FUEL
·
2021
·
IF 6.609
Tao Pan,Sida Ge,Mengnan Yu,Yana Ju,Ran Zhang,Pei Wu,Kuanyu Zhou,Zhijie Wu
Zn modified ZSM-5 zeolite supported Ni bifunctional catalysts were prepared by in-situ hydrothermal synthesis (Zn-Ni-ZSM-5), co-impregnation method (Zn-Ni/ZSM-5) as well as combining in-situ hydrothermal synthesis of Zn-ZSM-5 and sequential impregnation of Ni (Ni/Zn-ZSM-5) and used for the selective converting olefin to aromatics applicable for FCC gasoline hydro-upgrading. The Lewis (L) acid sites generated by ZnOH + species and hydrogenation active sites from Ni 0 species were varied with preparation method, in which their locations at the external surface or micropores of zeolite changed the acid properties of catalysts. Comparing to the Zn-Ni/ZSM-5 from the co-impregnation method, direct in-situ hydrothermal method could incorporate Zn and Ni species within zeolite, which makes the strong interaction between the metal species and the framework Al to form medium-strong L acids (ZnOH + /NiOH + ). This leads to the decrease of ratio of Brønsted acid sites to L acid sites (B/L) from 0.40 to 0.12 and the difficulty in reducing of Ni cations to Ni 0 from 57% to 30% Ni 0 percent. Ni/Zn-ZSM-5 sample prepared by incorporating Zn species into micropores and sequential depositing Ni species at the external surface of zeolite possesses a low B/L ratio similar to Zn-Ni-ZSM-5 (0.20 versus 0.12) but a much higher Ni 0 percent (52% versus 30%). Zn-Ni-ZSM-5 shows closer intimacy between Zn and Ni species comparing to Zn-Ni/ZSM-5 and Ni/Zn-ZSM-5. For the 1-hexene aromatization, the formed iso -alkene at acid sites was quickly saturated to iso -alkanes by the adjacent Ni 0 particles over Ni-Zn-ZSM-5 catalyst in hydrogen steam. However, the location of aromatization active sites (ZnOH + , L acid sites) in micropores and hydrogenation active sites (Ni 0 species) on external surface of Ni/Zn-ZSM-5 makes the tandem conversion of n-alkene → iso -alkene → aromatics, rather than the n-alkene → iso -alkene → iso -alkane. Thus, Zn-Ni-ZSM-5 with close intimacy of ZnOH + and Ni 0 particles shows a high iso -alkane selectivity (27.9% iC 4 + ), while Ni/Zn-ZSM-5 exhibits a high aromatics selectivity (39.6 %) in the conversion of 1-hexene in hydrogen steam. Similar results have also found in the conversion of n-heptane. Here, the control of the intimacy of Zn and Ni in ZSM-5 zeolites has been realized to be a good protocol to adjust the selective conversion of olefins/alkanes to aromatics versus iso -alkanes.
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2023
·
IF 13.3
Aiguo Han,Shijie Xu,Xinyu Wang,Haolong Chang,Rongzheng Tian,Xin Zhang,Xing Chen,Dawei Song,Yongan Yang
Sulfide solid electrolytes (SSEs) are highly wanted for solid-state batteries (SSBs). While their liquid-phase synthesis is advantageous over their solid-phase strategy in scalable production, it confronts other challenges, such as low-purity products, user-unfriendly solvents, energy-inefficient solvent removal, and unsatisfactory performance. This article demonstrates that a suspension-based solvothermal method using single oxygen-free solvents can solve those problems. Experimental observations and theoretical calculations together show that the basic function of suspension-treatment is “interparticle-coupled unification”, that is, even individually insoluble solid precursors can mutually adsorb and amalgamate to generate uniform composites in nonpolar solvents. This anti-intuitive concept is established when investigating the origins of impurities in SSEs electrolytes made by the conventional tetrahydrofuran-ethanol method and then searching for new solvents. Its generality is supported by four eligible alkane solvents and four types of SSEs. The electrochemical assessments on the former three SSEs show that they are competitive with their counterparts in the literature. Moreover, the synthesized SSEs presents excellent battery performance, showing great potential for practical applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Shuaishuai Ding,Qing Yan,Hong Jiang,Zhaoxiang Zhong,Rizhi Chen,Weihong Xing
By adjusting the addition time of palladium nanoparticles, during the formation of ZIF-8, an efficient and facile method was proposed to control the palladium spatial distribution within ZIF-8 crystals. Characterizations reveal that the addition time can significantly affect the particle size of Pd@ZIF-8 and palladium spatial distribution. As the PVP-stabilized palladium nanoparticles are added at the early stage of the ZIF-8 formation, larger ZIF-8 crystals with completely embedded palladium nanoparticles can be obtained. Introducing the PVP-stabilized palladium nanoparticles later can lead to the formation of smaller ZIF-8 crystals with all the palladium nanoparticles on the outer surfaces of ZIF-8. The catalytic performance of Pd@ZIF-8 strongly depends on the palladium spatial distribution, and the Pd@ZIF-8 with completely embedded palladium nanoparticles can provide excellent product selectivity and better catalytic stability in the hydrogenation of alkenes.
