JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Meile Yue,Kankan Bu,Yahong,Zhang,Wei Shen,Hualong Xu,Zhen Huang
Propane dehydroaromatization (PDA) provides a promising route to produce valuable chemicals such as benzene, toluene and xylene via non-petroleum feedstocks, in which Ga-modified MFI zeolites demonstrate high activity but are susceptible to severe coke deposition. The defect-derived silanols (Si-OH) in zeolite formed during synthesis has emerged as a predominant factor, making the prolongation of the catalyst longevity a major challenge. Here, we developed a gallosilicate MFI zeolite with silanol-defect remediated (Ga-MFI-AHFS) through an ammonium hexafluorosilicate post-treatment, which exhibited an extraordinary activity and stability. Ga-MFI-AHFS exhibits a nearly unchanged propane conversion around 82.0 % with aromatics selectivity around 64.5 % compared to a 25.4 % conversion decline on the raw zeolite with defects exposed during the 20-h CO 2 assisted PDA reaction. The results of FTIR and MAS NMR showed a decreased content of silanol nests as well as the internal Si-OH groups, indicating the successful repair of silicon hydroxyl defects. The restored framework endows the Ga-MFI-AHFS zeolite with an excellent coking resistance, giving a much lower coking-rate of 5.8 × 10 −8 mol C /mol C-in-produced-Aromatics , which is one-sixth of that on Ga-MFI. This work developed a facile route to prepare Ga-MFI zeolite with suppressed silanol-defects, which could help to realize a stable dehydroaromatization of light alkanes.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Yi Liu,Kaishi Ding,Xiao Fan,Sixing Chen,Shengyan Meng,Jiahui Yan,Yunlei Gao,Jinming Lu,Yi Liu
Despite that oriented MFI zeolite films exhibit significant prospects for a wide range of applications due to microstructural superiority, their precise orientation control entails rigorous demands on reaction conditions (e.g., reaction temperature). In this work, we achieved facile synthesis of continuous b -oriented MFI zeolite films with few twins over a wide crystallization temperature range of 30–210 °C through adopting NH 4 F-mediated gel as nutrient during epitaxial growth. Both ammonium ions and fluorine ions were found crucial for enhancing the gel reactivity, endowing epitaxial growth with higher crystallization rates; moreover, the above morphology could be maintained even under fluctuating temperature conditions during film processing, thereby showing great potential for their bath production in a facile and reproducible manner.
研究领域:
材料科学
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化学工程
·
催化
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Guojun Lv,Xuyang Zou,Yan Chen,Qing Zhang,Xubin Zhang,Fumin Wang
The successful one-pot synthesis of MCM-41/MFI composite is mainly concentrated on the trivalent heteroatom of Al 3+ and Fe 3+ , however there are almost no reports about the one-pot synthesis of Ti-MCM-41/MFI composite. In this work, we reported the one-pot synthesis of Ti-MCM-41/MFI composite with a temperature-gradient hydrothermal strategy using hexadecyl trimethylammonium bromide CTAB and silicalite-1 seed as structure directing agents as well as ammonia solution as alkali source, and its application as heterogeneous catalyst in the cyclohexene epoxidation reactions. The impact of Si/Ti molar ratio and ammonia dosage as well as CTAB amount on the formation and property of Ti-MCM-41/MFI composite were systematically investigated. In addition, a possible partial transformation mechanism of Ti-MCM-41/MFI composite sample was proposed. The synthesized Ti-HMZ-50-N3.77-Se0.05 sample with ordered mesoporous structure and high content of framework titanium active centers revealed the eminent cyclohexene epoxidation performance, achieving a 32.51 % of cyclohexene conversion and a 61.27 % selectivity of cyclohexene oxide within 5 h of reaction.
