INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Rui Feng,Zhou Fang,Runxi Zhang,Xiaoyan Hu,Tianbo Li,Wei Zhou,Feifei Yang,Xinlong Yan,Shijian Lu
Direct hydroxylation of benzene to phenol is a more environmentally friendly way to generate phenol compared with the traditional method. This study developed vanadium-modified hollow-structured titanium silicate-1 (TS-1) as a catalyst for the effective hydroxylation of benzene to phenol under moderate conditions using hydrogen peroxide as an oxidant. The synthesis of TS-1 zeolites has been improved using traditional hydrothermal, crystal seed, and dissolution–recrystallization techniques. Compared with conventional TS-1, hollow-structured TS-1 exhibited a higher mesopore volume and surface area. Later, vanadium doping increased the charge density associated with the framework Ti centers and acid site content. In the radical reaction process, the adsorption and activation of benzene on highly reactive Ti–OOH intermediates, as well as the improvement of performances toward benzene hydroxylation to phenol, were facilitated by the increase in the concentration of open active centers and acid and electron characteristics.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Chenyang Zhao,Yujia Liu,Yupeng Tian,Yahui Li,Junjie Feng,Wei Xu,Ning Shi,Zhe Yang,Bing Sun
Direct epoxidation of propylene (C 3 H 6 ) with hydrogen (H 2 ) and oxygen (O 2 ) over Au/TS-1 catalyst was promising way for the synthesis of propylene oxide (PO). However, high selectivity of PO (>95 %) and conversion of C 3 H 6 (>5 %) cannot be achieved at the same time. The industrialization process was severely restricted. In this paper, Au/TS-1 catalysts were synthesized by deposition precipitation method with alkali metal promoter. And alkaline gases and silane coupling post-treatment were performed to promote the catalytic activity. The prepared samples exhibited a much better C 3 H 6 conversion (6.5 %) and PO selectivity (95.1 %) compared with general catalyst using normal synthetic technology. Cs 2 CO 3 was beneficial to increasing Au nanoparticles uptake efficiency. Both NH 3 and triethoxyvinylsilane post-treatment were good for smaller and more uniform loading of Au nanoparticles. The decreasing in surface hydroxyl density effectively alleviated the occurrence of PO ring opening isomerization. The increased hydrophobicity of TS-1 surface was conducive to the rapid desorption of generated PO and significantly increased PO selectivity. Multiple pretreatment was also favorable for extending the lifetime of Au/TS-1 catalyst.
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
·
催化科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Rui Feng,Zhou Fang,Wei Wang,Tianbo Li,Xiaoyan Hu,Xinlong Yan,Zhongdong Zhang
Direct hydroxylation of benzene to phenol is an environmentally friendly strategy to produce phenol compared with the conventional process. In this work, vanadium-modified titanium silicate-1 (TS-1) with enhanced Lewis acid and charge density were prepared as catalysts for efficient hydroxylation of benzene to phenol in the presence of hydrogen peroxide as an oxidant under mild conditions. The hierarchical TS-1 zeolites with a high framework Ti content were synthesized in the presence of NH4HCO3, and then vanadium doping was used to change the acidity and charge density. It was found that NH4HCO3 favored the titanium substitution of framework sites and nanocrystal stacking of TS-1. Vanadium doping increased the amount of Lewis acid sites and the charge density associated with the framework Ti. The enhancement in acid and electron characteristics boosted the intrinsic catalytic reactivity of Ti-OOH species, which further improved the performances toward benzene hydroxylation. The presented strategy and mechanistic results clarified the relationship between the structure and acidity in TS-1 zeolite. It was also verified that hydroxyl radicals (•OH) rather than superoxide radicals (•O2–) were the reactive agents responsible for the consecutive selective oxidation of benzene.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhuwei Yang,Linsen Li,Xiao Yang,Hui Xiong,Riguang Zhang,Zhao Jiang
