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Activity promotion of Rh_(1)Ca_(x)/Al_(2)O_(3) single-atom catalyst in 1-octene hydroformylation:a volcano curve exists between Ca adding ratio and catalytic activity

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Science China Chemistry 2024年第4期67卷 1187-1192页

作者： Hao Zhang Xingcong Zhang Xilun Wang Qingdi Sun Hao Liu Hongbing Ji Xiaohui He Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou 510275China Huizhou research institute Sun Yat-sen UniversityHuizhou 516081China State Key Laboratory Breeding Base of green-Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous *** conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and ***,a volcano curve between Ca addition ratio and catalytic activity is *** Ca significantly increases activity by decreasing the energy barrier,but excessive Ca decreases activity due to hindering substrate adsorption and reaction.

关键词： hydroformylation bimetallic single-atom catalysts rhodium heterogeneous catalyst

Tandem hydroformylation/hydrogenation of olefins to alcohols using atomically dispersed bifunctional catalysts

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Science China Chemistry 2024年第11期67卷 3706-3711页

作者： Ying Zhang Liyang Liu Ziyue Wang Xingcong Zhang Xiaohui He Hongbing Ji Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou 510275China State Key Laboratory Breeding Base of green-Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China Guangdong Technology research Center for Synthesis and Separation of Thermosensitive Chemicals Guangzhou 510275China

Tandem hydroformylation/hydrogenation of olefins to alcohols is an appealing and challenging route that has received continuous interest. Herein, we report a bifunctional atomically dispersed Rh and Co catalyst(Rh Co/Al_(2)O_(3)-10) prepared by a simple ball milling method that displays superior synergistic catalytic performance(>95% olefins conversion and >80% alcohols selectivity) and broad substrate scope for tandem hydroformylation/hydrogenation reaction, outperforming Rh/Al_(2)O_(3), Co/Al_(2)O_(3),and their physically mixed counterparts. In situ CO-DRIFTS, XPS, and kinetic experiments demonstrate that the electron interaction between Rh and Co atoms effectively lowers the apparent activation energy, thus promoting the tandem hydroformylation/hydrogenation reaction. This work not only presents a novel tandem hydroformylation/hydrogenation reaction system for converting olefins to alcohol but also throws light on the rational design of versatile bifunctional catalysts for ondemand synergistic catalysis.

关键词： tandem hydroformylation/hydrogenation alcohols bifunctional single atom catalysts

Preparation of Core-Shell Composite of Y@Mesoporous Alumina and Its Application in Heavy Oil Cracking

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China Petroleum Processing & petrochemical Technology 2016年第1期18卷 29-35页

作者： Yuan Chengyuan Wang Zhengwu Zhang Haitao Tan Zhengguo Pan Zhishuang Gao Xionghou Lanzhou petrochemical research Center Petrochemical Research Institute PetroChina Lanzhou 730060 PetroChina Dushanzi petrochemical Company Karamay 838600

A well core-shell composite of Y@meso-Al with a mesoporous alumina shell and a Y zeolite core was synthesized. The mesoporous alumina shell has a wormhole-like structure with large mesopores. The prepared catalytic cracking catalyst using this composite has exhibited excellent catalytic performance for heavy oil cracking thanks to its favorable physicochemical properties, such as high surface area, large pore volume and outstanding acid sites accessibility for large molecules provided by the composite. In comparison with the reference catalyst using pure Y zeolite, the oil conversion achieved by the above-mentioned catalyst increased by 2.73 percentage points, while the heavy oil yield and coke yield decreased by 2.23 percentage points and 1.28 percentage points, respectively, with the light oil yield increasing by 2.27 percentage points.

关键词： zeolite mesoporous alumina core-shell accessibility catalytic cracking

Understanding Zeolites Catalyzed Methanol-to-Olefins Conversion from Theoretical Calculations

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Chinese Journal of Chemistry 2018年第5期36卷 381-386页

作者： Chuanming Wang Yangdong Wang Zaiku Xie State Key Laboratory of green Chemical Engineering and Industrial Catalysis SINOPEC Shanghai Research Institute of Petrochemical TechnologyShanghai 20120B Ch{na

Zeolites catalyzed methanol-to-olefins （MTO） conversion provides an alternative process to produce light olefins such as ethene and propene from nonpetroleum resources. Despite of successful industrialization of the MTO process, its detailed reaction mechanism is not yet well understood. Here we summarize our work on the hydrocarbon pool reaction mechanism based on theoretical calculations. We proposed that the olefins themselves are likely to be the dominating hydrocarbon pool species, and the distribution of cracking precursors and diffusion constraints affect the selectivity. The similarities between aromatic-based and olefin-based cycles are highlighted.

