APPLIED CATALYSIS A-GENERAL
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2021
·
IF 5.706
Linghao Li,Wei Wang,Jian Huang,Rongmin Dun,Rui Yu,Yiwei Liu,Zile Hua
Nanosized hierarchical titanosilicate-1 zeolites ( nano TS-1_D) with variable Ti doping content were synthesized by a simple and sequent two-step procedure consisting of microporous TS-1 nanocrystal synthesis through steam-assisted dry-gel conversion and post alkali-etching treatment for mesopore formation. Comprehensive characterizations, e.g. XRD, N 2 sorption isotherms, DLS, UV-Vis, SEM, TEM and water-droplet contact angle, indicated that the resultant nano TS-1_D materials not only possess abundant intracrystal mesopores and high surface area, but importantly maintain the intrinsic surface hydrophobicity as those of microporous TS-1 zeolites. Consequently, they showed the expected superior catalytic performance in both bulky cyclohexene/cyclooctene epoxidation and phenol hydroxylation probe reactions, contrast to the microporous TS-1 and amorphous Ti-MCM-41 mesoporous counterparts. In the oxidative desulfurization of fuels, they exhibited 100% removal ability for thiophene and its bulky derivatives and excellent recyclability. In addition, a new Ti-dopant directed alkali-etching mechanism has been proposed to illustrate the synthesis of high-specific-surface-area nano TS-1_D.
研究领域:
材料科学
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催化化学
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高影响因子
Inorganics
·
2025
·Vol. 13
·期 2
·37
·
IF 3
Yao Wang,Hongda Yu,Huan Wang,Tiehong Chen
The environmental and health impacts of sulfur compounds in fuel oil have prompted considerable research interest in oxidative desulfurization (ODS) technology. Tetrahedrally coordinated titanium has been demonstrated to exhibit excellent activity in the context of oxidative desulfurization processes. However, further improving the catalytic property of the tetrahedrally coordinated titanium remains a challenging endeavor. In the context of ODS processes conducted at near room temperatures, the improvement of conversion remains a subject of considerable challenge. In this study, hierarchically porous titanosilicate hollow spheres were synthesized by using TS-1 zeolite precursors as Ti and Si sources to obtain the catalyst with only tetrahedrally coordinated titanium. The synthesized materials were characterized through transmission electron microscopy (TEM), Fourier-transform infrared spectroscopy (FT-IR), ultraviolet–visible diffuse reflectance spectroscopy (UV-Vis), and nitrogen adsorption analysis. These techniques confirmed the formation of hollow spherical hierarchically porous structures with Ti species uniformly incorporated in tetrahedral coordination and the presence of five-member rings of TS-1 zeolite. As a result, the hierarchically porous titanosilicate hollow spheres demonstrated excellent catalytic performance in ODS, achieving complete dibenzothiophene (DBT) removal within 15 min and a high turnover frequency (TOF) of up to 123 h−1at 30 °C.
研究领域:
催化化学
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环境化学
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材料科学
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化学工程
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2026
·
IF 2.6
Yining Chen,Fangna Shangguan,Weilong Chun,Lijia Li,Xin Yang,Jiale Qi,Yujing Xun,Huiyong Chen
TS-1 zeolite demonstrates notable activity and selectivity in cycloolefin epoxidation when employing H₂O₂ as the oxidant.However, the practical application of conventional TS-1 is significantly limited by factors including surface hydrophilic structures and mass transfer constraints. To address these challenges, a carbon-encapsulated hierarchical TS-1 (3DC_TS-1) has been synthesized through the confined growth approach, in which 3DOm carbon is used as a confined space provider for TS-1 crystallization and further acts as a hydrophobic wrapper to modulate the surface microenvironment of TS-1 crystals. In the epoxidation of cyclopentene and cyclohexene with using H₂O₂ as the oxidant, the hydrophobic 3DC_TS-1 catalyst exhibits a superior selectivity to epoxide products by suppressing epoxide hydrolysis and allyl oxidation side reactions, comparing with the 3D_TS-1 catalyst without carbon wrapper and the conventionally microporous TS-1 catalyst.It is expected that this study will provide an effective strategy for designing zeolite catalysts applying to selective oxidation reactions.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2015
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IF 3.091
Yao Chen,Ruofan Peng,Tongdong Shen,Shaoping Tong,Chunan Ma
