JOURNAL OF MATERIALS SCIENCE
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2019
·Vol. 55
·期 4
·1614-1626
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IF 3.442
Pan Liuyi,He Yulong,Niu Menglong,Dan Yong,Li Wenhong
Ni 2 P catalysts supported on different supports, such as SiO 2 from different sources, Al 2 O 3 , TiO 2 and ZrO 2 were prepared for the hydrodeoxygenation of p-cresol (monocyclic phenol model in coal tar). The reaction was carried out on a fixed-bed reactor at a temperature of 330–390 °C under 2 MPa. The order of conversion of p-cresol was as follows: Ni 2 P/SiO 2 -2 > Ni 2 P/SiO 2 -3 > Ni 2 P/SiO 2 -1 > Ni 2 P/Al 2 O 3 > Ni 2 P/ZrO 2 > Ni 2 P/TiO 2 . Ni 2 P/SiO 2 -3 shown higher DDO path selectivity, resulting in the conversion of p-cresol of 93% and a selectivity of 72.6% for BTX products under the reaction temperature of 370 °C with LHSV of 0.5 h −1 . This catalyst was also used for the hydrodeoxygenation of the crude phenolic mixture extracted from coal tar, which shown that the phenol deoxidation rate was 87.6% and the BTX product selectivity was 73.7% by GC–MS.
研究领域:
化学工程
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催化反应
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DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
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2026
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IF 7.8
Zunlong Hu,Denglei Gao,Huanrong Liu,Qingyang Li,Linjie Wang,Xiaofei Zhang,Haodong Xie,Yuhan He,Xiulin Wang,Changjian Liu,Zhijie Wu
Beta zeolite catalysts modified by compositing with USY and ZSM-5 achieve high BTX selectivity by integrating the advantages of different zeolite types. • The reaction pathway of 1-MN conversion to BTX in the graded catalytic system and the corresponding catalyst structure-activity relationship were elucidated. • The B-Y-Z three-bed graded catalyst enhances tandem relay catalysis between different zeolite beds, achieving the highest BTX selectivity. Hydrocracking of polycyclic aromatic hydrocarbons (PAHs) to produce benzene, toluene, and xylene (BTX) represents an effective route for upgrading light cycle oil (LCO). However, this process tends to generate large amounts of alkylbenzenes with long or multiple side chains, making it difficult for a single catalyst to achieve a high BTX selectivity. Herein, composite zeolite catalysts and graded catalyst systems were designed and prepared for the hydrocracking of 1-methylnaphthalene (1-MN) to BTX at a temperature of 420 °C and a pressure of 6 MPa. The NiW/BY-20 catalyst (Beta-USY zeolite composite) promotes the ring-opening cracking of monocyclic aromatics and the side-chain cleavage of alkylbenzenes, increasing the BTX selectivity and yield to 37.4% and 36.4%, respectively. The NiW/BZ-20 catalyst (Beta-ZSM-5 zeolite composite), with its strong acidity and high dealkylation capability, further improves the BTX selectivity and yield to 38.1% and 37.3%, respectively. These results indicate that composite zeolite catalysts can synergistically integrate the catalytic properties of zeolites with distinct topologies, enabling a relay catalysis pathway. Further investigations reveal that the graded catalyst system optimizes the reaction process; the B-Y catalyst (NiW/Beta in the upper bed, NiW/USY in the lower bed) increases the BTX selectivity and yield to 38.5% and 38.3%, respectively. The optimized B-Y-Z three-bed graded catalyst (upper: NiW/Beta, middle: NiW/USY, and lower: NiW/ZSM-5) exhibits excellent compatibility with the reaction pathway for 1-MN hydrocracking to BTX. It enhances the tandem catalytic effect while maintaining high hydrocracking activity, achieving BTX selectivity and yield of 41.3% and 40.2%, respectively, with alkylbenzene selectivity reduced by 3.3%. This work demonstrates that the synergistic design of composite zeolites and graded catalysts can effectively boost the efficient and targeted conversion of PAHs to BTX, providing valuable insights for the construction of bifunctional catalytic systems tailored for multistep tandem reactions. We propose a strategy that combines zeolite composite modification with different topologies and catalyst grading to developing efficient hydrocracking catalyst. The B-Y-Z three bed graded catalyst exhibits excellent compatibility with the reaction pathway for 1-MN hydrocracking to BTX. It enhances the tandem catalytic effect while maintaining high hydrocracking activity, achieving BTX selectivity of 41.3%, with alkylbenzene selectivity reduced by 3.3%. Download: Download high-res image (100KB) Download: Download full-size image
