JOURNAL OF CHEMICAL RESEARCH
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2022
·
IF 1.097
Mengting Zhang,Shengbin Shi,Yan Lei,Liuyu Gu,Lijing Gao,Guomin Xiao
Alkylphosphinates have received extensive attention in the past few decades because of their very useful mechanical properties, electrical properties, low density, and low toxicity, and have been widely used in flame-retardant materials and other fields. In this work, aluminum diethylphosphinate is successfully synthesized under atmospheric pressure. More importantly, two novel dialkylphosphinates, aluminum dioctylphosphinate and aluminum didecylphosphinate, are first synthesized and characterized. The structures of these aluminum dialkylphosphinates are confirmed by nuclear magnetic resonance, Fourier-transform infrared spectroscopy, and high-resolution mass spectrometry, and the microscopic morphology and thermal stability are analyzed by scanning electron microscopy and thermogravimetric analysis, respectively. Furthermore, conditions for the synthesis of aluminum dioctylphosphinate are optimized. Compared with the traditional method of synthesizing dialkylphosphinates under high pressure, the method reported in this paper has the advantages of high safety, easy operation, and low economic cost, which makes it suitable for industrial production.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 8
·3901-3908
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IF 3.925
Zhiping Chen,Li Liu,Faxiang Shi,Wenwu Zhou,Zhiyuan Yang,Anning Zhou
A series of hierarchical SAPO-11 molecular sieves synthesized by adding mesoporogens with different alkyl chain lengths were prepared. The synthesized hierarchical SAPO-11s were characterized by XRD, SEM, N2 adsorption–desorption, TEM, NH3-TPD and Py-IR. The results showed that the physicochemical properties of the hierarchical SAPO-11s change with the increase of the alkyl chain length, and the hierarchical SAPO-11 molecular sieve synthesized with DTAB has the largest external surface area and pore volume, and the most medium and strong B acid sites. Furthermore, the 1-octene hydroisomerization reaction on Ni catalysts supported on hierarchical SAPO-11 was investigated and the experimental results showed that the alkyl chain length of the mesoporogen has an obvious influence on the hydroisomerization selectivity. The hierarchical Ni/SAPO-11 catalyst synthesized using DTAB has the highest selectivity of C8 isomers and the lowest cracking selectivity. These results indicate that DTAB is the most suitable mesoporogen for the synthesis of hierarchical SAPO-11 molecular sieves for 1-octene hydroisomerization.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-9
·
IF 16.6
Liu Yifeng,Liu Zhiqiang,Hui Yu,Wang Liang,Zhang Jian,Yi Xianfeng,Chen Wei,Wang Chengtao,Wang Hai,Qin Yucai,Song Lijuan,Zheng Anmin,Xiao Feng-Shou
Hydroformylation is one of the largest industrially homogeneous processes that strongly relies on catalysts with phosphine ligands such as the Wilkinson’s catalyst (triphenylphosphine coordinated Rh). Heterogeneous catalysts for olefin hydroformylation are highly desired but suffer from poor activity compared with homogeneous catalysts. Herein, we demonstrate that rhodium nanoparticles supported on siliceous MFI zeolite with abundant silanol nests are very active for hydroformylation, giving a turnover frequency as high as ~50,000 h −1 that even outperforms the classical Wilkinson’s catalyst. Mechanism study reveals that the siliceous zeolite with silanol nests could efficiently enrich olefin molecules to adjacent rhodium nanoparticles, enhancing the hydroformylation reaction.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Xiujun Wang,Jian Zhang,Qiang Liang,Ming Duan,Shenwen Fang,Chunsheng Zhang,Jiaqing Chen
Hydrophobically modified polyacrylamide (HMPAM) is one of most used amphiphilic polymers for polymer flooding in oilfield. The interaction between HMPAM and crude oil is key to the oil displacement efficiency of HMPAM. However, due to the lack of experimental research method, there is little research on this aspect. In this work, HMPAMs containing different types of amphiphilic monomers were prepared, their interactions with crude oil were studied by dual polarization interferometry (DPI) for the first time, and their adsorption conformations on the surface of crude oil were discussed. The DPI results directly shown that the influence of amphiphilic monomer type on the interaction strength was as follows: nonionic type > cationic type ≈ anionic type. This order was consistent with the adsorption capacity of amphiphilic monomer on the surface of crude oil, indicating that the interaction strength between HMPAM and crude oil mainly depended on the type of amphiphilic monomers. In addition, the DPI results indirectly shown that the effect of amphiphilic monomer type on the HMPAM molecular coiled conformation on the surface of crude oil was also determined by the adsorption capacity of amphiphilic monomer. The research results of this paper can provide useful information for the amphiphilic monomer selection from the perspective of improving oil displacement efficiency of HMPAM.