In this study, a series of Ni-CeO 2 /TS-1 (Titanium Silicalite-1) catalysts were synthesized for dry reforming of methane (DRM). Among them, 5Ni-10CeO 2 /TS-1 exhibited the highest catalytic performance with 89 % CH 4 and 93 % CO 2 conversions, 4.81 mol CH4 ·g Ni -1 ·h −1 and 4.99 mol CO2 ·g Ni -1 ·h −1 specific activities, 95.5 % H 2 /CO ratio after 50 h, accompanied by the good stability with 2.9 % CH 4 and 2.3 % CO 2 activity loss within 100 h. Combined with various characterizations, the structure–function relationship was also investigated. For the physical and morphological analysis, it was indicated that the appropriate CeO 2 content could effectively diminish, disperse the Ni nanoparticles, and maintain MFI backbone structure. For the electronic structure, the introduced CeO 2 could improve the amount and strength of the surface Ni-O-X (Ti or Ce) species by changing the interaction among Ni nanoparticles, TS-1 and CeO 2 . It led to more Ni nanoparticles in stronger electron-deficient state, as well as more medium-strength basic sites, favoring for the activation of CH 4 and CO 2 . However, Ni nanoparticles would be covered when excessive CeO 2 was introduced, preventing the exposure of the active sites. Therefore, only the suitable CeO 2 in the catalysts could significantly improve catalytic performance for DRM with long-term stability. Furthermore, the good anti-sintering and anti-coking properties of 5Ni-10CeO 2 /TS-1 were mainly dependent on the optimal amount of surface Ni-O-X species with high strength. In-situ DRIFTS (diffuse reflectance infrared spectroscopy) analysis demonstrated that the introduced CeO 2 could help catalyst favor for activating CH 4 and CO 2 molecules, and inhibiting the CH 4 overcracking and carbon accumulation, confirmed by the long-term measurement and structure analysis of spent catalysts.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ChemistrySelect
·
2022
·Vol. 7
·期 35
·e202202475
·
IF 2.307
Zhiqiang Zhang,Qingyan Chu,Yuan Sun,Hao Wang,Deming Lu,Yuying Liu,Haibin Xiao,Ping Wang,Hongyou Cui,Ming Wang
Graphical The hierarchical TS-1 with abundant mesopores was prepared by TPAOH/TIPA treatment, which was applied to the reaction of the ammoximation-oxidation of acetone to 2-nitropropane. Hierarchical TS-1 catalyst performed excellent reusability and catalytic activity with 97.5 % conversion and 96.8 % selectivity. The novel technology for clean and mild synthesis of nitroalkanes has been developed. Modified TS-1 catalysts for the acetone ammoximation-oxidation reaction were prepared by post-treating TS-1 with different concentrations of TPAOH/TIPA, and the effects of alkali treatment on the catalytic performance were systematically investigated. The techniques such as XRD, SEM, TEM and N 2 sorption were used to characterize the catalyst samples, which exhibited that the introduction of alkali increased the volume and quantity of mesopores, while there was no obvious influence on the framework structure and titanium content in the framework. And the improvement in catalyst performance after alkali treatment was attributed to the increase of mesopores and the decrease in diffusion limitation. In addition, three common ammoximation catalysts (Ti-MOR, Ti- MWW and TS-1) were systematically investigated in this reaction. Ti-MOR showed superiority in the ammoximation to oxime, while TS-1 displayed the best catalytic performance in the ammoximation oxidation of ketones to nitroalkanes. It was indicated that modified TS-1 could be a promising catalyst for the ammoximation-oxidation reaction of acetone.