研究领域:
催化化学
·
材料化学
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纳米材料
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多相催化
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绿色化学
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JOURNAL OF MATERIALS SCIENCE
·
2015
·Vol. 51
·期 6
·3257-3270
·
IF 2.371
Nian Pei,Su Meihui,Yu Ting,Wang Zheng,Zhang Binxing,Shao Xiuli,Jin Xiaoyong,Jiang Nanzhe,Li Shan,Ma Qiang
A novel highly compact and b -oriented MFI-type zeolite monolayer was obtained by assembling sec -butanol-modified rounded-coffin-shaped silicalite-1 microcrystals by Langmuir–Blodgett (LB) method. The LB monolayer was subsequently tested as a seed layer for the secondary growth of uniformly b -oriented and defect-free MFI zeolite films on stainless steel substrates and platinum electrodes. Three different methods were evaluated for identifying a suitable synthesis route to suppress the undesired a -oriented twin growth during the synthesis of MFI films. The crystal intergrowth and orientation of the MFI films were characterized by scanning electron microscopy and X-ray diffraction (XRD). The crystallographic preferred orientation indices and preferred orientation coverage values calculated using the XRD data were used to quantitatively determine the preferred orientation and surface coverage of the prepared zeolite films. The experimental results confirm that the low tetrapropylammonium hydroxide (TPAOH) method is the most effective route to suppress the undesired a -oriented twin growth, when the highly b -oriented LB monolayer was used as the seed layer for the secondary growth of the b -oriented MFI film. The highly b -oriented MFI-type zeolite film-modified electrodes were further tested as the working electrodes in electrochemical experiments. Cyclic voltammetry experimental results confirmed that the b -oriented MFI films fabricated at low TPAOH concentration were defect free and possessed a distinct molecular sieving property after calcination. The LB method, a highly reproducible and controllable method for the organization of zeolite crystals, can be further applied as an effective platform for the promotion and development of zeolite-modified electrodes as selective sensors. Graphical
研究领域:
材料科学
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电化学
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纳米材料
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传感器
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薄膜制备
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晶体工程
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高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Xianglong Tan,Jianwei Zhang,Yuting Zhang,Jiahuan Du,Chun Zhang,Xuehong Gu
MFI zeolite membranes are typically synthesized with the aid of an organic template, i.e., tetrapropylammonium hydroxide (TPAOH). Consequently, it is crucial to remove the template from the membrane and simultaneously minimize non-selective defects. Ozonation at low temperature has been known as a mild detemplation to produce high-selective zeolite membranes reproducibly. However, the microstructural evolution of zeolite membrane especially template molecules during ozonation remains unclear. In this study, the microstructural evolution of the TPAOH molecule in MFI zeolite during low-temperature ozonation was investigated. The thermogravimetric analysis (TGA) and N 2 adsorption results indicate the gradual reduction in the amount of template with increasing ozonation time. The Fourier-transform infrared (FT-IR) spectroscopy, in-situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) and 13 C nuclear magnetic resonance (NMR) results suggest the formation of new carbon species in the final zeolite. After ozonation for 8 h, ca. 87 % in mass of the template was removed from the MFI zeolite membrane. In comparison with the MFI zeolite membranes treated with air calcination, the MFI zeolite membranes detemplated in O 3 for 8 h (MFI-O 3 _8 h) exhibited a superior separation factor of 801 in para-xylene/ortho-xylene (PX/OX) separation at 150 °C, indicating fewer defects existed in the membrane. The as-synthesized membrane exhibited good separation stability during the PX/OX separation. In addition, MFI zeolite membranes were synthesized on hollow fiber supports with a length of 40 cm. These membranes showed excellent performance for xylene isomer separation (PX/OX separation factor >90).
研究领域:
材料科学
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化学工程
·
膜技术
·
无机化学
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JOURNAL OF POROUS MATERIALS
·
2022
·Vol. 30
·期 1
·247-258
·
IF 2.523
Wu Wenhui,Lei Qian,Liang Linlin,Wei Richu,Chen Honglin
ZSM-5 is considered to have great potential in the catalytic synthesis of Trioxane (TOX), and the effect of acidity on TOX selectivity was explored. [Al]-MFI-50, [B]-MFI-50, Platelike [Ga]-MFI-50 and a series of [Ga]-MFI-y materials were investigated by XRF, XRD, XPS, SEM, NH 3 -TPD, BET, Py-FTIR, 71 Ga MAS NMR and 1 H MAS NMR. According to the results, it is clear that the Ga-MFI have a better effect on the selective of TOX compared with the [Al]-MFI, Platelike [Ga]-MFI-50 and [B]-MFI. This is mainly due to the change in the ratio of Brønsted acid density to Lewis acid density (B/L ratio), and the selectivity of TOX increases with the B/L ratio. Moreover, the percentage increase in density of Brønsted acid is less than that of Lewis acid when the ratio of Si atoms to Ga atoms is decreased. So the ratio of Brønsted acid density to Lewis acid density(B/L ratio) decreases. [Ga]-MFI-50 exhibited better catalytic performance among all catalysts with a selectivity of 97.79% for TOX.