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Chenhao Wei,Di Gao,Guohao Zhang,Liang Zhao,Jinsen Gao,Chunming Xu
1-Hexene aromatization is a promising technology to convert excess olefin in FCC gasoline to high-value benzene (B), toluene (T), and xylene (X). Besides, the increasing market demand of xylene has put forward higher requirements for new generation of catalyst. For increasing xylene yield in 1-hexene aromatization, the effect of mesopore structure and spatial distribution on product distribution and Zn loading was studied. Catalysts with different mesopore spatial distribution were prepared by post-treatment of parent HZSM-5, including NaOH treatment, Tetra-propylammonium hydroxide (TPAOH) treatment, and recrystallization. It was found the evenly distributed mesopore mainly prolongs the catalyst lifetime by enhancing diffusion properties but reduces the aromatics selectivity, as a result of damage of micropores close to the catalyst surface. While the selectivity of high-value xylene can be highly promoted when the mesopore is mainly distributed interior the catalyst. Besides, the state of loaded Zn was also affected by mesopores spatial distribution. On the optimized catalyst, the xylene selectivity was enhanced by 12.4% compared with conventional Zn-loaded parent HZSM-5 catalyst at conversion over 99%. It was attributed to the synergy effect of mesopores spatial distribution and optimized acid properties. This work reveals the role of mesopores in different spatial positions of 1-hexene aromatization catalysts in the reaction process and the influence on metal distribution, as well as their synergistic effect two on the improvement of xylene selectivity, which can improve our understanding of catalyst pore structure and be helpful for the rational design of high-efficient catalyst.
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2023
·Vol. 8
·期 45
·e202303191
·
IF 2.1
Yumei Liu,Deshuai Yang,Guixiang Zeng,Kexin Li,Shuang Wei,Hao Li,Min Ji,Ruixia Liu
Graphical We developed a highly active and selective Ru/DES catalytic system for the alkoxycarbonylation of alkenes under mild conditions without strong acid additives. Conversion of 1-hexene reached 99.0 % at 1 MPa CO with 99.1 % ester selectivity. Notably, Ru/DES outperformed Ru 3 (CO) 12 . The excellent performance originated from [Ru(CO) 2 Br 3 ] − produced through Ru 3 (CO) 12 dissolution and coordination with DES. The catalytic alkoxycarbonylation of alkenes is an attractive, atom-efficient method for producing value-added carboxylic esters. However, the conventional catalyst system for this reaction needs coordination with a noble metal, sensitive ligands and proton acid additives. Therefore, the design of a simple and efficient catalyst system without any acid additives under mild conditions is still a major challenge. In this work, a simple ruthenium/deep eutectic solvent catalytic system was developed to effectively catalyse the alkoxycarbonylation reaction without any sensitive ligands or acid additives under mild conditions. The conversion of 1-hexene reached 99.0 %, and the ester selectivity was 99.1 %, much higher than that of Ruthenium carbonyl without deep eutectic solvent. The excellent performance of the catalytic system could be ascribed to the form of the ruthenium active species [Ru(CO) 2 Br 3 ] − in the deep eutectic solvent. This innovative catalyst system presents a significant advancement in the alkoxycarbonylation reaction, eliminating the use of acid additives and delicate ligands.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xiaomin Qiu,Chaoting Deng,Xiaoyu Cao,Hengjun Gai,Hongbing Song
In this work, choline fluoride, choline chloride, and 2-fluoroethyl-trimethylammonium bromide containing –F, –Cl, and –Br structures were used as hydrogen bond receptors. Acetamide, urea, trifluoroacetamide, xylitol, ethylene glycol, malonic acid and lactic acid containing –HN 2 , –COOH, –OH, and –F structures were used as hydrogen bond donors. We constructed functional deep eutectic solvents rich in hydrogen bond donors and acceptors while providing alcohol hydrogen bond attraction sites and aldehyde and ketone hydrogen bond attraction sites. The efficient separation and enrichment of trace alcohols, aldehydes, and ketones in Fischer-Tropsch (F-T) oil products were achieved through hydrogen bond interaction. The mechanism of selective extraction of different types of oxygenated compounds by functionalized deep eutectic solvents was revealed, and the linear relationship among structure, hydrogen bond descriptor, and extraction