MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
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IF 3.649
Chao Chen,Lei Cai,Liang Li,Lixia Bao,Zhengguo Lin,Guoqiang Wu
In order to develop an efficient and environmental friendly approach for epoxidation of soybean oil (SO), a series of hetero-catalysts, titanium silicalite-1 (TS-1) with different Si/Ti ratio (TS-1- x , x = 40, 70, 80), mesoporous TS-1-40 (MTS-1-40) and anatase TiO 2 , were prepared under controlled conditions. These different catalysts were characterized by various characterization methods like XRD , IR, UV–Vis, TGA , ICP , SEM, TEM and N 2 -adsorption, respectively, and the catalytic reaction experiments of the SO epoxidation were studied systematically using hydrogen peroxide (H 2 O 2 ) as clean oxidant over the different catalysts. The results reveal that the TS-1- x catalysts exhibit higher epoxidation catalytic activity and less consumption of H 2 O 2 than anatase TiO 2 , and the number of framework Ti sites in TS-1 structure played a very important role in their catalytic performance of the epoxidation reaction, which is attributed to the unique nature and coordination geometry of the Ti sites in TS-1 framework. Furthermore, the reusability and regeneration behaviors of TS-1-40 catalyst were also studied.
研究领域:
催化化学
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绿色化学
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材料科学
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工业化学
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有机合成
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环境友好工艺
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能源与资源工程
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2021
·
IF 5.455
Min Zhang,Shenyong Ren,Qiaoxia Guo,Baojian Shen
TS-1 is a typical microporous zeolite , which is hindering the timely diffusion of reaction products and is likely to cause secondary side reactions in heterogeneous catalytic reaction due to the micropore size. However, zeolite TS-1 with hierarchical pores of micropores and mesoporous/macropores can solve this problem to a great extent. In view of this, hierarchical zeolite TS-1 is synthesized by using tetrapropylammonium hydroxide (TPAOH) as structure directing agent and polyacrylamide (PAM) as a hierarchical pore-directing template. The texture property of hierarchical TS-1 can be optimized by changing the amount of PAM in the synthesis gel. With the increase of PAM content, the pore volume and specific surface area of the hierarchical zeolite TS-1 increases. Compared with the conventional TS-1, the hierarchical TS-1 samples have obvious pore size distribution in the range of 20–80 nm. It is interesting that the particle size of TS-1 decreases after adding PAM. When the hierarchical TS-1 is applied to the epoxidation reaction of 1-hexene with H 2 O 2 , the selectivity of the desired product 1,2-epoxyhexane is significantly increased.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
DOI
高影响因子
Catalysts
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2025
·Vol. 15
·期 7
·694
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IF 4
Ziyan Mi,Huayun Long,Yuhua Jia,Yue Ma,Cuilan Miao,Yan Xie,Xiaomei Zhu,Jiahui Huang
The development of non-noble metal catalysts for gas-phase propylene epoxidation with H2/O2remains challenging due to their inadequate activity and stability. Herein, we report a Cs+-modified Ni/TS-1 catalyst (9%Ni-Cs/TS-1), which exhibits unprecedented catalytic performance, giving a state-of-the-art PO formation rate of 382.9 gPO·kgcat−1·h−1with 87.8% selectivity at 200 °C. The catalyst stability was sustainable for 150 h, far surpassing reported Ni-based catalysts. Ni/TS-1 exhibited low catalytic activity. However, the Cs modification significantly enhanced the performance of Ni/TS-1. Furthermore, the intrinsic reason for the enhanced performance was elucidated by multiple techniques such as XPS, N2physisorption, TEM,29Si NMR, NH3-TPD-MS, UV–vis, and so on. The findings indicated that the incorporation of Cs+markedly boosted the reduction of Ni, enhanced Ni0formation, strengthened Ni-Ti interactions, reduced acid sites to inhibit PO isomerization, improved the dispersion of Ni nanoparticles, reduced particle size, and improved the hydrophobicity of Ni/TS-1 to facilitate propylene adsorption/PO desorption. The 9%Ni-Cs/TS-1 catalyst demonstrated exceptional performance characterized by a low cost, high activity, and long-term stability, offering a viable alternative to Au-based systems.
研究领域:
催化化学
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化学工程
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材料科学
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多相催化
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绿色化学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS LETTERS
·
2013
·
IF 2.224
Zhuang Zhuang,Libin Yang,Xue Jiang,Feng Xin
Highly b -oriented Titanium Silicalite-1 (TS-1) film grew on the surface of glass modified with TS-1 precursor solution . By means of a facile sol–gel method, the glass surface was covered with TS-1 precursor, which modified the glass surface property to make it suitable for the growth of oriented TS-1 film. The influence of different immersion times for the growth of the oriented TS-1 films on the glasses was studied. X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM) and attenuated total reflection infrared spectra (AT-FTIR) were used to study the crystal orientations , morphologies and the existence of framework Ti of the TS-1 films. The results showed that a highly b -oriented TS-1 monolayer could be prepared with the immersion time of 12 h, following with hydrothermal synthesis at 448 K for 24 h.