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Yihua Yue,Jian Tian,Jiechao Ma,Shui Yang,Wen Li,Jiale Huang,Qingbiao Li,Guowu Zhan
Herein, Ga-ZnZrO x &ZSM-5 bifunctional catalysts were designed for CO 2 thermal hydrogenation to aromatics, particularly, aiming to enhance the selectivity of high-value BTX ( i.e. , benzene, toluene, and xylene). It was evident that the exterior surface properties and acidity of ZSM-5 can be effectively tailored by in-situ silicon deposition originating from the rice husk template. Catalytic performance assessments demonstrate an optimized catalyst achieving 88.1 % aromatics selectivity (exclusive CO) in a single pass, with a notable 45.2 % BTX selectivity within total aromatics and a low CO selectivity of 23.6 %. This superior performance is attributed to the in-situ silicon deposition on ZSM-5 during one-pot synthesis and the optimized spacing between Ga-ZnZrO x and ZSM-5 facilitated by the rice husk platform. Furthermore, in-situ DRIFTS analysis identifies key reaction intermediates. This study offers an effective strategy for tuning zeolite acidity using rice husks, while modulating metal oxide-zeolite proximity on the bio-SiO 2 platform, thus boosting CO 2 conversion to aromatics.
研究领域:
催化
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化学工程
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环境科学
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材料科学
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DOI
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2022
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IF 6.437
Linlin Yi,Hong Yao,Xian Li,Zhenzhong Hu,Liu Shi,Yangwei Wu
The catalytic pyrolysis is a promising method for obtaining value-added aromatics, especially benzene, toluene and xylene (BTX). For different biomass-based materials, the dual catalyst system composed of CaO-based and ZSM-5-based catalysts showed an obvious selectivity for the BTX production. This study chose CaO derived from organic calcium precursors (Org-CaO) and nano-sized ZSM-5 (NZSM-5), and comprehensively investigated the effects mechanism of biomass components on the formation pathways of BTX via Py-GC/MS. Under the catalysis of NZSM-5, the BTX yields were only 7.8–30%. The BTX yields on Org-CaO/NZSM-5 were as follows: lipid (63.1%) > hemicellulose (55.4%) > cellulose (40.2%) > lignin (21.7%). Typical pyrolysis intermediates were employed to quantitatively reveal the intermediate reactions. Pyrolysis intermediates exhibited low BTX-forming reactivity over NZSM-5. The pre-catalysis of Org-CaO selectively converted part undesired intermediates (fatty acids and furans) into BTX precursors (short-chain olefins and ketones), facilitating the remarkable increase of BTX yield in the subsequent NZSM-5 catalysis process. However, the pre-catalysis of Org-CaO can hardly make the ring opening reaction of lignin-derived phenolic compounds that have very low reactivity on NZSM-5, and thence high-lignin biomass obtained low BTX production during catalytic pyrolysis by Org-CaO/NZSM-5. These findings afforded a new route for increasing the BTX yields by directionally forming BTX precursors or controlling biomass components.
研究领域:
能源与环境科学
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化学工程
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Hongdan Zhang,Chunyang Wu,Jialiang Wang,Ying Zhao,Peng Cheng,Zhen Zhao
In recent years, the efficient utilization of light alkanes, especially iso-butane and n-butane, has attracted increasing attention. Here, a series of ZSM-5 zeolite-encapsulated Pt-xZnO (x = 0, 0.05, 0.1, 0.25, 0.5, 1) catalysts were prepared via a one-pot hydrothermal method. The dispersion of metal particles, state of metal species, structure, and acidity of catalysts were confirmed by multiple physical and chemical characterizations. The catalysts were used in the catalytic cracking of iso-butane; the conversion of iso-butane would increase with the increase of ZnO content. However, Pt-0.1ZnO@ZSM-5 presented the best catalytic effect. The yield of ethylene and propylene reached 55% at 625 °C; meanwhile, the total yield of high value-added ethylene, propylene, butene, and BTX was as high as 80%.
