CRYSTENGCOMM
·
2024
·Vol. 26
·期 38
·5469-5478
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IF 2.6
Shengjie Zhu,Xiaomin Zhang,Lei Dong,Yangyang Yuan,Xiuyun Ma,Yanping Chen,Lei Xu
Hierarchically structured materials are considered to be one of the important options to enhance the mass transportation efficiency in microporous zeolites. Herein, we reported a highly efficient steam-assisted crystallization strategy for the synthesis of a hierarchical TS-1 zeolite with a tunable macropore size. The amorphous SiO2–TiO2 precursor dissolved gradually and acted as both a nutrient supplier and macropore template in situ. The framework Ti content of the synthesized TS-1 zeolites could be tuned over a wide range (Ti wt% = 0.70–1.39) by varying the Ti content of the SiO2–TiO2 precursor. Moreover, the pore size of the macropores could be modulated according to the particle size of the precursor based on the investigation of the formation mechanism of the macropores in the hierarchical TS-1 zeolite. The hierarchical TS-1 zeolite exhibited better catalytic activity in the epoxidation reaction of 1-hexene and hydroxylation of phenol compared to the typical microporous zeolites. The improved performance of the hierarchical TS-1 zeolite was probably caused by the improved diffusion performance of the hierarchical structure.
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高影响因子
FUEL
·
2025
·
IF 7.5
Yuanyuan Cui,Gang Fu,Jiaxing Wen,Li Yang,Jiaxu Zhang,Jianmin Sun
The direct synthesis of cyclic carbonates from olefins involves a tandem process of olefin epoxidation and CO 2 cycloaddition, but designing a single catalyst with multiple active sites remains a challenge. In this work, a series of dual ligands quaternized Zr-based MOFs (Zr-Bpydc(Py + Br − )/CoTCPP-x, x = 1–5) were successfully synthesized by co-assembling 2,2′-bipyridine-5,5′-dicarboxylic acid (Bpydc) and cobalt(II) 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin (CoTCPP) with Zr 6 clusters, followed by post-synthetic quaternization to incorporate nucleophilic Br − sites. Among them, Zr-Bpydc(Py + Br − )/CoTCPP-4 exhibited the best catalytic performance under mild reaction conditions (80 °C, 1.0 MPa, 12 h), achieving styrene conversion of 94.2 % and styrene carbonate (SC) selectivity of 66.5 %, significantly outperforming most previously reported heterogeneous catalytic systems under cocatalyst-free conditions. The excellent catalytic activity was attributed to the synergistic effect among redox-active Co 2+ sites, Lewis acidic Zr 4+ and Co 2+ sites, Br − sites, and basic pyridyl sites. Importantly, the catalyst also demonstrated broad substrate applicability and good recyclability, with negligible activity loss over five consecutive cycles. Furthermore, density functional theory (DFT) calculations elucidated the energy profile and reaction pathway of the styrene oxidative carboxylation reaction, revealing the cooperative roles of multiple active sites in both epoxidation and CO 2 cycloaddition reactions. Therefore, this work proposes a strategy based on the synergy of multiple active sites for developing efficient and recyclable heterogeneous MOF catalysts for CO 2 conversion.
