Aggregate
·
2023
·Vol. 4
·期 4
·e318
·
IF 18.8
Chang'an Wang,Guoqing An,Jing Lin,Xiaowei Zhang,Zhiyuan Liu,Yibin Luo,Siqi Liu,Zhixiang Cheng,Tingting Guo,Hongyi Gao,Ge Wang,Xingtian Shu
Simultaneous achievement of constructing mesopores and eliminating anatase is a long-term pursuit for enhancing the catalytic performance of TS-1. Here, we developed an aromatic compounds-mediated synthesis method to prepare anatase-free and hierarchical TS-1 for olefin epoxidation. A series of hierarchical TS-1 zeolites were prepared by introducing aromatic compounds containing different functional groups via the crystallization process. The formation of intercrystalline mesopores and insertion of titanium into framework were facilitated at different extent. The synergistic coordination of carboxyl and hydroxyl in aromatic compounds with Ti(OH) 4 realizes the uniform distribution of titanium species and eliminates the generation of anatase. Noteworthily, eight machine learning models were trained to reveal the mechanism of additive functional groups and preparation conditions on anatase formation and microstructure optimization. The prediction accuracy of most models can reach more than 80%. Benefiting from the larger mesopore volumes (0.37 cm 3 ·g −1 ) and higher content of framework Ti species, TS-DHBDC-48h samples exhibit a higher catalytic performance than other zeolites, giving 1-hexene conversion of 49.3% and 1,2-epoxyhenane selectivity of 99.9%. The paper provides a facile aromatic compounds-mediated synthesis strategy and promotes the application of machine learning toward the design and optimization of new zeolites.
研究领域:
催化
·
化学工程
·
材料科学
·
机器学习
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Kaiwei Wang,Hao Ruan,Fumin Wang,Yi Zhai,Mingshuai Sun,Yan Chen,Jiaxing Zhang,Yihao Wang,Xuyang Zou,Xubin Zhang
The construction of abundant TiO 6 active sites within the zeolite framework is essential for further enhancing the catalytic performance of TS-1 zeolite. Here, we employ a strategy involving treatment with a mixture of amines and ammonium salts to generate abundant TiO 6 species within zeolites synthesized with the assistance of N,N-dimethylformamide (DMF). It was observed that during the post-treatment process, the presence of amines and ammonium salts plays a key role for the formation of highly active TiO 6 species. The incorporation of DMF can significantly enhance the TiO 6 content in the post-treated zeolite, increasing it to 61.5 % compared with 28.5 % in the zeolite synthesized without DMF. The effect of the DMF/SiO 2 ratio in the synthesized gel on the morphology and catalytic performance was also examined. It is noteworthy that the incorporation of DMF influences the microenvironment of the Ti active sites following post-treatment. 1 H MAS NMR analysis reveals that the characteristic peaks corresponding to Ti-OH and isolated Si-OH groups in the DMF-synthesized catalyst are significantly intensified after treatment with amines and ammonium salts. When H 2 O 2 is employed as an oxidant, the optimal catalytic performance achieves a cyclohexene conversion of 51.1 % and a cyclohexene oxide yield of 39.4 %, with a high TOF value of 92.77 h −1 . Notably, the catalyst exhibits a significantly conversion rate of 79.4 % and a yield of 72.7 % using O 2 as the oxidant.
研究领域:
催化化学
·
材料科学
·
无机化学
·
石油化工
·
绿色氧化
✓ 已验证
产品关联
DOI
高影响因子
Materials Chemistry Frontiers
·
2022
·Vol. 6
·期 15
·2072-2084
·
IF 8.683
Yi Zhai,Fumin Wang,Xubin Zhang,Guojun Lv,Zhiguo Zhu,Kaiwei Wang,Zhibo Xu,Linfang Jiang
Realizing anatase-free hollow TS-1 with a controllable titanium micro-environment via dissolution-recrystallization for diverse catalytic reactions remains a great challenge due to the insufficient comprehension of dissolution-recrystallization mechanism, high cost and environmental issues. Here, anatase-free hollow TS-1 was economically synthesized via mother-liquor-induced dissolution-recrystallization, realizing the controllable micro-environment and spatial distribution of titanium. A novel kinetic-thermodynamic co-regulatory pathway was unveiled for the first time to describe the magical reversible varying of titanium micro-environment during the dissolution-recrystallization process (dissolution-reinsertion-secondary dissolution). Thermodynamically, temperature and liquid-to-solid ratio cause the formation of anatase and unsaturated silicon, and the unsaturated silicon species (Q1 and Q2) determine the subsequent capture and re-insertion of anatase. Original unsaturated silicon species in the mother liquor endow it with a unique function to further facilitate the elimination of anatase. Kinetically, temperature determines the dynamic progress of the reversible process such as evolution speed and deposition priority of titanium and silicon species. Multi-factor dynamic constraints directly determine the micro-environment, spatial distribution and content of titanium. This provides a new perspective for predicting and synthesizing hollow heteroatomic zeolites with ideal heteroatom micro-environments. Unique surface properties and diverse titanium micro-environments endow hollow TS-1 with superior mass-transfer abilities to exhibit different activities in 1-hexene epoxidation and phenol hydroxylation.
研究领域:
催化材料
·
化学工程
·
环境科学
✓ 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
MICROPOROUS AND MESOPOROUS MATERIALS
·
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
·
材料科学
·
化学工程
✓ 已验证
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
Computational and Structural Biotechnology Journal
·
2024
·
IF 4.4
Jian Wang,Meina Zhang,Chao Li,Mengyuan Liu,Yixin Qi,Xiaolin Xie,Changlin Zhou,Lingman Ma
Antimicrobial peptides are promising therapeutic agents for treating drug-resistant bacterial disease due to their broad-spectrum antimicrobial activity and decreased susceptibility to evolutionary resistance. In this study, three novel cathelicidin antimicrobial peptides were identified from Thamnophis sirtalis , Balaenoptera musculus , and Lipotes vexillifer by protein database mining and sequence alignment and were subsequently named TS-CATH, BM-CATH, and LV-CATH, respectively. All three peptides exhibited satisfactory antibacterial activity and broad antibacterial spectra against clinically isolated E. coli , P. aeruginosa , K. pneumoniae , and A. baumannii in vitro . Among them, TS-CATH displayed the best antimicrobial/bactericidal activity, with a rapid elimination efficiency against the tested drug-resistant gram-negative bacteria within 20 minutes, and exhibited the lowest cytotoxicity toward mammalian cells. Furthermore, TS-CATH effectively enhanced the survival rate of mice with ceftazidime-resistant E. coli bacteremia and promoted wound healing in meropenem-resistant P. aeruginosa infection. These results were achieved through the eradication of bacterial growth in target organs and wounds, further inhibiting the systemic dissemination of bacteria and the inflammatory response. TS-CATH exhibited direct antimicrobial activity by damaging the inner and outer membranes, resulting in leakage of the bacterial contents at super-MICs. Moreover, TS-CATH disrupted the bacterial respiratory chain, which inhibited ATP synthesis and induced ROS formation, significantly contributing to its antibacterial efficacy at sub-MICs. Overall, TS-CATH has potential for use as an antibacterial agent.
研究领域:
微生物学
·
药理学
·
传染病学
✓ 已验证
产品关联
DOI
PubMed
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
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
MICROPOROUS AND MESOPOROUS MATERIALS
·
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
·
无机化学
·
薄膜制备
·
沸石化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
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
·
催化化学
·
材料科学
·
工业化学
·
绿色化学
✓ 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
危险品化学品经营许可证（带存储）