The oxidative efficiency of H 2 O 2 /O 3 in the presence or absence of titanium silicalite of TS-1 was investigated at pH value of 3.0, in which acetic acid was selected as the target organic compound owing to its inert to ozone. The removal rate of acetic acid by H 2 O 2 /O 3 was negligible (5.6% in 30 min) because of the impossible deprotonation reaction of H 2 O 2 in acidic solution. However, addition of titanium silicalite of TS-1 could greatly improve the oxidative efficiency of H 2 O 2 /O 3 (29% in 30 min). The results of effects of different parameters such as concentration of H 2 O 2 , concentration of TS-1, rate of ozone input, and pH value, on the oxidative efficiency of TS-1/H 2 O 2 /O 3 showed that the degradation of HAc by TS-1/H 2 O 2 /O 3 was controlled by the transfers of reactants (including ozone and HAc) to the surface of TS-1. The tests of addition of tert-butyl alcohol and dimethyl sulfoxide (DMSO) both confirmed generation of hydroxyl radicals in this process. The rate of generation of hydroxyl radicals could be controlled by adjusting the concentration of H 2 O 2 . The mechanism for generation of hydroxyl radicals might be the reaction of some reactive oxygen species (including Ti(IV)-superoxide and Ti(IV)-hydroperoxide/peroxide), which resulted from the interaction of TS-1 with H 2 O 2 , with dissolved ozone. The results are of significance for the effective pretreatment of acidic wastewater containing refractory ozone-inert organic matter.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2026
·
IF 2.6
Qishan Chen,Hui Ding,Bo Zhu,Xu Li,Jinxiang Dong
The green and efficient epoxidation of long-chain linear α-olefins represents a crucial step in the synthesis of key industrial intermediates. Although the hydrogen peroxide/titanosilicate-1 (H2O2/TS-1) catalytic system is environmentally friendly, its broad industrial implementation has long been hindered by unsatisfactory epoxide selectivity and low H2O2 utilization efficiency, which limit large-scale and economical production. To overcome these limitations, a strategy employing tetrapropylammonium bromide (TPABr) as a crystallization modifier was developed to precisely engineer the active sites of TS-1 zeolites. By balancing the incorporation kinetics of titanium and silicon into the framework, uniform distribution of titanium species was achieved, accompanied by the enrichment of highly active Ti(OH)2(OH2)2(OSi)2 sites. The resulting TS-1-TPABr-40 catalyst delivered outstanding performance in the epoxidation of 1-hexene, exhibiting 97% epoxide selectivity, ∼76% effective H2O2 utilization, and good recyclability. These results highlighted how molecular-level coordination engineering in zeolite catalysts could simultaneously enhance catalytic efficiency and oxidant economy, providing a sustainable and scalable strategy for green chemical synthesis.
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DOI
高影响因子
Journal of Physical Chemistry C
·
2024
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IF 3.3
Jiaojiao Yu,Yi Zuo,Gudan Li,Hong Yang,Xinwen Guo
To synthesize a high-performance titanium silicalite-1 (TS-1), this paper reports a simple and environmentally friendly approach to regulate the alkalinity in the synthesis of titanium silicalite-1 (TS-1) involving tetrapropylammonium hydroxide (TPAOH) and tetrapropylammonium bromide (TPABr). Essentially, the pH of the synthesis gel was controlled by n(TPAOH/TPA+), while keeping the total tetrapropylammonium cations (TPA+) constant. The study shows that at a relatively moderate alkalinity of pH = 10.7, TS-1 produced exhibits nanocrystalline microstructure favorable for diffusion, contains high contents of TiO4 and TiV, and delivers 94.3% of H2O2 conversion with a turnover frequency of 565.6 mol (mol h)−1 in propylene epoxidation. Through detailed analysis of crystallization processes of TS-1 at different alkalinities, this study unveils the effect of alkalinity on the rate of Si–Ti condensation, which dictates the formation of the framework structure and incorporation of Ti species into the framework. Essentially, only at moderate alkalinity of pH = 10.7, comparable Si–OH and Ti–OH condensation rates permit the highest amount of Ti being inserted in TS-1 as active (TiO4 + TiV) and limits the self-condensation of Ti species to form inactive anatase-TiO2.
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
Inorganic Chemistry Frontiers
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2025
·
IF 6.4
Xing-Yu Yue,Yuan-Yuan Wang,Shen Yu,Chun-Mu Guo,Zhan Liu,Yi-Long Wang,Zhi-Yi Hu,Yu Li,Li-Hua Chen,Bao-Lian Su
Bio-inspired catalyst materials with diverse functions and excellent performance are highly demanding for efficient catalytic conversion. However, precisely imitating the natural structure to achieve optimized performance is still highly challenging. Inspired by the fast mass diffusion and exchange ability of an alveolus structure, we prepared hierarchically macro-meso-microporous TS-1 zeolite microspheres with precisely designed alveolus-like structure (HAS-TS-1) by developing a method combining of template and emulsion approaches. The alveolus-like zeolite microspheres possessed interconnected macropores (280 nm) and mesopores (40 nm) with a BET surface area of 484 m2/g. This novel bio-inspired structure showed a significantly enhanced adsorption ability of thiophenic molecules, which was four times of that in a microporous TS-1 zeolite. The HAS-TS-1 exhibited excellent catalytic oxidative desulfurization performance of a series of bulky thiophenic molecules, completely removing 4,6-dimethyldibenzothiophene (DMDBT) in 15 min, which was twelve times faster than a TS-1 microsphere (180 min). The superiority of this bio-inspired hierarchically alveolus-like structure in mass transfer and diffusion might stimulate its advanced functions in the field of catalysis, energy, and sensor.