关键词： zeolite catalysis methanol-to-olefins conversion hydrocarbon pool mechanism computational catalysis density functional theory

Hyperbranched polymer hollow-fiber-composite membranes for pervaporation separation of aromatic/aliphatic hydrocarbon mixtures

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Chinese Journal of Chemical Engineering 2024年第5期69卷 13-22页

作者： Tong Liu Hao Sun Xiangqiong Wang Jie Li Zhanquan Zhang Pei Wu Naixin Wang Quanfu An Beijing Key Laboratory for green Catalysis and Separation Department of Chemical EngineeringCollege of Materials Science and EngineeringBeijing University of TechnologyBeijing 100124China petrochemical research institute CNPCBeijing 102206China

The separation of aromatic/aliphatic hydrocarbon mixtures is crucial in the petrochemical *** is regarded as a promising approach for the separation of aromatic compounds from alkanes. Developing membrane materials with efficient separation performance is still the main task since the membrane should provide chemical stability, high permeation flux, and selectivity. In this study, the hyperbranched polymer(HBP) was deposited on the outer surface of a polyvinylidene fluoride(PVDF)hollow-fiber ultrafiltration membrane by a facile dip-coating method. The dip-coating rate, HBP concentration, and thermal cross-linking temperature were regulated to optimize the membrane *** obtained HBP/PVDF hollow-fiber-composite membrane had a good separation performance for aromatic/aliphatic hydrocarbon mixtures. For the 50%/50%(mass) toluene/n-heptane mixture, the permeation flux of optimized composite membranes could reach 1766 g·m^(-2)·h^(-1), with a separation factor of 4.1 at 60℃. Therefore, the HBP/PVDF hollow-fiber-composite membrane has great application prospects in the pervaporation separation of aromatic/aliphatic hydrocarbon mixtures.

关键词： Aromatic/aliphatic hydrocarbons Hyperbranched polymer Pervaporation Hollow fiber membrane Dip-coating

Systematic engineering of BiVO_(4)photoanode for efficient photoelectrochemical water oxidation

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Carbon Energy 2024年第4期6卷 12-21页

作者： Zhiting Liang Meng Li Kai‐Hang Ye Tongxin Tang Zhan Lin Yuying Zheng Yongchao Huang Hongbing Ji Shanqing Zhang Guangzhou Key Laboratory of Clean Transportation Energy Chemistry School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhouChina Chemical Engineering Guangdong Laboratory Jieyang Branch of ChemistryJieyangChina Key Laboratory for Water Quality and Conservation of the Pearl River Delta Institute of Environmental Research at Greater Bay AreaMinistry of EducationGuangzhou UniversityGuangzhouChina State Key Laboratory Breeding Base of green‐Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhouChina School of Environment and Science Centre for Catalysis and Clean EnergyGriffith UniversityGold Coast CampusSouthportQueenslandAustralia

BiVO_(4)is one of the most promising photoanode materials for photoelectrochemical(PEC)solar energy conversion,but it still suffers from poor photocurrent density due to insufficient light‐harvesting efficiency(LHE),weak photogenerated charge separation efficiency(Φ_(Sep)),and low water oxidation efficiency(Φ_(OX)).Herein,we tackle these challenges of the BiVO_(4)photoanodes using systematic engineering,including catalysis engineering,bandgap engineering,and morphology *** particular,we deposit a NiCoO_(x)layer onto the BiVO_(4)photoanode as the oxygen evolution catalyst to enhance theΦ_(OX)of Fe‐g‐C_(3)N_(4)/BiVO_(4)for PEC water oxidation,and incorporate Fe‐doped graphite‐phase C_(3)N_(4)(Fe‐g‐C_(3)N_(4))into the BiVO_(4)photoanode to optimize the bandgap and surface areas to subsequently expand the light absorption range of the photoanode from 530 to 690 nm,increase the LHE andΦ_(Sep),and further improve the oxygen evolution reaction activity of the NiCoO_(x)catalytic ***,the maximum photocurrent density of the as‐prepared NiCoO_(x)/Fe‐g‐C_(3)N_(4)/BiVO_(4)is remarkably boosted from 4.6 to 7.4 mA cm^(−2).This work suggests that the proposed systematic engineering strategy is exceptionally promising for improving LHE,Φ_(Sep),andΦ_(OX)of BiVO_(4)‐based photoanodes,which will substantially benefit the design,preparation,and large‐scale application of next‐generation high‐performance photoanodes.