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ACS Omega
·
2024
·
IF 3.7
Jin Quan Tao,Yi Jing Jia,Yan Cui,Tian Yu Bai,Xi Nan Xue,Rong Peng Yao,Ya Song Zhou,Qiang Wei
The synthesis of zeolites through more efficient, environmentally friendly, and cost-effective methods was deemed significant in both industrial applications and academic fields. Conventional hydrothermal synthesis strategies have encountered difficulties in producing pure silica MFI zeolite (silicalite-1) under amine-free conditions. This was primarily attributed to the competitive growth of quartz, keatite, or magadiite during the crystallization process. In this work, it was found that the lack of nucleation ability was an important reason for the poor crystallization stability of the methanol solution. Well-crystallized silicalite-1 zeolites with uniform particle sizes were achieved through the cooperative guidance of methanol and seed crystals. Large-scale experiments with silicalite-1 zeolite demonstrated good reproducibility. Combined with the TG-IR and N2 adsorption–desorption results, it was observed that, when an extremely small amount of seed (0.97 wt %) was introduced, methanol could play a role as a crystallization promoter in the hydrothermal synthesis system. Furthermore, a lower alkaline-to-silica ratio and water-to-silica ratio were conducive to the progression of the crystallization process. In summary, this work presented a hydrothermal synthesis strategy for the synthesis of silicalite-1 zeolite in a methanol solution without the need for a large amount of seeds and provided an effective pathway for the low-cost, large-scale production of silicalite-1 zeolite.
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高影响因子
Nature Catalysis
·
2024
·Vol. 7
·期 6
·666-677
·
IF 42.8
Dou Xiaomeng,Yan Tao,Qian Lixiang,Hou Huaming,Lopez-Haro Miguel,Marini Carlo,Agostini Giovanni,Meira Debora M.,Zhang Xiangjie,Zhang Liang,Cao Zhi,Liu Lichen
Achieving the regioselective hydroformylation of linear α-olefins to linear aldehydes using solid catalysts with regioselectivities comparable to the corresponding homogeneous process is a great challenge in the chemical industry. Despite the tremendous efforts devoted to this research topic, most of the reported heterogeneous metal catalysts still give considerably lower regioselectivities than well-established homogeneous metal catalysts. Here we show the design of efficient Rh-zeolite catalysts, in which subnanometre Rh clusters are selectively confined in the sinusoidal ten-membered-ring channels of MFI zeolite, for the hydroformylation of long-chain linear α-olefins (C 6 –C 12 ) into linear aldehydes with very high linear-to-branched aldehyde ratios (up to 400). The exceptional catalytic performances result from the involvement of the MFI zeolite framework as a rigid solid ligand that accommodates subnanometre Rh clusters in the sinusoidal channels of the MFI zeolite.
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Membranes
·
2026
·Vol. 16
·期 4
·122
·
IF 4.2
Zhenming Yi,Zilin Pan,Feng Ye,Shuanshi Fan,Xuemei Lang,Yanhong Wang,Gang Li
Conventional high-temperature calcination for activating MFI zeolite membranes is energy-intensive and prone to inducing defects. Here, we demonstrate that a rapid ozonation treatment at 200 °C for only 1 h effectively decomposes organic templates while preserving membrane integrity. The resulting membrane exhibits H2/CH4and H2/N2ideal selectivities of 10.3 and 6.5, respectively, at room temperature, with C3H8and SF6permeances below the detection limit. These results confirm a dense, defect-minimized architecture and good molecular sieving performance of the zeolite membrane. In contrast, extending ozonation to 48 h leads to defect formation and a marked reduction in selectivity. For H2/CH4mixture separation, the membrane achieves a selectivity of 23.8 at 100 °C, which is highly competitive among reported MFI membranes. In isopropanol dehydration, it achieves a water flux of 2.3 kg·m−2·h−1and a separation factor of 3278 at 70 °C with a 10 wt% water feed, while maintaining >99.5 wt% water content in the permeate over a broad operating temperature range (30–70 °C). This work establishes rapid ozonation as a scalable, energy-efficient activation method for high-performance MFI zeolite membranes in both gas and liquid separations.
