CATALYSIS TODAY
·
2021
·
IF 6.766
Hai Wang,Liang Wang,Dong Lin,Xiang Feng,Xuefeng Chu,Lina Li,Feng-Shou Xiao
In situ release of hydrogen from liquid organic hydrogen carriers―such as methanol by steam reforming, offers a feasible way to potentially solve the problem of hydrogen storage and transport. Here we report that the titanosilicalite-1 (TS-1) zeolite support efficiently accelerates the Pt catalyzed methanol steam reforming (MSR), giving the hydrogen productivity at 639.7 mol H2 mol Pt −1 h −1 at 250 °C, which steadily outperforms the Pt nanoparticles supported on other carriers, including ZSM-5 zeolite, amorphous SiO 2 , and TiO 2 anatase. Further studies reveal that the electronic metal-support interactions (EMSIs) between Pt and TS-1 zeolite occurs, which modifies Pt nanoparticles surface charge state to accelerate the reaction. More importantly, the interactions could stabilize the Pt nanoparticles, achieving sinter-resistant Pt/TS-1 catalyst in the continuous MSR tests. This finding indicates the important role of heteroatoms in the zeolite framework for supported metal nanoparticles, which open a new way to guide the design of highly efficient heterogeneous catalysts in the future.
研究领域:
催化化学
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材料科学
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能源化学
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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
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环境化学
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产品关联
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
·
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
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催化化学
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产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2025
·
IF 4.2
Yu-Le Wang,Songhai Wu,Yu-Zhen Xu,Yu-Dong Shan,Yong Liu,Xu Han
The selective oxidation of cyclohexene (Cy) to cyclohexene oxide (Cy-ep) using O2 remains challenging due to low epoxidation selectivity. In this work, a series of Mo-doped TS-1 (Mo-TS-1) catalysts were successfully synthesized for the epoxidation of Cy under solvent- and initiator-free conditions with O2 as the oxidant. Among them, 5Mo-TS-1 exhibited high catalytic performance, achieving 43.5% Cy conversion and 50.6% selectivity toward Cy-ep. Additionally, valuable byproducts such as 2-cyclohexen-1-ol (Cy-ol) and 2-cyclohexen-1-one (Cy-one) were obtained with yields of 28.0% and 21.4%, respectively. Since both Cy-ol and Cy-one are valuable intermediates in fragrance synthesis, over 43.5% of Cy was effectively converted into high-value products. Quenching experiments and Raman spectroscopy revealed that surface oxygen vacancies (Ov) facilitate the activation of O2 to form ≡Ov‑superoxo species, which abstract hydrogen from the allylic C-H bond of Cy to generate 3-cyclohexenyl radicals (Cy•). These radicals subsequently react with O2 to form Cy-OO•, followed by hydrogen abstraction from another Cy molecule to yield 2-cyclohexene-1-hydroperoxide (Cy-OOH). A positive correlation between Cy-OOH and Cy-ep formation underscores the critical role of Cy-OOH in the epoxidation process. Furthermore, Raman spectroscopy confirmed the presence of ≡Mo-(η2-O2) peroxo species on the catalyst surface, which preferentially attack the C=C bond of Cy to form Cy-ep. DFT calculations elucidated two distinct O2 activation pathways: In Pathway I, O2 is activated at Ov sites to form ≡Ov‑superoxo, which subsequently reacts with Cy to generate ≡Ov‑peroxo, Cy-OOH, and Cy•. In Pathway II, Mo(V/VI) sites either directly activate O2 or react with peroxo intermediates (≡Ov‑peroxo or Cy-OOH) to form ≡Mo-(η2-O2). This species selectively epoxidizes the alkene bond in Cy to Cy-ep. Notably, the direct activation of O2 at Mo(V/VI) sites bypasses the allylic oxidation route, thereby enhancing the epoxidation selectivity beyond the theoretical limit of 50.0%. This study provides new insight on the importance of surface superoxo and peroxo mediated by Ov and Mo(V/VI) in the epoxidation processes.
研究领域:
催化化学
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材料化学
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绿色化学
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多相催化
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氧化反应
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产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2025
·Vol. 19
·期 8
·1-11
·
IF 4.5
Zhang Yingqi,Chen Chao,Xie Enxue,Hu Mengping,Fu Guoying,Wang Yan,Li Liang,Yan Xianzai,Zhang Zedong,Wu Guoqiang
Microporous and mesoporous silicalite-1 (S-1) and titanium silicalite-1 (TS-1) zeolite supported molybdenum (Mo) catalysts were synthesized and applied in the transesterification of Jatropha seed oil (JO) to produce biodiesel. Various analytical results have revealed that the MoO 3 species are highly dispersed on their surface without destroying the zeolite framework and pore structure. Compared with the mesoporous 7Mo/mesoporous S-1 and 7Mo/mesoporous TS-1 catalysts, the microporous 7Mo/S-1 and 7Mo/TS-1 catalysts exhibit high Mo species contents and surface acidity, indicating that Mo species can enter the inner surface of mesoporous zeolites. However, the Mo species on the outer surface of catalysts are only activity centers owing to the accessibility between the Mo species and JO. Therefore, compared with the low activity of the S-1 and TS-1 catalysts, the 7Mo/S-1 catalyst exhibited the highest catalytic performance, with a JO conversion of 95.7% and a biodiesel selectivity of 99.9%. Finally, 7Mo/S-1 demonstrated good catalytic stability, regeneration performance and broad substrate versatility, and the fuel properties of the as-synthesized biodiesel conformed to the current international standard. The influence of the pore structure and Mo species on the catalytic activity has been clarified, providing a theoretical and practical foundation for developing efficient heterogeneous catalysts for biodiesel production.
