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学者姓名:陈晓晖
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Abstract :
Au and Zr are uniformly loaded on the surface of TS-1 by coprecipitation method to obtain atomically dispersed Au-Zr binary clusters. The interaction between Au clusters, Zr and TS-1 is analyzed by Independent Gradient Model based on Hirshfeld partition (IGMH), adsorption energy of Au cluster, Mayer bond order. It is found that the existence of Zr is conducive to the stability of nano Au on TS-1 surface. The catalyst is applied to the gas phase epoxidation of C3H6 to obtain 14.06 % initial conversion, 93.93 % initial selectivity and 479.52 gPO center dot kg(cat)(-1)center dot h(-1) initial productivity. It shows good stability in the continuous test for more than 50 h. Density functional theory (DFT) is used to calculate the possible catalytic reaction mechanism on the surface of atomically dispersed Au clusters. The whole process from C3H6 epoxidation reaction to catalyst regeneration is completely described. In the analysis of H2O desorption, the concept of "relay desorption" is proposed. Combined with charge and surface electrostatic potential analysis, the different attack directions of C3H6 on the catalyst surface are dis-cussed in detail. This will provide guidance and help for the synthesis and catalytic application of nano Au catalysts.
Keyword :
Coprecipitation method Coprecipitation method DFT DFT Interaction of Au Zr and TS-1 Interaction of Au Zr and TS-1 Propylene epoxidation Propylene epoxidation Sub-nano Au-Zr clusters Sub-nano Au-Zr clusters
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GB/T 7714 | Peng, Jiahui , Li, Bin , Chen, Wenkai et al. Atomically dispersed nano Au clusters stabilized by Zr on the TS-1 surface: Significant enhancement of catalytic oxidation ability using H-2 and O-2 [J]. | APPLIED SURFACE SCIENCE , 2023 , 619 . |
MLA | Peng, Jiahui et al. "Atomically dispersed nano Au clusters stabilized by Zr on the TS-1 surface: Significant enhancement of catalytic oxidation ability using H-2 and O-2" . | APPLIED SURFACE SCIENCE 619 (2023) . |
APA | Peng, Jiahui , Li, Bin , Chen, Wenkai , Hu, Hui , Huang, Qingming , Chen, Xiaohui . Atomically dispersed nano Au clusters stabilized by Zr on the TS-1 surface: Significant enhancement of catalytic oxidation ability using H-2 and O-2 . | APPLIED SURFACE SCIENCE , 2023 , 619 . |
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CuZnZrAl catalysts were synthesized by the co-precipitation and coprecipitation-ammonia methods and modified with Y and Ce promoters for the methanol steam reforming hydrogen production process. The physicochemical properties of the catalysts were analyzed by XRD, BET, H2-TPR, and XPS methods. The methanol conversion, as well as CO selectivity of MSR at different temperatures, were investigated, and its stability was probed using repeated start and stop test to simulate the onboard hydrogen production process. The results showed that the methanol conversion of CuZnZrAl catalyst prepared by coprecipitation-ammonia method was 96.9% at a tem-perature of 270 degrees C, S/C molar ratio of 1.2, and WHSV of 2.6 h-1, which was higher than that of 94.6% by the co-precipitation method. In addition, the best catalytic performance was obtained for the catalyst with Ce promoter addition using coprecipitation-ammonia method. The conversion was 100% at 270 degrees C with a CO selectivity of only 0.31%, and the conversion remained 98.7% after 20 reactions were repeated.
Keyword :
Coprecipitation-ammonia method Coprecipitation-ammonia method CuZnZrAl catalysts CuZnZrAl catalysts Hydrogen Hydrogen Methanol steam reforming Methanol steam reforming
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GB/T 7714 | Li, Linfeng , Chen, Jiayuan , Zeng, Cuibing et al. Preparation of CuZnZrAl catalysts by coprecipitation-ammonia method for methanol steam reforming and the effect of promoters Y and Ce [J]. | MOLECULAR CATALYSIS , 2023 , 537 . |
MLA | Li, Linfeng et al. "Preparation of CuZnZrAl catalysts by coprecipitation-ammonia method for methanol steam reforming and the effect of promoters Y and Ce" . | MOLECULAR CATALYSIS 537 (2023) . |
APA | Li, Linfeng , Chen, Jiayuan , Zeng, Cuibing , Liu, Quan , Hu, Hui , Huang, Qingming et al. Preparation of CuZnZrAl catalysts by coprecipitation-ammonia method for methanol steam reforming and the effect of promoters Y and Ce . | MOLECULAR CATALYSIS , 2023 , 537 . |
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The epoxidation of propylene (C3H6) over TS-1 molecular sieve supported with nano-Au clusters by deposition-precipitation (DP) method has always been the focus of the catalytic field. A quantity of atomically dispersed Au clusters can be synthesized induced by NH3 as an assistant in the DP system. These smaller Au clusters show 14.3% C3H6 conversion, 91.7% propylene oxide (PO) selectivity, 10.6% H-2 efficiency and 477.4 gPO center dot kg(cat)(-1)center dot h(-1) PO productivity in the epoxidation reaction of C3H6. The interaction between NH3 and [AuCl4](-) in aqueous solution is analyzed by means of experiments and Density Functional Theory (DFT), and it is concluded that at least 2 times of NH3 is needed to make Au precipitate completely. Similarly, the mechanism of C3H6 epoxidation catalyzed by Aun (n = 2, 3, 4) clusters in coordination with Ti sites is calculated with the help of DFT. It is believed that the in-situ formation of Ti-OOH structure at Ti sites through H-2 and O-2 is the key to initiate C3H6 epoxidation. The general rules of catalytic mechanism under different size of Au clusters are also analyzed.
