Molecular Catalysis
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2025
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IF 4.9
Jinghui Lyu,Tao Liu,Shihao Wang,Jun Wei,Jinke Yao,Yiyong Zhao,Han Wu,Xianghao Zhang,Peikun Li,Zhizheng Wang,Qunfeng Zhang,Dahao Jiang,Qingtao Wang,Guofu Zhang,Chengrong Ding,Xiaonian Li
TS-1 zeolite is a catalyst known for its high selective oxidation performance and broad industrial applications. The titanium atom in the TS-1 often acts as the active center in catalytic reactions, especially in oxidation reactions, so increasing the titanium content in TS-1 is of great significance in chemical reactions and catalytic applications. This paper explores a Novel Boron Extraction and Titanium Incorporation Strategy to enhance the titanium content within the TS-1 framework. During the dry gel preparation process, boron species were introduced in situ into the framework of the TS-1 to form a framework boron-titanium-silicon TS-1-B with tetra-coordinated or tri-coordinated positions. TS-1-B is then treated with acid to remove the framework boron, while an appropriate amount of titanium precursor is introduced to fill the vacancy left by the removal of the framework boron. The results of XRD, FT-IR, UV–Vis, BET, NH 3 -TPD, XRF, and XPS showed that the titanium content of the tetracoordinate framework in the TS-1 was improved. The catalytic performances of TS-1-B, TS-1-BS, and TS-1-BST were comparatively evaluated through two representative reactions: propylene epoxidation and the direct synthesis of hydrogen peroxide from H₂ and O₂.
研究领域:
催化化学
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材料科学
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无机化学
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化学工程
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多孔材料
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DOI
高影响因子
Inorganic Chemistry Frontiers
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2021
·Vol. 8
·期 12
·3077-3084
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IF 6.569
Jiani Zhang,Huaizhong Shi,Yue Song,Wenjing Xu,Xianyu Meng,Jiyang Li
Titanium silicalite-1 (TS-1) zeolite, as a promising shape-selective catalyst, has excellent catalytic activity in many oxidation reactions. However, there are still challenges to rapidly synthesize TS-1 and achieve a high content of Ti in TS-1 without anatase TiO2. In this work, a high-efficiency strategy has been proposed by using 1,3,5-benzenetricarboxylic acid (H3BTC) as a crystallization modifier to rapidly synthesize enhanced-Ti TS-1 zeolite without extra-framework anatase TiO2. In such a synthetic system, a mixed liquid–solid precursor phase is formed within 4.5 hours, and then TS-1 crystals can be produced within one day based on the special combination mechanism of liquid-phase and solid-phase conversion. Ti species enter into the TS-1 framework by the transformation from the liquid phase to crystals as well as by the in situ transformation of the solid phase, which makes the content of framework Ti increase significantly, and the Si/Ti ratio can reach 48.5 without any anatase TiO2. In the epoxidation of 1-hexene with H2O2 as an oxidant, the conversion of alkene over the synthesized TS-1 was improved by 8.01% compared to the traditional TS-1 (18.11% vs. 10.10%). The high-efficiency strategy reported in this paper will provide new opportunities for further promoting the industrial application of TS-1 zeolite.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 6
·1-16
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IF 2.4
Li Tong,Liu Fuliang,Wang Xiaofang,Han Zhaohao,Jia Xiaoqiong,Wang Ping,Chu Qingyan,Sheng Yuxuan
The precise embedding of metal species within specific sites of zeolite frameworks and their unique microenvironments exert fascinating influences on catalytic performance. Herein, we report the rational design of a highly efficient Co-Cu@CTS-1 catalyst through the strategic incorporation of Co, Cu, and Ce into TS-1 zeolite, where Ce is doped at silicon atomic sites while Co and Cu are encapsulated within the zeolite cages. Mechanistic investigations reveal that the synergistic interplay among Co, Cu, and Ce is pivotal for catalytic activity: Co facilitates molecular oxygen activation to generate reactive oxygen species (O⁻), while Ce(III) enhances oxygen vacancy concentration, significantly boosting styrene conversion. Moreover, the distinctive electronic interaction between Ce and Cu markedly improves the selectivity toward styrene oxide. The optimized Co-Cu@CTS-1 catalyst exhibits exceptional performance in the aerobic epoxidation of styrene, achieving a remarkable conversion of 78.11% with 87.31% epoxide selectivity under mild conditions (80 °C, 2 h). Furthermore, the catalyst demonstrates outstanding stability, retaining 68.21% conversion even after 20 reaction cycles, underscoring its superior resistance to metal sintering and long-term durability. This work provides valuable insights into the rational design of multifunctional zeolite catalysts through precise metal positioning and microenvironment modulation. Graphical
研究领域:
催化化学
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材料科学
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环境化学
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
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2019