研究领域:
化学工程
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催化科学
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可再生能源
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Shuxin Zhang,Kun Liu,Shuyuan Yu,Zifeng Lin,Yu Xie,Yanbin Jiang,Longfu Wei,Changlin Yu
Traditional propylene oxide (PO) production processes consume large amounts of organic feedstock and release hazardous by-products. The synthesis of PO via the epoxidation of propylene using O 2 is an ideal route offering 100% atomic economy. However, achieving high selectivity and high efficiency under mild conditions remains a significant challenge. In this study, we have developed a visible-light-driven tandem reaction system combining a carbon- and oxygen-co-doped three-dimensional spherical indium sulfide (C,O-In 2 S 3 ) photocatalyst with titanium silicate molecular sieve (TS-1), thereby achieving the distinctly selective oxidation of propylene at ambient temperature. Assembled from ultra-thin nanosheets, the three-dimensional structure of C,O-In 2 S 3 provides abundant active sites and mass transfer space, with carbon‑oxygen co-doping narrowing the bandgap and enhancing visible light absorption. In a pure water system, the H 2 O 2 yield of C,O-In 2 S 3 reached 1450.40 μmol·g −1 ·h −1 , which is 17.8 times that of pristine In 2 S 3 . Utilizing the excellent compatibility of the methanol/water system, the photocatalytic generated H 2 O 2 was directly employed in the TS-1-catalysed epoxidation of propylene, achieving a PO yield of 2230.03 μmol·g −1 within 2 h with a selectivity of 99.1%. This work applies sulfide-based photocatalysts to a tandem reaction involving photocatalytic H 2 O 2 production and propylene epoxidation, providing a new strategy for the green, safe and efficient synthesis of PO.
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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
Catalysts
·
2026
·Vol. 16
·期 5
·417
·
IF 4.5
Ziyan Mi,Huayun Long,Yuhua Jia,Yue Ma,Cuilan Miao,Yan Xie,Xiaomei Zhu,Jiahui Huang
Developing effective catalysts for the epoxidation of propylene with H2and O2holds significant scientific and industrial significance. This study synthesized a series of Au/TS-1 catalysts modified with alkali metals (Na+, Cs+) and carefully examined their impact on gas-phase propylene epoxidation, with particular attention to the role of anions. The optimal Au–CsC(1:10)/TS-1 catalyst (Cs2CO3modified, Au/Cs molar ratio = 1:10) achieves a propylene conversion of 16.8%, a PO selectivity of 88.5%, an H2efficiency of 40.8%, a record PO formation rate of 383.9 gpo·kgcat−1·h−1, and unprecedented long term stability (>380 h without deactivation). To the best of our knowledge, no previous study has simultaneously achieved such balanced and outstanding performance across all these key indicators. Comprehensive characterization reveals that Cs+modification suppresses side reactions and coke formation, increases microporosity, tunes surface acid–base properties and hydrophobicity, restricts Au particle size, and stabilizes both Au0and tetra coordinated Ti sites, thereby inhibiting H2O2decomposition and PO isomerization while greatly enhancing reaction efficiency. This holistic advancement represents a significant leap forward for Au based catalysts in gas phase propylene epoxidation, offering both a theoretical foundation and practical guidance for the development of high performance epoxidation catalysts.
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Huimin Li,Bin Wu,Zhimin Zhu,Chenyang Li,Zhihan Liu,Fuweng Zhang,Huidong Zheng,Longfei Yan
Ethylene sulfate (DTD) is a new type of solid electrolyte interphase (SEI) film-forming additive for lithium-ion batteries. DTD was typically synthesized in the industry by oxidation of ethylene sulfite (ES) with NaClO via a RuCl 3 -catalyzed reaction. However, this route generates significant amount of Cl-containing wastes, and the recovery of RuCl 3 is costly and technically challenging. Herein, we present a green and heterogeneous route for synthesizing DTD from ES, utilizing the Titanium Silicalite-1 (TS-1) and H 2 O 2 as catalysts and green oxidants, respectively. Our research reveals that the tetra-coordination framework of Ti in TS-1 serves as the main active site for the oxidation of ES, achieving a remarkable yield of DTD up to 92 % under optimized reaction conditions. Additionally, we developed a continuous green oxidation process for synthesizing DTD from ES, which is the first of its kind and has been successfully operated continuously for over 300 h. This work provides a cost-effective, green, and efficient route for synthesizing DTD from ES.
研究领域:
绿色化学
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催化化学
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材料科学
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化学工程
·
储能技术
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）