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高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Kaiwei Wang,Fumin Wang,Xubin Zhang,Mingshuai Sun,Yi Zhai,Yihao Wang,Hongyu Wang,Yang Qin,Hao Ruan
Nanosheet MFI zeolite with a shortened b-axis length is highly desirable for industrial applications due to the predominant mass transfer pathway provided by its larger straight channels along the b-axis. The introduction of specific additives into the precursor fluid of the zeolite can facilitate crystal anisotropic growth. However, the range of available additives is limited, and their role and underlying mechanisms remain poorly understood. Herein, the effect of three pyrrolidone compounds on the anisotropic growth of the TS-1 zeolite is unveiled within the crystallization engineering, such as 2-pyrrolidone, N-methylpyrrolidone, and N-vinyl-2-pyrrolidinone. The effects of different water content (H2O/SiO2 = 40, 100, and 160), pyrrolidone compound addition (x/SiO2 = 0.2, 0.6, 1, and 2), and seed liquid concentration on the nanosheet morphology of zeolite were studied. The TS-1 nanosheet zeolite synthesized using pyrrolidone compounds as an additive exhibits abundant high coordination titanium active sites and demonstrates excellent catalytic performance in olefin epoxidation. In this work, the crystals form a nanosheet zeolite in a nonclassical growth path. The ATS-100-1-1 sample had a thickness of 112 nm in the b-axis direction and an Lc/Lb aspect ratio of 20.08. The development of morphological engineering strategies can be extended to zeolites with other topological structures based on the intrinsic properties and interactions of additive molecules with different crystal faces.
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高影响因子
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2026
·
IF 3
Zijian Wang,Jiashuo Zheng,Jiahan Li,Hao Pang,Ming Ke,Zhaozheng Song
During the isoamylene oligomerization catalyzed by MFI zeolite, it is found that the dimerization selectivity is clear correlated with micropore volume and percentage of external surface area. The sample with balance of mesopore and acidity makes the conversion and yield rates exceed 92.3 % and 60 % within 12 h.
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高影响因子
Catalysts
·
2026
·Vol. 16
·期 5
·452
·
IF 4.5
Jingang Zhao,Guanchao Wang,Taoyang Zou,Yuekun Jing,Fang Liu
While the petroleum industry undergoes structural adjustments in supply and demand alongside a green and low-carbon transition, water drilling mud generated during oil extraction poses severe environmental challenges. Consequently, addressing the solid waste pollution and disposal issues associated with drilling mud has become critical. In this study, ZSM-5 zeolite was synthesized using water drilling mud as a silicon and aluminum source, inexpensive n-butylamine as a template agent, and a combined approach of alkali-melting activation pre-treatment and seed-directed hydrothermal synthesis. By adjusting key parameters such as water content, template agent dosage, and seed addition, optimal synthesis conditions were determined. Based on these conditions, a series of ZSM-5 zeolites with varying silicon-to-aluminum ratios were synthesized. Characterization results from XRD, TEM, SEM, and N2adsorption–desorption experiments revealed that all prepared samples exhibited high crystallinity, regular morphology, and high specific surface area.27Al MAS NMR results indicated that almost aluminum species were located at the framework structures with four-coordination. In the 1,3,5-triisopropylbenzene cracking reaction, the conversion rate increased with decreasing silicon-to-aluminum ratio, consistent with variations in acid amount. These findings achieve high-value utilization of waste drilling mud, offering a novel pathway for low-cost synthesis of high-performance ZSM-5 zeolite. This breakthrough injects fresh momentum into the petroleum refining industry’s green sustainable development, fostering a win–win scenario that harmonizes ecological conservation with industrial profitability.
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高影响因子
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