Keyword :
Atomically dispersed Au clusters Atomically dispersed Au clusters Deposition-precipitation method Deposition-precipitation method DFT DFT NH3 induction NH3 induction Propylene epoxidation Propylene epoxidation
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GB/T 7714 | Peng, Jiahui , Liu, Kexing , Guo, Shujuan et al. Synthesis strategy of atomically dispersed Au clusters induced by NH3 on TS-1: Significantly improve the epoxidation activity of propylene [J]. | CHEMICAL ENGINEERING JOURNAL , 2023 , 472 . |
MLA | Peng, Jiahui et al. "Synthesis strategy of atomically dispersed Au clusters induced by NH3 on TS-1: Significantly improve the epoxidation activity of propylene" . | CHEMICAL ENGINEERING JOURNAL 472 (2023) . |
APA | Peng, Jiahui , Liu, Kexing , Guo, Shujuan , Chen, Wenkai , Hu, Hui , Huang, Qingming et al. Synthesis strategy of atomically dispersed Au clusters induced by NH3 on TS-1: Significantly improve the epoxidation activity of propylene . | CHEMICAL ENGINEERING JOURNAL , 2023 , 472 . |
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The pure silicon MWW were synthesized for the first time by means of a dry-gel conversion method utilizing N, N, N-trimethyl-1-adamantyl ammonium hydroxide and hexamethyleneimine as the structural directing agents. A vapor transport assisted crystallization method for obtaining complete crystallinity was developed to replace the traditional dry-gel conversion methods. TiCl4 acid solution treatment was cleverly used for the implantation of titanium in MWW. Compared with Ti-ERB-1, the Ti content of boron-free Ti-MWW is only 20% of the former, the conversion rate of 1-hexene epoxidation is 2.3 times of the former and nearly 100% of H2O2 efficiency.
Keyword :
1-Hexene epoxidation 1-Hexene epoxidation Atom-planting Atom-planting Boron-free Ti-MWW Boron-free Ti-MWW TOF TOF
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GB/T 7714 | Ge, Zhijin , Li, Xin'ao , Hu, Hui et al. Synthesis of boron- free titanosilicate zeolite by TiCl4/HCl treatment of pure silicon MWW as an epoxidation catalyst [J]. | JOURNAL OF CATALYSIS , 2023 , 428 . |
MLA | Ge, Zhijin et al. "Synthesis of boron- free titanosilicate zeolite by TiCl4/HCl treatment of pure silicon MWW as an epoxidation catalyst" . | JOURNAL OF CATALYSIS 428 (2023) . |
APA | Ge, Zhijin , Li, Xin'ao , Hu, Hui , Huang, Qingming , Chen, Xiaohui . Synthesis of boron- free titanosilicate zeolite by TiCl4/HCl treatment of pure silicon MWW as an epoxidation catalyst . | JOURNAL OF CATALYSIS , 2023 , 428 . |
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The efficient and economic heteroatom-implanting method for MWW-type zeolite has been the focus of attention and needs further exploration. Ti incorporated MWW zeolite was synthesized by sequential treatment of boron-containing zeolite precursor. The catalysts were applied to the epoxidation of 1-hexene. The implanting titanium process was conducted under a mild condition with Ti(SO4)(2)/NH4HF2/HNO3 solution, and the product Ti-MWW precursors have framework titanium alone, the novel method is named as refluxing and implanting titanium method which integrates acid treatment and titanium incorporation into one step and reduces the consumption of time of this process into 1 h. A density functional theory was conducted to explain the formation mechanism of interlayer-expanded structure of Ti-MWW zeolite. Subsequently, Ti-MWW precursors were treated in modified reagent solution to obtain larger pore structure, which increase the conversion of 1-hexene from 20.45 to 62.96%. The catalytic performance of Ti-MWW zeolite in this work are superior to Ti-MWW zeolite synthesized by traditional dry-gel conversion method the conversion of 1-hexene of which was 4.2%. This novel method is a promising approach for the synthesis of high catalytic performance heteroatomic zeolite. [GRAPHICS] .
