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
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Shuai Li,Tianxiang Yang,Wenlian Wang,Jing Lu,Xiaoyang Zhao,Weizhen Fan,Xiaoxi Zuo,Junmin Nan
2-thiophene sulfonamide (2-TS) is demonstrated as a multi-functional additive to functionalize the electrolyte and improve the performances of LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811)/graphite batteries . Compared with the batteries without 2-TS, the performances of batteries with 2-TS containing electrolyte are significantly improved at wide temperature and high cut-off charge voltage of 4.40 V (vs. Li/Li + ）. After 500 cycles at room temperature and in the voltage range of 2.80–4.20 V, the batteries with 1% 2-TS and without 2-TS additive lose 8.40% and 23.59% initial discharge capacity, respectively. At an elevated temperature of 45 °C and in the voltage range of 2.80–4.40 V, the cycle performance of the batteries with 1% 2-TS is also enhanced, i.e., 68.68% initial discharge capacity is remained after 115 cycles, while the batteries without 2-TS has already decayed to the lifespan point. It is shown that 2-TS molecules can both consume the H 2 O/HF residues to alleviate the decomposition of LiPF 6 and preferentially react on the electrodes to form uniform and dense low-resistance films. These results demonstrate this electrolyte can effectively improve the battery performances and has promising prospects applying in high-voltage and high-nickel NCM-based batteries.
研究领域:
材料科学
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电化学
·
能源存储
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2013
·
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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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
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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产品关联
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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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
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
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 LETTERS
·
2024
·Vol. 154
·期 7
·3787-3797
·
IF 2.3
Han Zhaohao,Chu Qingyan,Wang Hao,Jia Xiaoqiong,Jiang Peng,Li Tong
We successfully synthesized a bifunctional alkaline catalyst (Co@CTS-1), on the one hand, which demonstrates exceptional catalytic performance in the aerobic oxidation of alkenes, particularly in the epoxidation of styrene, in the absence of both an initiator and a co-reducing agent, achieving a conversion rate of 74.94%, a selectivity of 71.84% for styrene oxide; on the other hand, the catalyst maintained its high activity throughout a cyclic reaction run lasting up to 2500 min, demonstrating exceptional stability in the epoxidation of styrene. The Co@CTS-1 catalyst utilizes TS-1 as the carrier, and it is modified with cobalt and cerium elements. Through the embedding of cobalt elements within the TS-1 cage, the catalyst gains the ability to activate O 2 , and by inserting cerium elements into the atomic positions of silicon, the conversion rate is further enhanced. This encapsulated structure stabilizes cobalt nanoparticles, overcoming the short lifespan issues caused by sintering and leaching in conventional supported catalysts. This work provides practical clues for the development and application of novel catalysts, and will inspire the advancement of olefin air epoxidation. Graphical
研究领域:
催化化学
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材料科学
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化学工程
·
无机化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wei Du,Zhihua Zhang,Jundi Wang,Nan Song,Xuezhi Duan,Xinggui Zhou
Propylene epoxidation by H 2 and O 2 to propylene oxide (HOPO), as a novel method for PO production, has attracted widespread attention due to its economic and environmental advantages. Acrolein is a notable byproduct arising in HOPO reaction over Au/TS-1 catalyst, and is traditionally thought to be exclusively formed on Au site through propylene oxidation. However, on the intraporous and external surface Au sites of Au-Ti catalysts, the HOPO reaction have been shown to proceed by different mechanisms, yet the effect of active sites distribution on acrolein formation is far from being understood. Herein, we found that the reaction orders in acrolein formation on Au/TS-1 catalyst (H 2 , 0.19; O 2 , 0.44; C 3 H 6 , 0.44) relative to Au/TS-1 with blocked pores (Au/TS-1-B) catalyst (H 2 , −0.36; O 2 , 0.61; C 3 H 6 , 0.52) were quite different, suggesting a variation in the reaction pathway on the catalysts with different Au locations. Moreover, it is found that PO can be converted to acrolein by O 2 on TS-1 zeolite, which is absent on TS-1-B zeolite without micropores. Consequently, acrolein formation on Au/TS-1 catalyst can proceed through two parallel pathways: propylene hydro-oxidation on Au site, and PO conversion by O 2 inside micropores. Furthermore, by designing and preparing the Au/TS-1 catalysts with different structures, the Au locations are closely related to acrolein formation mechanism and kinetic behaviors. This work provides kinetic insights into the acrolein formation pathways in the HOPO reaction on Au/TS-1 catalyst, and is helpful to the rational design and preparation of efficient catalysts with high selectivity.
研究领域:
催化化学
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材料科学
·
环境化学
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DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2026
·
IF 7.8
Zicong Wang,Jing Zhao,Weijiong Dai,Linquan Li,Yan Wang,Jiajun Zheng,Ruifeng Li
The fabrication of hierarchical zeolite structure and rational modulation of Ti active sites in TS-1 zeolite are both recognized as critical factors for improving catalytic performance in selective oxidation reactions. Herein, we propose a facile and cost-effective strategy combined a dry-gel conversion (DGC) method with a preliminary aging step for the direct synthesis of anatase-free hierarchical TS-1 zeolite containing highly active TiO 6 species. The coordination states of Ti species in TS-1 zeolites were thoroughly investigated via UV–vis, FTIR, XPS and UV-Raman spectroscopy. Additionally, systematic characterizations were performed to investigate the impacts of the synthetic strategy on the crystallization process, including the formation of hierarchical TS-1 zeolite structure and the modulation of Ti species coordination. The obtained TS-1 zeolite demonstrated exceptional catalytic activity and stability in olefin epoxidation and oxidative desulfurization reactions. This discovery not only advances the design and synthesis of titanosilicate zeolites but also expands their potential applications in various selective oxidation processes.
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Guoqing An,Chang'an Wang,Hongyi Gao,Ge Wang,Yibin Luo,Zhiyuan Liu,Changjiu Xia,Siqi Liu,Xinxin Peng,Zhixiang Cheng,Xingtian Shu
Titanosilicate-1 zeolites (TS-1) as one of the most commonly used catalysts for alkene epoxidation , construction of hierarchical pores as well as elimination of anatase to promote mass transportation and avoid invalid decomposition of hydrogen peroxide are always desirable yet challenging goals. Here, a novel and unique Ti-based metal organic frameworks (MOFs)-induced synthetic strategy for fabricating anatase-free hierarchical TS-1 was first proposed. All the components of MOFs perform different functions: the uniformly distributed Ti nodes replace conventional tetrabutyl titanate (TBOT) to serve as sole Ti source for constructing zeolite crystal; the separated ligands can be embedded in the zeolite framework and act as template to in situ build hierarchical pore structure ; the coordination interaction between Ti nodes and ligands can efficiently avoid the anatase generation by balancing the forming rates of Ti-OH and Si-OH. This synthetic strategy is of general applicability, and two different synthetic routes including traditional hydrothermal process and steam assisted crystallization (SAC) procedure are successfully adopted. The obtained hydrothermal TS-1 and SAC anatase-free samples all possess abundant intercrystalline mesopores of 20–50 nm and even macropores between 50 and 150 nm, improving the conversion over 25 % for 1‑hexene epoxidation than TS-1 sample prepared by conventional route. The influences of the amount of Ti MOFs precursor and the crystallization process are studied in detail, and possible synthesis mechanisms are proposed. This MOFs-induced strategy might open up an avenue for the rational design of ideal and hierarchical zeolite to boost the catalytic efficiency.
研究领域:
材料科学
·
催化化学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）