✓ 已验证
DOI
高影响因子
RSC Advances
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2014
·Vol. 4
·期 52
·27259-27266
·
IF 3.708
Libin Yang,Feng Xin,Junzhong Lin,Zhuang Zhuang,Rui Sun
In this study, a hydrothermal synthesis was developed to prepare a thin titanium silicalite-1 catalyst layer in the internal channels of the honeycomb cordierite support, which was used in a continuous heterogeneous reaction. The as-prepared thin TS-1 catalyst layer was characterized by SEM, XRD, UV-vis and ATR-FTIR methods. Multiple hydrothermal syntheses were used for controlling the crystalline growth to optimize catalytic activity and lifetime. Moreover, a monolithic TS-1/cordierite reactor with external looping was utilized to investigate the characteristics of the continuous heterogeneous ammoximation reaction without the organic solvent tert-butanol (TBA). The reaction results showed that the conversion of cyclohexanone and selectivity of oxime approached more than 0.96 and 0.98, respectively. When compared with the reaction using TBA as the reaction solvent, the activity of the monolithic TS-1/cordierite showed no differences except for a longer lifetime.
研究领域:
化学工程
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催化化学
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材料科学
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工业化学
·
绿色化学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2013
·
IF 3.365
Xue Jiang,Zhuang Zhuang,Feng Xin
Highly b-oriented Titanium Silicalite-1 (TS-1) zeolite films were synthesized on polyvinyl acetate (PVAc) modified glasses by hydrothermal crystallization. The prepared samples were characterized by X-ray diffraction (XRD), field-emission scanning electron microscope (FE-SEM), atomic force microscopy (AFM), Fourier transform infrared spectroscopy (FT-IR) and a contact-angle instrument. The results showed that the mass of PVAc on the glasses would influence the process of superficial nucleation and oriented growth of TS-1 films profoundly. A favorable amount of PVAc on smooth surface of glassy substrate was determined to form a highly b-oriented and fully covered TS-1 film by attracting appropriate precursor and template, then making TS-1 nucleate and grow orientedly. Based on the obtained results, a scheme of fabricating b-oriented TS-1 films was proposed.
研究领域:
材料科学
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无机化学
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薄膜制备
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沸石化学
✓ 已验证
DOI
高影响因子
Inorganics
·
2025
·Vol. 13
·期 2
·37
·
IF 3
Yao Wang,Hongda Yu,Huan Wang,Tiehong Chen
The environmental and health impacts of sulfur compounds in fuel oil have prompted considerable research interest in oxidative desulfurization (ODS) technology. Tetrahedrally coordinated titanium has been demonstrated to exhibit excellent activity in the context of oxidative desulfurization processes. However, further improving the catalytic property of the tetrahedrally coordinated titanium remains a challenging endeavor. In the context of ODS processes conducted at near room temperatures, the improvement of conversion remains a subject of considerable challenge. In this study, hierarchically porous titanosilicate hollow spheres were synthesized by using TS-1 zeolite precursors as Ti and Si sources to obtain the catalyst with only tetrahedrally coordinated titanium. The synthesized materials were characterized through transmission electron microscopy (TEM), Fourier-transform infrared spectroscopy (FT-IR), ultraviolet–visible diffuse reflectance spectroscopy (UV-Vis), and nitrogen adsorption analysis. These techniques confirmed the formation of hollow spherical hierarchically porous structures with Ti species uniformly incorporated in tetrahedral coordination and the presence of five-member rings of TS-1 zeolite. As a result, the hierarchically porous titanosilicate hollow spheres demonstrated excellent catalytic performance in ODS, achieving complete dibenzothiophene (DBT) removal within 15 min and a high turnover frequency (TOF) of up to 123 h−1at 30 °C.
研究领域:
催化化学
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环境化学
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材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2026
·
IF 2.6
Yining Chen,Fangna Shangguan,Weilong Chun,Lijia Li,Xin Yang,Jiale Qi,Yujing Xun,Huiyong Chen
TS-1 zeolite demonstrates notable activity and selectivity in cycloolefin epoxidation when employing H₂O₂ as the oxidant.However, the practical application of conventional TS-1 is significantly limited by factors including surface hydrophilic structures and mass transfer constraints. To address these challenges, a carbon-encapsulated hierarchical TS-1 (3DC_TS-1) has been synthesized through the confined growth approach, in which 3DOm carbon is used as a confined space provider for TS-1 crystallization and further acts as a hydrophobic wrapper to modulate the surface microenvironment of TS-1 crystals. In the epoxidation of cyclopentene and cyclohexene with using H₂O₂ as the oxidant, the hydrophobic 3DC_TS-1 catalyst exhibits a superior selectivity to epoxide products by suppressing epoxide hydrolysis and allyl oxidation side reactions, comparing with the 3D_TS-1 catalyst without carbon wrapper and the conventionally microporous TS-1 catalyst.It is expected that this study will provide an effective strategy for designing zeolite catalysts applying to selective oxidation reactions.