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Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 47
·40842-40849
·
IF 9.5
Yumeng Hu,Yulin Yao,Zhenheng Diao,De Sun,Yuanyuan Dong
The catalytic performance of TS-1 zeolites in selective oxidation reactions is strongly influenced by both the TiO6 concentration and specific surface area. However, simultaneously optimizing these two critical factors remains a significant challenge. Herein, a biuret-assisted hydrothermal synthesis strategy was developed to fabricate hierarchical TS-1 zeolites with high TiO6 concentration and enhanced specific surface area. The interaction between the amide groups of biuret and Ti monomers promoted the formation of TiO6 during crystallization, while the confinement effect of biuret facilitated the construction of mesopores. The resulting hierarchical TS-1 exhibited good catalytic activity and stability towards 1-hexene epoxidation and oxidative desulfurization reactions, where the conversion was 1.41 and 3.36 times higher than that of conventional TS-1, respectively. This work provides a facile approach for designing high-performance TS-1 catalysts by dual regulation of active sites and porosity.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jilong Lu,Meizhen Xie,Lipin Chen,Qing Song,Siew Yin Chan,Yong-Huan Yun
Iridescent CSM is obtained from shrimp shell by deproteinization, demineralization and deacetylation. • Iridescent CSM is a mesoporous material with Bouligand structure. • CSM exhibited chromatic responsiveness toward aldehydes, ketones and acids. • CSM successfully identified all highly oxidized samples through noticeable color changes. Lipid oxidation is a major cause of food deterioration and can be detected visually using colorimetric sensors. However, existing sensors often involve the use of harmful chemicals or dyes. This study aimed to exploit the potential of structurally colored biomaterials as lipid oxidation sensors. An iridescent chitosan membrane (CSM) with structural color was fabricated from shrimp shells by chemical deproteinization, demineralization and deacetylation. Its responsiveness toward 28 volatile lipid oxidation products was investigated, and its effectiveness as a lipid oxidation sensor was evaluated. The results showed that the CSM exhibited a Bouligand structure. The membrane had a deacetylation degree of 83.97%, a specific surface area of 0.30 m 2 /g, an average pore volume of 0.0006 cm 3 /g, and an average pore diameter of 8.76 nm. It showed visible color changes upon exposure to aldehydes, ketones, and organic acids, with minimum visually discernible concentrations of 14 μmol/L for organic acid, 54 μmol/L for aldehydes and 1085 μmol/L for ketones. Moreover, CSM exhibited excellent structural stability and remained chemo-responsive during one year of storage under room temperature conditions. Eight soybean oil samples derived from the same oil but at different oxidation stages were used for assessing the performance of CSM as a lipid oxidation sensor. Out of the eight oil samples, the CSM correctly identified the oxidation status of seven, showing no color change for fresh samples and visible color changes for oxidized ones. This work demonstrates the potential of the structurally colored CSM as a biocompatible and chemical-free colorimetric indicator for lipid oxidation detection. Download: Download high-res image (225KB) Download: Download full-size image
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2026
·
IF 3.1
Shiyang Wang,Lijia Ding,Ruotong Chen,Yang Yang,Jianhao Guo,Xiaofeng Xue,Ning Zhao,Yibin Zhan,Tiedong Xie,Boping Liu,Yulong Jin
Trimetallic catalysis provides a potential route for the one-pot production of multimodal PE with balanced mechanical and processing properties. Herein, a series of CrO x /VO x /CpCr/SiO 2 trimetallic catalysts are constructed by grafting CrCp 2 onto a CrO x /VO x /SiO 2 with tunable CrCp 2 loadings and benchmarked against mono- and bimetallic catalysts. FT-IR spectroscopy confirmed successful CrCp 2 immobilization, and the catalyst containing 0.25 wt% CrCp 2 exhibited the highest productivity. Owing to the distinct H 2 sensitivities of the three active sites, both molecular weight (MW) and molecular weight distribution (MWD) can be efficiently regulated through CrCp 2 loading and H 2 partial pressure, enabling the synthesis of tri- or broad-modal PE in a single reactor. Compared with unimodal PE of comparable MW, the trimodal PE exhibited lower melt viscosity and an improved stiffness-toughness balance.