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JOURNAL OF MOLECULAR LIQUIDS
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2023
·
IF 6
Jian Zhang,Xiujun Wang,Qiang Liang,Ming Duan,Shenwen Fang,Chunsheng Zhang,Jiaqing Chen
Hydrophobically modified polyacrylamide (HMPAM) is one of the commonly used polymers for polymer flooding. Because it is water soluble, there are many reports on the impact of HMPAM on the stability and treatment of produced water (it is O/W emulsion), but few reports on its influence on the demulsification of W/O crude oil emulsion. In this paper, firstly, three types of HMPAM containing cationic, anionic, and nonionic hydrophobic monomers (abbreviated as P(AM-AANa-N)Cn, P(AM-AANA-S)Cn, and P(AM-AANA-O)Cn, respectively) were synthesized; Then, demulsification experiments and interface behavior experiments (including dynamic interfacial tension, dilatational rheology and dynamic coalescence time measurement) were conducted to investigate the influence of HMPAM on the demulsification performance of a W/O heavy oil emulsion demulsifier D1. The demulsification results showed that HMPAM reduced the dehydration speed of D1, the type of hydrophobic monomer and the length of hydrophobic chain in HMPAM can affect the final water separated of D1. P(AM-AANa-S)Cn, P(AM-AANa-N)Cn with long hydrophobic chain, and P(AM-AANa-O)Cn with short hydrophobic chains had the negative effect on performance of D1. The results of dynamic interfacial tension experiments indirectly showed that HMPAM had the influence on the D1′s conformation and speed of rearrangement at the W/O interface during the water droplet coalescence process, thereby affecting the reduction of elastic modulus ( G ′ ) of W/O interface and the coalescence rate of water droplets. When there was HMPAM in water, the coalescence time of water droplets increased, resulting in the decrease of dehydration rate. At the meantime, HMPAM had an impact on the lg ( G 1 ′ / G demulsifier ′ ) / lg G 1 ′ , thereby affecting the final water separated of D1.
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CHEMISTRY-A EUROPEAN JOURNAL
·
2023
·
IF 4.3
Li-Zhi Zhang,Hong-Bin Ju,Tao Geng,De-Bao Li,Ya-Jie Jiang,Ya-Kui Wang
Graphical A novel phase transfer catalyst comprising phosphotungstic acid and biquaternary ammonium cation salt is synthesized for the epoxidation of long carbon chain olefins under solvent-free conditions, which exhibits high selectivity for epoxides. Different methods are used to characterize the fundamental structure and catalytic mechanism of this catalyst. In this study, we have developed a novel catalyst synthesized by phosphotungstic acid and a gemini quaternary ammonium cation salt. This quaternary ammonium salt not only reduces the interfacial tension between olefins and hydrogen peroxide but also forms a notably stable structure with phosphotungstic acid. Dodecene was successfully epoxidized to epoxy dodecane with a selectivity of 82.9 %. The impact of initial conditions was systematically investigated such as molar ratio, temperature, reaction time, and catalyst dosage on the catalytic performance. Characterization of the catalyst morphology was performed by SEM, TEM and SAXS. Raman spectra, FT-IR and XPS spectra were employed to perform the catalyst transformation during the epoxidation reaction. This catalytic mechanism study could provide the industrial application in the epoxidation of long-chain olefins.
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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.