performance was clarified through quantum chemistry calculations. Further, liquid–liquid extraction was used to extract and separate the oxygenated compounds from high-temperature F-T oil products using the synthesized functional deep eutectic solvent. The experimental results showed that propanol, butyraldehyde, and methylethylketone could be extracted simultaneously and efficiently, and the solvent effects were consistent with the results of quantum chemistry calculation. The excellent extraction and separation effects were due to the large number of hydrogen bonds and oxyphilic atomic forces of deep eutectic solvents. The modern solvent was reasonably designed, which is significant for extracting different oxygenated compounds from high-temperature F-T oil products.
✓ 已验证
产品关联
DOI
高影响因子
TENSIDE SURFACTANTS DETERGENTS
·
2023
·Vol. 60
·期 6
·569-587
·
IF 1
Qian Wang,Xu Li,Jinxiang Dong
In this paper, anionic branched-chain tertiary fatty alcohol sulfate surfactants were synthesized from n -hexene and n -octene using selective olefin dimerization, hydration reaction (hydroxylation), and sulfur trioxide sulfation. The direct hydration reaction of the α-olefin dimer 2-butyl-1-octene with water as a model reaction was explored for the synthesis of branched-chain tertiary fatty alcohols. Two branched-chain tertiary fatty alcohol sulfate surfactants, namely C 12 -SBTAS and C 16 -SBTAS, with different carbon chain lengths, were synthesized by the sulfur trioxide sulfation method. Their structures were confirmed by various analytical techniques, including HPLC, FT-IR, HR-MS, and 1 H NMR. Equilibrium and dynamic surface tension, foaming, wetting, and emulsifying properties were compared with those of Guerbet cetyl alcohol sulfate (C 16 -SGAS). C 12 -SBTAS and C 16 -SBTAS exhibited good surface activity with equilibrium surface tension ( γ
CMC ) values of 27.41 mN m −1 and 26.69 mN m −1 , respectively. They also had low foaming and rapid defoaming abilities, as well as good wetting and emulsifying properties, which match the application characteristics of typical branched-chain surfactants.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Lujie Liu,Lu Liu,Kaidi Zhang,Mingyang Qin,Huimin Luan,Zhaochi Feng,Jiexun Chen,Liang Wang,Feng-Shou Xiao
Selective transformation of olefins is an important route to produce cyclic monoether glycol products, but the current catalysts still suffer from insufficient activity, selectivity, and durability. Herein, we reported that molybdenum oxide on siliceous beta zeolite was highly efficient for the selective conversion of cyclohexene with a trans-2-methoxycyclohexanol yield as high as 95% in the presence of methanol and tert-butyl hydroperoxide as an oxidant. This reaction included the epoxidation of cyclohexene and subsequent solvolysis. Mechanistic studies revealed that the siliceous beta zeolite benefited the formation of abundant monomeric MoOx species, which was efficient for both the epoxidation of cyclohexene and subsequent solvolysis. Furthermore, this catalyst was also active for the conversion of other olefins, achieving the corresponding β-alkoxyalcohols.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yulin Yao,Zonghan Yang,Pengfei Zheng,Zhenheng Diao
The accessible TiO 6 concentration and the hydrophobicity of hierarchical TS-1 zeolites are both considered as critical factors for promoting the catalytic performance of selective oxidation. However, simultaneously enhancing these two factors still remains a challenge. Herein, hierarchical TS-1 zeolites with high hydrophobicity and concentration of accessible TiO 6 were fabricated via sequential amphiphilic organosilane-assisted pre-treatment, dry-gel conversion and hydroxyl radical post-treatment, using amphiphilic organosilane and surfactant as meso -porogens. The synthesis mechanism was investigated, and it was found that the interaction between the amphiphilic organosilane and Ti species formed during the pre-treatment benefited the formation of accessible TiO 6 during the subsequent dry-gel conversion. During the post-treatment of zeolite with H 2 O 2 solution under ultraviolet light irradiation, appropriate H 2 O 2 concentration facilitated the generation of hydroxyl radical and thus enhanced the hydrophobicity of zeolite without significantly influencing the TiO 6 concentration. The hierarchical TS-1 displayed excellent catalytic performances in 1-hexene epoxidation and oxidative desulfurization, with conversion improvements of 91.2%±2.8% and 348%±17%, respectively, compared with the conventional counterpart.