Keyword :
1-hexene 1-hexene Implanting titanium method Implanting titanium method Interlayer modification Interlayer modification Ti-MWW Ti-MWW
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GB/T 7714 | Chu, Jidong , Ge, Zhijin , Peng, Jiahui et al. Synthesis of Ti-MWW Zeolite by Refluxing and Implanting Titanium Method and Further Application in 1-Hexene Epoxidation [J]. | CATALYSIS LETTERS , 2022 , 153 (2) : 348-363 . |
MLA | Chu, Jidong et al. "Synthesis of Ti-MWW Zeolite by Refluxing and Implanting Titanium Method and Further Application in 1-Hexene Epoxidation" . | CATALYSIS LETTERS 153 . 2 (2022) : 348-363 . |
APA | Chu, Jidong , Ge, Zhijin , Peng, Jiahui , Hu, Hui , Guo, Shujuan , Chen, Xiaohui . Synthesis of Ti-MWW Zeolite by Refluxing and Implanting Titanium Method and Further Application in 1-Hexene Epoxidation . | CATALYSIS LETTERS , 2022 , 153 (2) , 348-363 . |
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Nanosized hierarchical pure Si-Beta zeolite was prepared by the solvent-free method. With the assistance of 1% seeds and low organic template content (TEAOH/SiO2 = 0.06), pure Si-Beta zeolite is well crystallized within 16 h, neither fluoride mineralizing agent nor mesoporogen agent. Here we comprehensively investigated the physicochemical properties of the resulting samples, including X-ray diffraction, scanning electron microscopy, nitrogen adsorption-desorption, water adsorption, Fourier transform infrared and thermogravimetric analyses (TGA). These characterization results suggest that the silicon sources would influence the crystal size, but all samples possessed high surface area (509-647 m(2) g(-1)), pore volume (0.40-0.71 cm(3) g(-1)), and superior hydrophobicity.
Keyword :
Hierarchically Hierarchically Pure Si-Beta zeolite Pure Si-Beta zeolite Silicon source Silicon source Solvent-free Solvent-free
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GB/T 7714 | Lei, Wu , Li, Linfeng , Chen, Xiaohui . Fast synthesis of hierarchical nanosized pure Si-Beta zeolite with low organic template content via the solvent-free method [J]. | JOURNAL OF SOLID STATE CHEMISTRY , 2022 , 308 . |
MLA | Lei, Wu et al. "Fast synthesis of hierarchical nanosized pure Si-Beta zeolite with low organic template content via the solvent-free method" . | JOURNAL OF SOLID STATE CHEMISTRY 308 (2022) . |
APA | Lei, Wu , Li, Linfeng , Chen, Xiaohui . Fast synthesis of hierarchical nanosized pure Si-Beta zeolite with low organic template content via the solvent-free method . | JOURNAL OF SOLID STATE CHEMISTRY , 2022 , 308 . |
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Density Functional Theory is used to calculate the epoxidation of propylene on the dimer MoOx by Gaussian 09 software. We calculate the dehydrogenation process of propylene and the formation process of propylene oxide. It is found that the activity of O in Mo-O-Si, which is beneficial to the dehydrogenation process of propylene, is high. Furthermore, we establish a dimer MoOx model with defect sites, and find that the defect sites in the dimer MoOx can activate O-2 (O-2(2-)) effectively. Consequently, the catalyst containing defect sites is conducive to the selectivity of propylene oxide.
Keyword :
Defect Defect DFT DFT Dimer MoOx Dimer MoOx Propylene epoxidation Propylene epoxidation
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GB/T 7714 | Peng, Jiahui , Wan, Zhehong , Chen, Wei et al. Theoretical comparative study on the mechanism of gas phase epoxidation of propylene about complete and defective dimer MoOx [J]. | COMPUTATIONAL AND THEORETICAL CHEMISTRY , 2022 , 1210 . |
MLA | Peng, Jiahui et al. "Theoretical comparative study on the mechanism of gas phase epoxidation of propylene about complete and defective dimer MoOx" . | COMPUTATIONAL AND THEORETICAL CHEMISTRY 1210 (2022) . |
APA | Peng, Jiahui , Wan, Zhehong , Chen, Wei , Hu, Hui , Huang, Qingming , Chen, Xiaohui . Theoretical comparative study on the mechanism of gas phase epoxidation of propylene about complete and defective dimer MoOx . | COMPUTATIONAL AND THEORETICAL CHEMISTRY , 2022 , 1210 . |
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Au particles supported on TS-1 are prepared by deposition precipitation method with ammonium salt solution as Promoter. FT-IR and Si-29 NMR indicate that the modifications do not destroy the MFI structure of TS-1 and retain the tetra-coordination skeleton titanium. DFT and UV-Vis analysis show that under the transition from [AuCl4](-) to [AuCl4-x(NH3)(x)](x-1) (x = 0-2) in the preparation process, NH3 enhance the attraction of gold precursors and supports (the gold capture effectivity is 94.5%), and C2O42- reduces the gold complex into AuNPs (1.14 nm).