研究领域:
化学工程
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催化
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材料科学
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 35
·15512-15523
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IF 2.7
Sen Fu,Hanxu Guo,Hong Yuan
A nano-ZSM-5 zeolite having a hierarchical pore structure was synthesized using L-lysine as a mesopore template and growth inhibitor. The effects of the L-lysine/Si and Si/Al molar ratios on the morphology and pore structure of the zeolite were studied. The products were characterized by scanning electron microscopy, transmission electron microscopy and N2-Brunauer–Emmett–Teller surface area analysis. These assessments showed that the particle size of the ZSM-5 zeolite could be reduced to 60 nm with a surface area as high as 395 m2 g−1 and a high density of mesopores. These zeolites were applied to the catalytic pyrolysis of oleic acid in a fixed-bed reactor to generate benzene, toluene and xylenes (BTX). At a reaction temperature of 500 °C, the catalyst having L-lysine/Si and Si/Al ratios of 0.4 and 30, respectively, gave a BTX yield of 27.4 wt%. This yield decreased with increases in the Si/Al ratio whereas varying the L-lysine/Si ratio did not produce a specific trend. The spent catalyst was characterized by thermogravimetric analysis and exhibited superior anti-coking ability and longer catalytic lifetime compared with a standard ZSM-5 zeolite.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Jian Zhang,Liang Wang,Zhiyi Wu,Hai Wang,Chengtao Wang,Shichao Han,Feng-Shou Xiao
We report the synthesis of Zn/ZSM-5 particles coated with a silicalite-1 zeolite shell (core–shell Zn/ZSM-5@silicalite-1) via grinding of the raw silica source materials with TPAOH and Zn/ZSM-5, followed by solvent-free crystallization at 180 °C for 72 h. The product was well characterized by the XRD patterns, N2 sorption isotherms, SEM images, and TEM images. Because of the core–shell structure, the Zn/ZSM-5@silicalite-1 sample exhibits high selectivities for benzene, toluene, and xylenes in the conversion of methanol, compared with those over ZSM-5 and Zn/ZSM-5 samples. The solvent-free synthesis offers an alternative method for preparing core–shell Zn/ZSM-5@silicalite-1 catalysts.
研究领域:
催化化学
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材料科学
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2026
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IF 10.6
Shihe Zhang,Shuo Li,Yijun Tian,Chengna Dai,Ruinian Xu,Biaohua Chen
Cr-Zr/ZSM-5 converts PE at 280 °C to BTX and SAF with 93% selectivity. • Self-supplied H from BTX formation saturates C 9 -C 16 to SAF without external H 2 . • Zr doping lowers dehydrogenation barrier and boosts electron transfer. The catalytic conversion of polyethylene (PE) into a C 6 -C 8 BTX-rich fraction and a C 9 -C 16 SAF-range hydrocarbon fraction provides a potential route for plastic-carbon valorization, where “SAF-range” refers to the aviation-fuel-relevant carbon-number range rather than to specification-compliant finished SAF. However, many reported PE-upcycling routes require elevated temperatures, external H 2 , noble-metal catalysts, or high catalyst-to-feed ratios. Herein, we report a rationally engineered bifunctional Cr-Zr/ZSM-5 catalyst that converts PE at 280 °C and 0.5 MPa into targeted products with a liquid yield of 62 wt% and approximately 90% selectivity within the BTX-rich C 6 -C 8 fraction and SAF-range C 9 -C 16 hydrocarbons. Combined characterization, pyridine-adsorbed FTIR, online mass spectrometry, in situ FTIR, product analysis, and model-surface DFT calculations support a proposed bifunctional reaction network. A proposed reaction network is constructed, in which initial conversion may involve thermal and surface-assisted fragmentation at accessible external/near-external regions. Cr-Zr oxide-related species may subsequently facilitate adsorption, C-H activation, dehydrogenation, and olefin-intermediate formation. The resulting smaller olefinic intermediates can then undergo Brønsted-acid-initiated secondary conversion within the MFI channels, while product formation is accompanied by dynamic, competitive internal hydrogen redistribution without external H 2 . This work bridges atomic-scale engineering with catalytic function, providing a scalable, mechanism-guided platform for plastic waste valorization and establishing a fundamental mechanistic framework for the rational design of tandem catalytic systems in waste-to-fuel conversion. Download: Download high-res image (206KB) Download: Download full-size image
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Jie Li,Yuxiang Yang,Guangtong Xu,Xiangxu Du,Anbang Dai,Yangchuan Ke