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Journal of Physical Chemistry C
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2023
·
IF 3.7
Kang Yuan,Hao Li,Rui Zuo,Baiqin Gan,Chengjia Xiong
Photonic band gaps of photonic crystals (PCs) are related to the effective refractive indices; therefore, it is quite difficult to detect homologues and isomers with similar reflection indices by PCs. Some researchers have tried to use some complex PCs for detecting homologues and isomers. However, there are few reports in trace detection of isomers (cis–trans isomers) and mixed isomers by using simple amorphous photonic crystals (APCs). Herein, dynamic reflection spectrum (DRS) patterns of APCs are obviously different by changing species of compounds, mixtures of two similar isomers, volatility temperatures, and diameters of SiO2. Isomers with a refractive index difference of only 0.001 and their mixtures could be distinguished based on different DRS patterns of simple APCs. For example, the difference in the refractive indices of cis-3-hexene and trans-3-hexene is only 0.001, and the difference of desorption balance time of APCs is 142 s. The method shows high sensitivity detection in isomers and cis–trans isomers.
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高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 39
·13955-13961
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IF 4
Xiaorui Yan,Lele Chen,Haisheng Wei,Tiantian Liu,Kairui Li,Jing Li
The stability of Rh-based heterogeneous catalysts is a key issue in the hydroformylation of olefins. Confinement of active Rh species has been considered an effective strategy to achieve stable catalysts. In this work, a phosphine ligand was successfully confined in ZIF-8 material and coordinated with Rh metal by a reduction procedure to develop an efficient and stable Rh-based catalyst for hydroformylation of 1-octene. The results indicate that the catalyst reduced at 300 °C under H2 atmosphere exhibits better stability than that with NaBH4 as reductant and undoped P catalyst. Various characterization studies demonstrate that the superior performance is due to the strong interaction between Rh metal and P, which inhibits the leaching of active Rh species. This work reveals an effective strategy for the synthesis of highly stable catalysts for use in the hydroformylation reaction.
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JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Lu Ye,Xiaojing Liu,Yangcheng Lu
In this work, a highly efficient palladium catalyst was facilely immobilized on the surfaces of magnetic nanoparticles with the coordination of N -heterocyclic carbene. The prepared Pd–NHC@NCPs were characterized by transmission electron microscopy, Fourier transform infrared spectroscopy, energy dispersive spectroscopy, X-ray photoelectron spectroscopy, and inductively coupled plasma atomic emission spectrometry. With suitably designed emulsion polymerization and immobilization, the final palladium loading could reach 0.78 mmol/g. The catalyst showed outstanding catalytic performance in the Suzuki–Miyaura cross-coupling reaction among various substrates, with little catalyst usage (0.03 mol.%), short reaction time, and mild reaction conditions. In addition, the catalyst could be separated conveniently from the reacting system with an external magnet and show good catalytic performance even after being reused five times or more, indicating good recyclability.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 1
·162-171
·
IF 3.186
Yang Xingyu,Li Xu,Dong Jinxiang
The epoxidation of terminal olefins (e.g., 1-octene) presents an enormous challenge owing to their electron-deficient nature, whereas the vicinal diols that are derived from epoxides are highly desirable as fine chemicals. We report the facile preparation of magnesium pyrophosphate via the thermal decomposition of commercially available newberyite and the first use of magnesium pyrophosphate as a solid catalyst for terminal olefin epoxidation. The as-synthesized magnesium pyrophosphate was characterized by XRD, FTIR, SEM–EDS, and CO 2 -TPD techniques. The CO 2 -TPD results proved that the medium base was dominant in magnesium pyrophosphate. Magnesium pyrophosphate exhibited an effective catalytic activity in the liquid-phase epoxidation of 1-octene with a 94.2% selectivity of epoxide using aqueous hydrogen peroxide as oxidant in the presence of acetonitrile solvent. The influences of various reaction parameters, including solvent, temperature, H 2 O 2 to 1-octene molar ratio, amount of magnesium pyrophosphate, reaction time, and solvent amount were investigated. According to the reaction mechanism, the perhydroxyl ion that originated from H 2 O 2 heterocracking formed in the presence of magnesium pyrophosphate and reacted with acetonitrile to generate active intermediate peroxycarboximidic acid. The epoxide and amide formed when active oxygen was transferred from peroxycarboximidic acid to the olefin. Therefore, magnesium pyrophosphate was an appropriate catalyst for 1-octene epoxidation. Graphic Abstract
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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.
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