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Inorganic Chemistry Frontiers
·
2026
·
IF 6.4
Rui Feng,Wei Wang,Tianbo Li,Feifei Yang,Xiaoyan Hu,Xinlong Yan,Lianming Zhao,Shijian Lu
The selective production of linear aldehydes from long-chain α-olefins using heterogeneous Rh catalysts faces a challenge, as non-selective sites in unconfined environments severely compromise regioselectivity. Herein, we report a strategy to achieve high regioselectivity and activity in 1-hexene hydroformylation by confining atomically dispersed Rh sites within the micropores of a silicalite-1 (S-1) zeolite, followed by the selective poisoning of external Rh sites. A series of Rh@S-1 catalysts with varying loadings were synthesized by an in situ hydrothermal method. Comprehensive characterization (XRD, XPS, STEM) confirmed the successful incorporation of Rh as atomically dispersed species within the MFI framework while preserving the zeolite’s textural properties. In the hydroformylation of 1-hexene, the unpoisoned catalyst exhibited high conversion (98.3%) but poor regioselectivity (n/i = 2.7). The introduction of bulky thiol poisons (DMBT and TPMT), which are size-excluded from the zeolite micropores, selectively passivated the external Rh sites. Consequently, the reaction was confined predominantly to the internal Rh sites, thereby dramatically boosting the n/i ratio to 59.9 and 9.3 for DMBT and TPMT poisoned catalysts, respectively, at a low 1-hexene concentration. The superior regioselectivity achieved with DMBT over TPMT is attributed to its more effective poisoning of pore-mouth Rh sites. However, it also introduced higher diffusion resistance, leading to lower conversion and higher apparent activation energy. Moreover, the catalysts demonstrated excellent recyclability. This work elucidates the decisive roles of confined internal versus unconfined external Rh sites in the atomically dispersed Rh@S-1 catalyst for 1-hexene hydroformylation. This finding provides a key design principle for developing efficient heterogeneous Rh catalysts for long-chain α-olefin hydroformylation.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Jiayi Xin,Jiawen Hu,Ziyang Song,Changwen Zhao,Dong Chen,Wantai Yang
The persistent accumulation of polymers in terrestrial ecosystems poses significant environmental challenges. Herein, the biodegradation of poly(1-hexene-maleic anhydride) (HMA) in soil and Pseudomonas aeruginosa was investigated to mitigate its environmental impact. The experimental results revealed that the mineralization rate of HMA reached 17.6% after 90 days of incubation in soil. Bacterial degradation led to a 79.0% weight loss after cultivation with Pseudomonas aeruginosa for 30 days. In addition, HMA exposure induced distinct shifts in soil microbial communities, with Proteobacteria abundance increasing from 40.3 to 48.9% after the initial 5 days but subsequently declining to 34.6% due to the inhibitory effects of biodegradation intermediates. Furthermore, phytotoxicity assays demonstrated that soybean seedlings exhibited pronounced root elongation, reduced lateral root formation, and elevated oxidative stress biomarkers after HMA exposure. Earthworm (Eisenia fetida) tests revealed that the biotoxicity of HMA depended on both concentration and exposure time. The median lethal concentration after 24 h was 3.63 mg/cm2, and the mortality rate reached 46.7% after 14 days in soil. Progressive degradation of HMA mitigated both oxidative stress and biotoxic effects over time, indicating a self-attenuating ecological risk profile. These findings provide a comprehensive understanding of the environmental behavior, biodegradation mechanisms, and biotoxic effects of HMA, offering valuable insights for the design and assessment of sustainable petroleum-based polymers.
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PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Yuanlong Guo,Yang You,Gu Guo,Zixiang Chen,Wei Peng,Lijie Hu,Songmiao Liang,Haibo Xie
Herein, a serial of full cellulose and lignosulfonate derivatives (LS), including sodium lignosulfonate (LSS), calcium lignosulfonate (LSC), lignosulfonic acid (LSA), composite films were generated through dissolving cellulose in reversible carbon dioxide (CO 2 ) ionic liquids solvent system (TMG/EG/DMSO/CO 2 solvent system), followed by a facile solution-gelation transition and absorption strategy. The findings indicated that LS aggregated and embedded inside the cellulose matrix via H-bond interaction. The cellulose/LS derivatives composite films showed good mechanical properties which the tensile strength reaches the maximum value of 94.7 MPa in MCC3LSS film. While for the MCC1LSS film, the breaking strain increases to 11.6 %. The outstanding UV shielding effect and high transmittance in the visible region of composite films were also achieved and the shielding performance of the whole UV region (200–400 nm) tended to 100 % for MCC5LSS film. In addition, thiol-ene click reaction was selected as model reaction to verify the UV-shielding performance. It was also found that the oxygen and water vapor barrier performances of composite films were evidently associated with the intense H-bond interaction and tortuous path effect. The OP and WVP of MCC5LSS film were 0 and 6 × 10 −3 g·μm/m 2 ·day·kPa, respectively. These outstanding properties make them with great potential for packaging field.