Spatially orthogonal CeO x –Zn sites were integrated into aerogel-derived hierarchical HZSM-5. • CeO x shifted HCl release and chlorinated-intermediate conversion to lower temperatures. • Zn promoted BTX-selective aromatization of dechlorinated and oxygenated fragments. • Accessibility-weighted bifunctional catalysis enabled cleaner and higher-value PVC/PET upcycling. Catalytic upcycling of chlorine-containing mixed plastics remains limited by the intrinsic conflict between efficient dechlorination and high-selectivity aromatization. Here we report a spatially orthogonal CeO x –Zn/Aero-40 catalyst derived from a diatomite-aerogel-templated hierarchical HZSM-5 support, in which CeO x -rich outer mesopores and Zn-containing MFI channels are integrated into a gated tandem architecture. The hierarchized support decreased the mean particle size from 386 ± 42 nm for Conv-40–274 ± 31 nm for Aero-40 and retained a shortened crystallite length of 289 ± 24 nm after dual-site loading, while exposing 3.01 wt% surface Ce and 1.86 wt% surface Zn on CeO x –Zn/Aero-40. Under the optimized two-stage conditions, CeO x -Zn/Aero-40 affords a BTX yield of 64.0 wt% on the initial dry-polymer feed basis, a BTX selectivity of 90.0% within the quantified liquid aromatics, and a dechlorination efficiency of 98.9%. Product-family analysis showed that aromatics rose to 71% whereas organochlorines fell to 2%; chlorine balance further demonstrated that 88% of chlorine was released as gaseous HCl, with only 3% remaining as oil-phase organochlorine. Taken together, the time-resolved spectroscopic/thermal analyses, probe experiments and kinetic measurements are consistent with a functionally staged mechanism in which Ce-associated sites facilitate low-temperature HCl elimination and chlorine management, whereas Zn-associated acid environments favor downstream cyclization/dehydrogenation-aromatization toward BTX. The DFT calculations support the intrinsic feasibility of these site-specific elementary steps but do not, by themselves, establish dynamic inter-site kinetic coupling. Across ten independent parallel runs, the mean BTX yield was 63.9 wt% of the initial dry polymer feed (RSD 1.0%), while the mean dechlorination efficiency was 98.8% (RSD 0.2%), retained 96.3% Zn after five cycles, and maintained high dechlorination efficiency for model and real feeds. These results establish a hierarchical dual-site zeolite platform for chlorine-tolerant aromatics-oriented upcycling of PVC/PET mixed plastics. Download: Download high-res image (274KB) Download: Download full-size image
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高影响因子
Journal of Orofacial Orthopedics-Fortschritte der Kieferorthopadie
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2024
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IF 1.3
Pang Huiqi,Ding Luhua,Che Xiaoxia
Purpose We aimed to investigate early effects of regulating alpha‑7 nicotinic acetylcholine receptor (α7nAChR) agonists and antagonists on maxillary expansion in mice. Methods We allocated 36 six-week-old male C57BL/6J mice into three group: 1) expansion alone, 2) expansion plus the α7nAChR-specific agonist 3‑(2,4-dimethoxybenzylidene)-anabaseine dihydrochloride (GTS-21), and 3) expansion plus alpha-bungarotoxin (α-BTX), a competitive antagonist of α7nAChR. The groups were daily injected with saline, GTS-21 (4 mg/kg/day) or α‑BTX (1 mg/kg/day), respectively, from days 0–7. In addition, a mouse model of maxillary expansion was established. Masson’s trichrome staining was used to observe morphological changes and immunohistochemistry was performed to analyze α7nAChR, interleukin (IL)-1β, IL‑6, tumor necrosis factor (TNF)-α, runt-related transcription factor 2 (RUNX2), and osteocalcin (OCN) expression in the midpalatal suture. Microcomputed tomography was used to measure midpalatal suture and palatal basal bone widths. We assessed the normal distribution of our data using the Kolmogorov–Smirnoff test and evaluated the homogeneity of variance by Levene’s test, followed by a two-way ANOVA and Bonferroni tests at a significance level of P < 0.05. Results In the GTS-21+expansion group, osteogenesis was more active in the middle palatine suture. New bone was calcified and deposited in the suture and we observed decreased IL-1β, IL‑6, and TNF‑α expression ( P < 0.05). In the α‑BTX+expansion group, we observed increased proinflammatory cytokine and decreased RUNX2 and OCN expression and increased midpalatal suture and palatal basal bone widths ( P < 0.05). Conclusion Using α7nAChR agonists and antagonists to regulate the cholinergic anti-inflammatory pathway, the secretion of inflammatory factors and osteoblast markers during maxillary expansion were altered, indicating the potential for clinical modulation of maxillary palatal suture expansion.