研究领域:
催化化学
·
绿色合成
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS RESEARCH BULLETIN
·
2024
·
IF 5.3
Lei Cai,Xiu Gao,Peihang He,Beining Luo,Xianzai Yan,Zedong Zhang,Wenjun Wang,Guoqiang Wu
To improve the catalytic epoxidation activity of conventional TS-1 zeolite under acid-free conditions, a series of TS-1-supported zinc ( x Zn/TS-1) catalysts were prepared and evaluated in the epoxidation of 1-hexene and methyl oleate (MO) with H 2 O 2 oxidant. The microstructure of x Zn/TS-1 was investigated using various characterization techniques, and the results showed that the introduction of Zn species was not only well dispersed on the surface of TS-1 but also did not disrupt the crystal structure of TS-1 and tetrahedral framework titanium. Furthermore, the Ti-O-Zn structure can be formed between Zn and Ti species through O-atomic coordination, which improves the vulnerability of the Ti-O bond to attack the H 2 O 2 molecule, and ultimately facilitates the epoxidation reaction between 1-hexene and MO. In addition, the 2% Zn/TS-1 catalysts showed optimal conversions of 45.7 % and 75.41 % for 1-hexene and MO, respectively, and exhibited good catalytic stability and regeneration during the epoxidation process.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2023
·Vol. 17
·期 6
·772-783
·
IF 4.5
Gao Xiu,Luo Beining,Hong Yanping,He Peihang,Zhang Zedong,Wu Guoqiang
Development of a titanium silicalite-1 (TS-1) catalyst with good crystallinity and a four-coordinate Ti framework is critical for efficient catalytic oxidation reaction under mild conditions. Herein, a size-controlled TS-1 zeolite (TS-1#0.1ACh (acetylcholine)) was synthesized via steam-assisted crystallization by introducing acetylcholine as a crystal growth modifier in the preparation process, and TS-1#0.1ACh was also employed in epoxidations of different substrates containing C=C double bonds. The crystalline sizes of the as-synthesized TS-1#0.1ACh catalysts were controlled with the acetylcholine content, and characterization results showed that the particle sizes of highly crystalline TS-1#0.1ACh zeolite reached 3.0 µm with a good Ti framework. Throughout the synthetic process, the growth rate of the crystals was accelerated by electrostatic interactions between the connected hydroxyl groups of the acetylcholine modifier and the negatively charged skeleton of the pre-zeolites. Furthermore, the TS-1#0.1ACh catalyst demonstrated maximum catalytic activity, good selectivity and high stability during epoxidation of allyl chloride. Importantly, the TS-1#0.1ACh catalyst was also highly versatile and effective with different unsaturated substrates. These findings may provide novel, easily separable and large TS-1 catalysts for efficient and clean industrial epoxidations of C=C double bonds.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Weilong Hou,Kehang Lin,Xiangyu Zhang,Bowen Xu,Yuexia Wang,Xinqing Lu,Yijing Gao,Rui Ma,Yanghe Fu,Weidong Zhu
Nonoxidative propane dehydrogenation (PDH) has been regarded as an economic and efficient route to meet constantly increasing global demands for propylene. However, over industrially applied catalysts, thermally induced deactivation including coke formation and sintering of the active species occurs and simultaneously hydrocarbon cracking significantly reduces the selectivity for propylene. In the present work, titanosilicate-1 (TS-1) zeolite supported catalysts (Pt/TS-1) were developed for PDH. The results on the extensive characterizations of the prepared materials, in combination with density functional theory (DFT) calculations, verify that the framework Ti species in Pt/TS-1 can increase the dispersion and electron density of Pt, which significantly enhances the catalyst stability and selectivity for propylene. Utmost importantly, no sintering of the Pt active species in Pt/TS-1 occurs at the high temperatures required for the reaction and catalyst regeneration processes. Therefore, the current investigation provides a strategy for developing efficient PDH catalysts for practical applications.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2018
·
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
·
绿色化学
·
材料科学
·
工业化学
·
有机合成
·
环境友好工艺
·
能源与资源工程
✓ 已验证
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
·
催化化学
·
材料科学
·
化学工程
·
储能技术
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2025
·Vol. 15
·期 7
·694
·
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
·
化学工程
·
材料科学
·
多相催化
·
绿色化学
✓ 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）