·Vol. 150
·期 6
·1641-1649
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IF 2.372
Luo Qianqian,Lu Tianliang,Xu Jun,Yang Xiaomei,Zhou Lipeng
Abstract Methyl pyruvate (MPA) was synthesized from dihydroxyacetone (DHA), the oxidation product of glycerol, over Sn-β and TS-1 hybrid molecular sieves at low temperature. Sn-β and TS-1 provide the active sites for conversion of DHA to methyl lactate (MLA) and oxidation of MLA to MPA, respectively. Synergism of Lewis acid sites on Sn-β and TS-1 realize the production of MPA from DHA. After optimization, 71% yield of MPA can be obtained under 50 °C. This is the first report for the synthesis of MPA from DHA directly. Graphic Abstract
研究领域:
催化
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绿色化学
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化工
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 16
·7810-7818
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IF 3.3
Yanke Guo,Qiaoyun Qin,Jing Zhu,Baohe Wang
Propylene glycol methyl ether was directly synthesized from propylene and hydrogen peroxide under mild conditions via aluminum modified titanium silicalite-1 as a bifunctional catalyst. It has both active sites capable of epoxidation and active sites capable of ring opening reactions, thus realizing the one-pot preparation of propylene glycol methyl ether by propylene. The synergistic effect of Ti–Al on the catalytic performance and the distribution of propylene glycol methyl ether isomer were investigated in detail, and the synergistic catalysis between the two active sites was characterized. The gradual introduction of aluminum reduced the activation ability for hydrogen peroxide, but gradually increased the selectivity for propylene glycol methyl ether. Under the optimum conditions, the selectivity for propylene glycol methyl ether reached 91.53%. Combined with Density Functional Theory (DFT) calculations, the synergistic catalytic effect of doped Al and framework Ti in titanium silicalite-1 is discussed in detail from a microscopic perspective. Al increases the Lewis acid strength of Ti active sites and promotes the conversion of propylene to propylene oxide (PO), and simultaneously Ti increases the Brønsted acid strength of Al active sites and promotes the conversion of propylene oxide to propylene glycol ether.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2013
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IF 3.41
Cheng Liu,Jiale Huang,Daohua Sun,Yao Zhou,Xiaolian Jing,Mingming Du,Haitao Wang,Qingbiao Li
Anatase type extra-framework titanium in titanium silicate-1 (TS-1) molecular sieves has been observed to cause adverse catalytic impediments such as carbon–carbon bond cleavage and low H 2 O 2 efficiency during the epoxidation of terminal alkenes. In this study, a series of TS-1 sieves were synthesized, and used as catalysts for styrene epoxidation. Among the catalysts, the TS-1 with a Si/Ti molar ratio of 35 and 0.21 mol% of anatase type extra-framework titanium exhibited the best styrene conversion and styrene oxide (SO) selectivity. The results suggests that, framework Ti species have no effect on the stabilization of SO selectivity, whereas the synergetic interaction between the framework Ti species and the anatase type extra-framework titanium is essential for the outstanding catalytic performance of TS-1 in styrene epoxidation. In addition, our results demonstrate that the usage of tetraethyl orthosilicate (TEOS), tetrabutyl titanate (TBOT), and isopropyl alcohol in the synthesis of TS-1 does not guarantee the absence of extra-framework Ti species. Instead, the asynchronous degrees of hydrolysis between TEOS and TBOT might account for the formation of the anatase type extra-framework titanium. The influence of H 2 O 2 amount, reaction temperature and time, as well as the types of solvent, oxidant, and catalyst amount, on the catalytic performance of TS-1 with anatase type extra-framework titanium was likewise investigated.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2017
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IF 6.216
Guoqiang Wu,Zhengguo Lin,Liang Li,Lei Zhang,Yanping Hong,Wenjun Wang,Chao Chen,Yan Jiang,Xianzai Yan
An efficacious approach to improve the catalytic performance of titanium silicalite-1 (TS-1) catalysts in epoxidation of allyl chloride with hydrogen peroxide has been developed. A series of modified TS-1 catalysts were prepared by corroding the classic TS-1 catalyst with different concentrations of tetrapropyl ammonium hydroxide (TPAOH) under controlled conditions. The resultant catalyst samples were characterized by XRD, ICP, N 2 -adsorption, FT-IR, UV–vis, SEM and TEM. The catalytic activity of the modified TS-1 catalysts is significantly improved, which could be attributed to the increase of the mesopore volume and pore diameter and decrease of the diffusion limitation but without obvious changes of the framework structure, framework Ti content, the outer surface shape and crystal size of the modified TS-1. Furthermore, the kinetics of the epoxidation of allyl chloride over TS-1-0.05 catalyst was also systematically studied, the apparent orders of reaction with respect to H 2 O 2 and allyl chloride are 0.68 and 0.62, respectively, and the activation energy of the epoxidation reaction on the TS-1-0.05 catalyst is 57.4 kJ mol −1 .