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Hailing Sun,Liyuan Cao,Yuhao Zhang,Liang Zhao,Jinsen Gao,Chunming Xu
The effect of acid concentration and reaction temperature on the reaction of 1-hexene cracking to propylene was investigated. The catalysts with different acid concentrations were prepared by the alkali ion and phosphorus modification of ZSM-5 zeolite. It was observed that both decreasing the concentration of strong Brønsted acid sites (SBASs) and increasing reaction temperatures can enhance the selectivity and yield of propylene and hinder the formation of side products including hydrogen, C1∼C5 alkanes, aromatics, and coke. The hydrogen transfer reaction had an important effect on the selectivity of C3∼C5 olefins in the high concentration of SBASs. Besides, high temperatures intensified monomolecular reactions and hindered bimolecular or multimolecular reactions.On the basis of product distributions, possible main and side reaction routes were summarized under the real industrial reaction conditions. The conclusion was significant to optimize the catalyst design of olefin cracking or pyrolysis processes and operation conditions for increasing the yield of propylene.
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Xiao Li,Liusha Li,Tingting Qin,Gong Gun,Tiejun Lin,Liangshu Zhong
Tandem hydroaminomethylation is an efficient and green route for one-pot synthesis of amines directly from olefins. Herein, heterogeneous hydroxyapatite (HAP) supported single-atom Rh catalyst was prepared and used for tandem hydroaminomethylation of olefins. Characterization techniques confirmed the atomic dispersion of Rh species on HAP. Up to 99% conversion of 1-hexene with high selectivity to the desired amines (93.2%) was obtained over 0.5Rh 1 /HAP catalyst. Mechanism study demonstrated that the first hydroformylation step during the tandem catalytic process was rate-determining. Compared with the Rh nanoparticles on other oxide supports (Mg 3 Al, MgO and Al 2 O 3 ), the atomically dispersed Rh sites on HAP ensured the high hydroformylation activity, thereby guaranteed the outstanding catalytic performance for the total tandem process. Furthermore, various corresponding amines can be obtained with satisfactory yields over 0.5Rh 1 /HAP catalyst from a wide scope of olefins or amines substrates.
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 12
·3077-3084
·
IF 6.569
Jiani Zhang,Huaizhong Shi,Yue Song,Wenjing Xu,Xianyu Meng,Jiyang Li
Titanium silicalite-1 (TS-1) zeolite, as a promising shape-selective catalyst, has excellent catalytic activity in many oxidation reactions. However, there are still challenges to rapidly synthesize TS-1 and achieve a high content of Ti in TS-1 without anatase TiO2. In this work, a high-efficiency strategy has been proposed by using 1,3,5-benzenetricarboxylic acid (H3BTC) as a crystallization modifier to rapidly synthesize enhanced-Ti TS-1 zeolite without extra-framework anatase TiO2. In such a synthetic system, a mixed liquid–solid precursor phase is formed within 4.5 hours, and then TS-1 crystals can be produced within one day based on the special combination mechanism of liquid-phase and solid-phase conversion. Ti species enter into the TS-1 framework by the transformation from the liquid phase to crystals as well as by the in situ transformation of the solid phase, which makes the content of framework Ti increase significantly, and the Si/Ti ratio can reach 48.5 without any anatase TiO2. In the epoxidation of 1-hexene with H2O2 as an oxidant, the conversion of alkene over the synthesized TS-1 was improved by 8.01% compared to the traditional TS-1 (18.11% vs. 10.10%). The high-efficiency strategy reported in this paper will provide new opportunities for further promoting the industrial application of TS-1 zeolite.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）