Keyword :
Ammonium salt Ammonium salt Epoxidation Epoxidation Gold Gold Propylene oxide Propylene oxide TS-1 TS-1
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GB/T 7714 | Dong, Tao , Huang, Qian , Chen, Lu et al. Propylene epoxidation over Au/TS-1 modified by ammonium salt: Enhancement of the attractiveness of gold precursors and supports [J]. | CHEMICAL PHYSICS LETTERS , 2022 , 804 . |
MLA | Dong, Tao et al. "Propylene epoxidation over Au/TS-1 modified by ammonium salt: Enhancement of the attractiveness of gold precursors and supports" . | CHEMICAL PHYSICS LETTERS 804 (2022) . |
APA | Dong, Tao , Huang, Qian , Chen, Lu , Peng, Jiahui , Hu, Hui , Huang, Qingming et al. Propylene epoxidation over Au/TS-1 modified by ammonium salt: Enhancement of the attractiveness of gold precursors and supports . | CHEMICAL PHYSICS LETTERS , 2022 , 804 . |
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本发明提供了一种具有高转化率的丙烯气相环氧化催化剂的制备方法。本发明采用沉积沉淀法,并在制备过程中通过生物质活性剂和铵盐对Au/TS‑1进行改性,催化剂中金和氮的摩尔比为0.001~0.1,TS‑1的硅钛比摩尔比为50~100。在制备过程温度控制在25~100℃的条件下,改性制备过程中能更好地锚定金原子,提高了金的捕获率进而增加了有效金位点的数量,使得环氧丙烷的产速提高了15倍。该催化剂制备方法简单,稳定高效,是一种有前景的催化剂。
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GB/T 7714 | 陈晓晖 , 陈璐 , 黄清明 et al. 一种具有高转化率的丙烯气相环氧化催化剂的制备方法 : CN202110788401.8[P]. | 2021-07-13 . |
MLA | 陈晓晖 et al. "一种具有高转化率的丙烯气相环氧化催化剂的制备方法" : CN202110788401.8. | 2021-07-13 . |
APA | 陈晓晖 , 陈璐 , 黄清明 , 胡晖 . 一种具有高转化率的丙烯气相环氧化催化剂的制备方法 : CN202110788401.8. | 2021-07-13 . |
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With the extensive use of internal combustion engines, the large volume of lubricant consumption has become an urgent problem. In this study, a new adsorbent of modified sawdust (MS) was used to clean the waste diesel engine lubricant and prepared into a pure biomass oil filter (PBF) for the actual operation of buses. The characterization results of sawdust showed that the crystallinity index of MS enhanced 19.26%, and MS had smoother morphology, obvious pores than raw sawdust (RS). In on-road tests, both total acid number (1 mg KOH center dot g(-1)) and total base number (9 mg KOH center dot g(-1)) were within the permitted range of the standard, and the kinematic viscosity showed a decreasing trend. In addition, the concentration of metals and insoluble colloids (<0.2%) in the lubricant was far below the oil change limit, which made the oil drain interval of the two vehicles extended from 15 000 km (recommended by manufacture) to 60 500 and 71 500 km, respectively. Conclusively, it is believed that PBF is efficient to alleviate lubricant deterioration and prolong the oil drain interval.
Keyword :
adsorption adsorption lubricant property lubricant property modified sawdust modified sawdust oil drain interval oil drain interval pure biomass oil filter pure biomass oil filter
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GB/T 7714 | Chen, Xiaohui , Chen, Lu , Gan, Xianqian et al. Extension of lubricant drain interval by modified pure biomass oil filter [J]. | ASIA-PACIFIC JOURNAL OF CHEMICAL ENGINEERING , 2021 , 16 (4) . |
MLA | Chen, Xiaohui et al. "Extension of lubricant drain interval by modified pure biomass oil filter" . | ASIA-PACIFIC JOURNAL OF CHEMICAL ENGINEERING 16 . 4 (2021) . |
APA | Chen, Xiaohui , Chen, Lu , Gan, Xianqian , Pan, Shouquan , Pan, Hongkun . Extension of lubricant drain interval by modified pure biomass oil filter . | ASIA-PACIFIC JOURNAL OF CHEMICAL ENGINEERING , 2021 , 16 (4) . |
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