研究领域:
材料科学
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催化化学
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能源化学
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DOI
高影响因子
MATERIALS RESEARCH BULLETIN
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2024
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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
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材料科学
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产品关联
DOI
高影响因子
Particuology
·
2025
·
IF 4.3
Liping Zhao,Chun Shen,Guangsheng Luo
Supported small TS-1 particles are important catalysts in the ammoximation of ketones, but still facing challenges such as agglomeration in the reaction system and long synthesis time. In this work, we report the fast synthesis of small TS-1 particles supported on porous glass beads in a microreactor. Short crystallization time of only 1.5 h is needed for the synthesis of TS-1 particles with the mean size of ∼200 nm. Effects of aging time, size of the microchannel, sol/support mass ratio, crystallization temperature, and surface areas of the porous glass beads on the morphology and catalytic performance for ammoximation of cyclohexanone have been studied systematically. The as-synthesized supported TS-1 catalyst achieved 82.4% cyclohexanone conversion and > 99% selectivity to cyclohexanone oxime after reaction at 353 K for only 20 min, and the conversion rises to 97.6% if the duration prolongs to 40 min, outperforming the commercial TS-1 catalyst and supported TS-1 catalyst synthesized in an autoclave (crystallized for 48 h).
研究领域:
催化化学
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化学工程
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材料科学
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微反应技术
·
有机合成
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
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IF 3.375
Zheng Zhang,Rui Fang,Xiao-Xin Kong,Miao Feng,Gui-Ping Cao,Hui Lu,Shuang Ji,Peng Gao,Jia-Hao Zhang
In this paper, monolithic TS-1 (a zeolitic material containing both silicon and titanium) was successfully synthesized on polymer-modified carbon nanotubes/nickel foam (PMTS-1). PMTS-1 had high surface areas and aggregated pores (confined pores formed in an aggregated structure), and TS-1 could be evenly dispersed on the surface, which could facilitate reactant transport and improve dispersibility of TS-1. TS-1 strongly interacted with the polymer-modified CNTs/NF and is highly dispersed because the PDDA-modification could enhance the positivity of CNTs/NF. PMTS-1 was beneficial to the adsorption of the reactant propylene and the desorption of the product propylene oxide, which reduced the side reaction of the deep oxidation of propylene oxide, pore blocking, and coke formation. Also, the adsorption capacity of PMTS-1 to H2O2 was enhanced, which created a microenvironment conducive to the forward reaction. After the reaction, PMTS-1 was easily separated from the reactants, which offered an economical application prospect.
研究领域:
催化化学
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材料科学
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化学工程
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纳米复合材料
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沸石化学
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DOI
高影响因子
Journal of Materials Chemistry A
·
2025
·Vol. 13
·期 47
·40842-40849
·
IF 9.5
Yumeng Hu,Yulin Yao,Zhenheng Diao,De Sun,Yuanyuan Dong
The catalytic performance of TS-1 zeolites in selective oxidation reactions is strongly influenced by both the TiO6 concentration and specific surface area. However, simultaneously optimizing these two critical factors remains a significant challenge. Herein, a biuret-assisted hydrothermal synthesis strategy was developed to fabricate hierarchical TS-1 zeolites with high TiO6 concentration and enhanced specific surface area. The interaction between the amide groups of biuret and Ti monomers promoted the formation of TiO6 during crystallization, while the confinement effect of biuret facilitated the construction of mesopores. The resulting hierarchical TS-1 exhibited good catalytic activity and stability towards 1-hexene epoxidation and oxidative desulfurization reactions, where the conversion was 1.41 and 3.36 times higher than that of conventional TS-1, respectively. This work provides a facile approach for designing high-performance TS-1 catalysts by dual regulation of active sites and porosity.
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yuxia Zhong,Zhihua Zhang,Min Zhang,Yujie Liao,Shudong Shi,Wenyao Chen,Liang Wang,Xinggui Zhou,Xuezhi Duan
The selective oxidation of alkanes is challenging due to the inertness of C–H bonds and the tendency for overoxidation to COx. Metal-zeolite catalysts offer a promising solution by spatially decoupling oxygen and C–H bond activation on distinct active sites. This study introduces a strategy using surface hydrophobic modification of titanium silicalite-1 (TS-1) zeolites to achieve high selectivity in propane oxidation to acetone. Hydrophobic organosilanes with methyl groups were applied via a one-step co-condensation process, followed by Au nanoparticle immobilization. The hydrophobic groups prolong the residence time of the intermediate isopropanol on the catalyst surface, enhancing its conversion to acetone while stabilizing H 2 O 2 to prevent excessive oxidation of carbon-containing species into CO 2 during the process. The modified TS-1 demonstrated excellent thermal stability and selectivity, particularly under extreme hydrogen-to-oxygen ratios conditions. The alkylated Au/TS-1 catalysts significantly improved acetone production, providing a new pathway for selective alkane oxidation.
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高影响因子
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