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Chenyang Zhao,Hongwei Zhu,Yujia Liu,Junjie Feng,Xiang Feng,Wei Xu,Zhe Yang,Bing Sun
The direct epoxidation of propylene has been a hot topic in the academic field for years. Researchers have spent extensive effort on the development of catalyst, however, only limited attention on the effect of reaction conditions, especially pressure. In this paper, we found for the first time that elevated pressure should favor the forward epoxidation reaction, it actually led to a drop of reaction rate in this system. We proposed explanation by considering the difficulty of gas molecules diffusing into and out of the micropores on the TS-1 zeolite surface. Higher pressure would inhibit the escaping of the gas molecules from the micropores and lead to carbon deposition inside the channel. To validate this hypothesis, we designed and compared catalysts with micropores blocked (BTS-1) and unblocked (TS-1) and found that the BTS-1 showed higher resistance to pressure change and significantly longer life time than the TS-1.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·
IF 9.3
Yuefeng Qiu,Peng Jiang,Wenkai Ye,Jiahao Hu,Bin Zhang,Tuo Ji,Liwen Mu,Xin Feng,Xiaohua Lu,Jiahua Zhu
An electrochemical–thermal tandem reaction system was designed in this work and enabled the highly efficient synthesis of propylene oxide (PO) at 1 atm without the use of H2O2. The electrochemical part produced OOH− through a 2e− oxygen reduction reaction, which migrated and distributed in the full space of a chamber filled with a mixture of solid electrolyte particles and modified TS-1 (m-TS-1) catalysts. Mediated by the relay of OOH− and protic solvent methanol, full space tandem reactions were achieved with a high PO selectivity of 95.2% and a productivity of 319.75 mmol gecat−1 h−1. A mechanistic study revealed that the m-TS-1 catalysts accepted the migrated OOH− and formed a Ti-OOH intermediate, which played a key role in relaying the tandem reactions for an efficient propylene epoxidation reaction. Techno-economic analysis and life-cycle assessment revealed favorable figures for the proposed process compared to the conventional process.
研究领域:
化学工程
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催化科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2026
·
IF 2.6
Qishan Chen,Hui Ding,Bo Zhu,Xu Li,Jinxiang Dong
The green and efficient epoxidation of long-chain linear α-olefins represents a crucial step in the synthesis of key industrial intermediates. Although the hydrogen peroxide/titanosilicate-1 (H2O2/TS-1) catalytic system is environmentally friendly, its broad industrial implementation has long been hindered by unsatisfactory epoxide selectivity and low H2O2 utilization efficiency, which limit large-scale and economical production. To overcome these limitations, a strategy employing tetrapropylammonium bromide (TPABr) as a crystallization modifier was developed to precisely engineer the active sites of TS-1 zeolites. By balancing the incorporation kinetics of titanium and silicon into the framework, uniform distribution of titanium species was achieved, accompanied by the enrichment of highly active Ti(OH)2(OH2)2(OSi)2 sites. The resulting TS-1-TPABr-40 catalyst delivered outstanding performance in the epoxidation of 1-hexene, exhibiting 97% epoxide selectivity, ∼76% effective H2O2 utilization, and good recyclability. These results highlighted how molecular-level coordination engineering in zeolite catalysts could simultaneously enhance catalytic efficiency and oxidant economy, providing a sustainable and scalable strategy for green chemical synthesis.
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Jiaojiao Yu,Yi Zuo,Gudan Li,Hong Yang,Xinwen Guo
To synthesize a high-performance titanium silicalite-1 (TS-1), this paper reports a simple and environmentally friendly approach to regulate the alkalinity in the synthesis of titanium silicalite-1 (TS-1) involving tetrapropylammonium hydroxide (TPAOH) and tetrapropylammonium bromide (TPABr). Essentially, the pH of the synthesis gel was controlled by n(TPAOH/TPA+), while keeping the total tetrapropylammonium cations (TPA+) constant. The study shows that at a relatively moderate alkalinity of pH = 10.7, TS-1 produced exhibits nanocrystalline microstructure favorable for diffusion, contains high contents of TiO4 and TiV, and delivers 94.3% of H2O2 conversion with a turnover frequency of 565.6 mol (mol h)−1 in propylene epoxidation. Through detailed analysis of crystallization processes of TS-1 at different alkalinities, this study unveils the effect of alkalinity on the rate of Si–Ti condensation, which dictates the formation of the framework structure and incorporation of Ti species into the framework. Essentially, only at moderate alkalinity of pH = 10.7, comparable Si–OH and Ti–OH condensation rates permit the highest amount of Ti being inserted in TS-1 as active (TiO4 + TiV) and limits the self-condensation of Ti species to form inactive anatase-TiO2.
研究领域:
材料科学
·
催化化学
✓ 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）