研究领域:
化学工程
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催化科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2025
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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.
研究领域:
材料科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
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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DOI
高影响因子
CATALYSIS TODAY
·
2025
·
IF 5.3
Yupeng Tian,Yujia Liu,Shoutao Ma,Wei Xu,Chenyang Zhao,Bing Sun
This study introduces a heart-like micromixer reactor and Au/TS-1 catalyst to address the dual challenges of safety and efficiency in gas-phase propylene epoxidation using H 2 and O 2 . Conventional methods face inherent explosion risks and rapid catalyst deactivation due to sintering and coking. The microreactor architecture achieves over 99% flame-quenching efficiency via sub-millisecond radical suppression and enhanced heat transfer, enabling safe operation with minimal inert gas dilution (N 2 < 70 vol%). Coupled with alkali-promoted Au/TS-1 catalysts, the system sustains > 90 % propylene oxide (PO) selectivity for 500 h, outperforming static mixers where activity halved within 100 h. This work pioneers a reactor-catalyst co-design strategy, decoupling safety constraints from reaction efficiency, and establishes a scalable platform for sustainable PO synthesis. Besides, the critical gaps in industrial-scale implementation of explosive gas-phase reactions is bridged.
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DOI
高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2026
·
IF 3.5
Jiaojiao Yu,Yi Zuo,Gudan Li,Bosong Zhang,Hong Yang,Xinyue Wang,Xinwen Guo
PO 4 3- assists the one-step synthesis of highly active TS-1 containing Ti-VI species. • PO 4 3- induces plate-like TS-1 morphology and creates hierarchical micropores. • Ti-VI is constructed by Ti-O-PO 4 x- intermediate from bonding of Ti-OH with PO 4 3- . • TS-MAP-0.2 doubles the activity for 1-hexene epoxidation than additive-free TS-1. Titanium silicalite-1 (TS-1) is an efficient and green oxidation catalyst that has been employed in various industrial processes. In our previous work, a highly active TS-1 catalyst bearing Ti(OSi) 2 (OH) 4 (Ti-VI) was successfully prepared via post-treatment with alkaline solutions. Herein, a novel synthesis strategy is developed using monoammonium phosphate (MAP) as a regulator to fabricate thin TS-1 crystals with Ti-VI species, eliminating the complicated post-treatment operations. The study reveals that although the added phosphate anion (PO 4 3- ) is not incorporated into the MFI framework, it significantly affects the crystallization behavior of TS-1 during the synthesis. Essentially, PO 4 3- exerts two functions. First, it regulates the Ti species in the resulting TS-1 by forming Ti-O-PO 4 x - intermediates which not only promotes the formation of Ti-VI but also the construction of large micropores (0.7−0.8 nm) around Ti atoms in TS-1. Furthermore, PO 4 3- induces the formation of plate-like crystal morphology of TS-1. The obtained TS-1 catalyst exhibits remarkably enhanced catalytic performance in 1-hexene epoxidation, which is ascribed to the concurrent o ptimization of its intrinsic catalytic activity and mass transfer diffusion properties. Download: Download high-res image (354KB) Download: Download full-size image
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DOI
高影响因子
CATALYSIS LETTERS
·
2026
·Vol. 156
·期 7
·196
·
IF 2.5
Cai Chang,Li Jinhong,Li Rongwu,Zhao Nan,Zhang Yue,Fan Qiuyu,Zhang Jianguo,Chen Lidong
This study addresses the limitations of conventional industrial methods for acetophenone (AP) production by developing a modified TS-1 zeolite catalyst with a predominantly interparticle micro-mesoporous architecture for the selective oxidation of ethylbenzene (EB) under mild and environmentally benign conditions. To overcome the intrinsic pore constraints of TS-1 zeolite that restrict substrate accessibility and mass transfer, a specific sequential acid-then-alkali post-treatment strategy followed by cobalt oxide impregnation was employed. This treatment sequence leads to surface enrichment of framework-like Ti species and the creation of interparticle mesoporosity, resulting in a coexisting micro-mesoporous architecture while preserving the MFI framework. Under optimized reaction conditions, the catalyst achieved 76.2% EB conversion and 74.8% AP selectivity to AP. Systematic evaluation in the EB/H 2 O 2 oxidation system under acidic reaction conditions revealed a synergistic effect between framework titanium active sites and cobalt oxide active species. The developed catalyst offers distinct advantages, including straightforward synthesis procedure, high catalytic activity, and facile recoverability. Graphical This study constructs a micro-mesoporous TS-1 via specific sequential acid-then-alkali modification and loads optimal Co 3 O 4 to create dual active centers. This architecture reduces mass transfer resistance and optimizes active sites, enabling efficient ethylbenzene oxidation to acetophenone under mild conditions. The catalyst is easily recoverable, regenerable, and stable. The alternative text for this image may have been generated using AI.
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高影响因子
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