the pore plugging effect.Spatial distributions of pore size that would significantly enhance the plugging effect are also identified. | Yudong Shen Hao Liang Zuwei Liao Binbo Jiang Jingdai Wang Yongrong Yang Minggang Li Yibin Luo Xingtian Shu | 2021 | Chinese Journal of Chemical Engineering2021，34，4： | 0 |
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