研究领域:
牙科学
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免疫学
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药理学
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DOI
PubMed
高影响因子
ENERGY & FUELS
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2023
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IF 5.3
Haifeng Tian,Zhiyu Chen,Xing Yang,Peng Gao,Chunxue Jiao,Fei Zha,Yue Chang,Hongshan Chen
A method for the direct synthesis of hierarchical zeolites was developed by converting precursors of zeolites and mesoporous copolymers into homogeneous gels using conventional block copolymers as scaffolds. In this method, hydrothermal synthesis is accomplished on a steam-assisted basis, and the dry gel leaves the system free of the liquid water phase, which successfully avoids phase separation between the soft stencil and the solid silica phase. The catalytic performance of hierarchical zeolites was evaluated on a fixed-bed reactor for the methanol-to-aromatics reaction. The hierarchical structure greatly enhances the catalytic activity of the probe reaction due to the increased outer surface, decreased coke formation, and diffusion resistance in the microporous network. The selectivity of BTX reached 65.8%, and there was no significant deactivation after a reaction of 107 h. The transition state and energy barrier for methanol to aromatics were obtained by the minimum energy search of the LST/QST transition state.
研究领域:
化学工程
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催化
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材料科学
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高影响因子
Journal of Energy Chemistry
·
2025
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IF 14.9
Wenjun Chen,Yiyi Fan,Yue Liu,Xiaobin Xie,Fan Zhang
Converting waste plastics directly into valuable aromatic chemicals is a promising, cost-effective recycling strategy. Traditional zeolite-catalyzed cracking of polyolefins to produce aromatics often needs high temperatures and faces issues like low selectivity for liquid aromatics, separation difficulties, and rapid catalyst deactivation due to coking. To address this, a multifunctional Ni/HZSM-5 catalyst was developed to efficiently upgrade various polyolefins—including polyvinyl chloride—into gaseous alkanes (C 1 –C 5 ) and easily separable liquid aromatics (C 6 –C 12 ) at 400 °C, without added solvents or hydrogen. Aromatic products make up 57.1 wt% of total output, with more than 97.8% selectivity for the liquid phase and a BTX (benzene, toluene, and xylene) selectivity of 76.1%. The high activity and selectivity for aromatics stem from synergistic interactions between Ni nanoparticles (NPs) and acid sites in the zeolite, which promote selective C–C bond breaking and control hydrogenolysis and aromatization pathways. This synergy allows precise control over the distribution of products by carbon number and favors the formation of separable aromatics. Notably, the catalyst also prevents coking by hydrogenolyzing and hydrogenating reactive intermediates before they form stable graphite-like deposits. Consequently, Ni/ZSM-5 catalyst demonstrates excellent stability, maintaining consistent aromatics yield over 13 consecutive cycles and processing over 30 times its weight in plastics without regeneration. After regeneration, the activity of the catalyst was fully restored, highlighting its potential for industrial use. This work offers valuable insights for designing durable, high-activity catalysts, providing a practical route to improve plastic recycling technologies.
研究领域:
催化化学
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化学回收
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高分子化学
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材料科学
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环境科学
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石油化学
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高影响因子
危险品化学品经营许可证（带存储）