关键词： bismuth vanadate carbon nitride charge separation heterojunction water oxidation

Synthesis of newly cationic surfactant based on dimethylaminopropyl amine and their silver nanoparticles:Characterization;surface activity and biological activity

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Chinese Chemical Letters 2017年第2期28卷 264-273页

作者： Samy M.Shaban Ismail Aiad Mohamed M.El-Sukkary E.A.Soliman Moshira Y.El-Awady petrochemical Department Egyptian Petroleum Research Institute Faculty of Science Ain Shams University

The chemical structure of newly synthesized cationic surfactants based on Schiff base was confirmed using Fourier transform infrared spectroscopy,proton nuclear magnetic resonance spectroscopy,and mass *** synthesized surfactants were used in the synthesis of silver nanoparticles by a simple one-step *** silver nanoparticle（AgNPs） formation was confirmed using transmission electron microscopy（TEM）,electron diffraction（SAED）,dynamic light scattering（DLS）,and energy dispersive X-ray spectroscopy（EDX）.The structure of the surfactant played an important role in the synthesis *** the hydrophobic chain length,the stability,and the amount of surfactant increased the quantity of AgNPs *** surface activity of the synthesized cationic surfactants was determined using surface tension measurements at three different *** synthesized surfactants showed a high tendency toward adsorption and *** the hydrophobic chain length of the synthesized surfactant increased its *** the synthesized cationic surfactants and their nano-form against bacteria and fungi showed that they are highly *** silver nanoparticles enhanced the biological activity of the synthesized cationic surfactants.

关键词： Cationic surfactant Silver nanoparticles Dynamic light scattering Biological activity Surface parameters Thermodynamic parameters

Preparation of capped silver nanoparticles using sunlight and cationic surfactants and their biological activity

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Chinese Chemical Letters 2015年第11期26卷 1415-1420页

作者： Samy M.Shaban Ismail Aiad Mohamed M.El-Sukkary E.A.Soliman Moshira Y.El-Awady petrochemical Department Egyptian Petroleum Research Institute Faculty of Science Ain Shams University

Silver nanoparticles were prepared in situ using sunlight and cationic surfactants. Silver nano-particles were confirmed using UV-vis spectropbotometry, transmission electron microscopy （TEM）, electron diffraction, dynamic light scattering （DLS） and FTIR. Increasing the hydrophohic chain length of surfactants increase the amount of silver nano-particles formed in addition to increasing their stability. The results showed formed, uniform, well arranged hexagonal and spherical shapes. The prepared silver nanoparticles exhibit enhanced biological activity against Cram-positive, Gram-negative bacteria and sulfate reducing bacteria （SRB）.

关键词： Silver nano-particlesPhotosynthesisSpherical shapesZeta potentialBiological activitySRB

Application of New Heavy Metals Resistant Porous Binder Material Used in Fluid Catalytic Cracking Reaction

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China Petroleum Processing & petrochemical Technology 2014年第1期16卷 35-39页

作者： Zhang Zhongdong Liu Zhaoyong Yan Zifeng Gao Xionghou Zhang Haitao Wang Zhifeng State Key Laboratory of Heavy Oil Processing China University of Petroleum Lanzhou petrochemical research Center petrochemical research institute PetroChina

A novel porous binder was obtained from acid-treated kaolin. This new binder possessed abundant meso/macropores, good hydrothermal stability and heavy metal resistance. The prepared catalyst using new binder featured low attrition index and large pore volume. The catalysts were contaminated with Ni, V, and tested in a fixed-fluidized bed reactor unit. In comparison with the reference sample, the oil conversion achieved by the above-mentioned catalyst increased by 3.50 percentage points, and heavy oil yield decreased by 2.86 percentage points, while the total liquid yield and light oil yield increased by 2.82 percentage points and 0.79 percentage points, respectively. The perfect pore structure, good hydrothermal stability and heavy metal resistant performance of new binder were the possible causes leading to its outstanding performance.

关键词： fluid catalytic cracking binder conversion porous material hydrothermal stability heavy metal resistant