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SEPARATION SCIENCE AND TECHNOLOGY
·
2023
·
IF 2.8
XueFeng Sun,Yueqin Song,Xiaolong Zhou
With the massive requisition of light olefins in dedicated areas of petrochemical industry, adsorption separation approaches are developed to meet the requirements. The literature studying long-chain olefins/alkanes is scarce, and the actual adsorption capacity of liquid-phase is rarely studied. In this paper, the adsorption process of Ag-10× zeolite for long-chain alkanes/olefins was systematically studied, the preparation conditions and operating conditions of the zeolite were investigated. The samples were characterized by XRD, BET and XPS. The results show that silver ions were uniformly dispersed on the surface of the zeolite. The actual adsorption capacity of the modified zeolite was determined in intermittent experiments by liquid phase concentration difference and pore volume correction. The experimental data were fitted and the results showed that the Langmuir isotherm equation was more appropriate for adsorption, indicating that the adsorbent surface was homogeneous. The quasi-secondary kinetic chemical equation was consistent with the adsorption of olefins by the modified 10× zeolite, indicating that the process was a chemisorption process. Experimental results shows that Ag-10× zeolite is an excellent adsorbent for separating long-chain olefins/alkanes mixed systems.
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FUEL
·
2022
·
IF 8.035
Xu Li,Jiaqi Li,Xiaohong Wang,Lijun Yang,Hong Xu,Jinxiang Dong
Despite the significant progress that has been made regarding the purification of C5–C9 linear α-olefins from the liquid products of Fischer–Tropsch synthesis, the energy-consuming separation of olefins and paraffins with the same carbon number has restricted their industrial development. Herein, we first propose a reaction-separation-utilization integrated process that combines the zirconocene/methylalumoxane-catalyzed selective dimerization of linear α-olefins to α-olefin dimers, which can then be separated from paraffins in FTS liquid products via conventional distillation and catalytically converted into branched-chain sulfonate surfactants through homogeneously organocatalytic sulfonation with sodium bisulfite. The resulting branched-chain sulfonates have been characterized by FTIR, HPLC , LC-MS, HR-MS, and NMR techniques. Their surfactant properties, including equilibrium surface tension, dynamic surface tension , foaming property, wetting ability, and emulsifying power, and detergency performance, have been thoroughly investigated. The results showed that the resulting branched-chain sulfonate surfactants exhibit superior surfactant properties and detergency performance in comparison with commercially applied linear alkylbenzene sulfonate (LAS). In view of the growing demand for anionic surfactants in the detergent and cosmetics industries , this study represents a new route for the use of α-olefins from the Fischer–Tropsch synthesis for the production of branched-chain surfactants.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Chen Chen,Qiong Tang,Hong Xu,Mingxing Tang,Xuekuan Li,Lei Liu,Jinxiang Dong
Naphthenic base oil is an important lubricating base oil and very scarce in the global petroleum resources. Herein, a series of alkylated tetralin fluids similar to naphthenic base oils were produced by the alkylation of tetralin and α -olefins ( n -hexene, n -octene, n -decene) with ionic liquid Et 3 NHCl/AlCl 3 as the catalyst, where the applied raw materials are totally derived from the coal chemical industry. The product composition could be controlled by adjusting the feeding ratio of tetralin and olefin. The synthetic fluids were evaluated as lubricating base oils to reveal the structure–property correlations. Their principal physicochemical and tribological properties depend on the chain-length of α -olefins and the number of alkyl groups onto the aromatic rings. Bis-(octyl- or decyl-) alkyl tetralin exhibited good properties in terms of viscosity, thermo-oxidation stability and pour point, as well as friction-reducing and anti-wear performance, showing great potential for producing naphthenic base synthetic oils from coal-based chemicals.
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Reaction Chemistry & Engineering
·
2022
·Vol. 8
·期 4
·778-783
·
IF 5.2
Huan Liu,Yi-Xuan Yao,Hong-Yan Shang,Da Yang,Yuan-Yu Tian
The tandem hydroformylation–acetalization of olefins with H2O as the hydrogen source was accomplished over an Ir(I)-catalyst using the phased warming strategy. Due to the release of protons by AlCl3-hydrolysis equilibrium, the tandem reaction was significantly enhanced. The conversion of 1-hexene was 100% and the selectivity for oxo-products was 89%, where 91% of acetals was obtained. Moreover, the hydrogenation by-products were detected to be less than 3%, showing that H2O as the hydrogen source inhibited the hydrogenation of olefins in this tandem reaction. Moreover, isotope-labeling experiments confirmed that water was the hydrogen source, and the key Ir–H active species for hydroformylation were captured by high-pressure 1H NMR spectroscopy analyses.
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