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
Particuology
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2025
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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
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有机合成
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产品关联
DOI
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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高影响因子
Journal of Materials Chemistry A
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2025
·Vol. 13
·期 47
·40842-40849
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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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CHEMICAL ENGINEERING SCIENCE
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2025
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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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Inorganic Chemistry Frontiers
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2025
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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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产品关联
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
Nature Synthesis
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2026
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IF 22.6
He Feng,Lopez-Haro Miguel,Chen Tianxiang,Marini Carlo,Dou Xiaomeng,Wang Quan-Ming,Liu Lichen
Synthesis of hierarchical zeolites has been proven to be an effective strategy for improving reactant accessibility to active sites and extending catalyst lifetimes. Existing synthesis methods typically generate mesopores within zeolite crystallites instead of inside zeolites with an open-structure porosity. Here we have developed a general synthesis method by optimizing the crystallization conditions and molecular structures of the polymer template and linkage reagent, resulting in the formation of hierarchical MFI-, MEL-, BEA- and CHA-type zeolites with open porosity formed by highly interconnected microporous channels. Based on this method, we prepare a hierarchical TS-1 zeolite with open porosity as a support for a gold catalyst. The resultant Au/TS-1 catalyst exhibits high activity and stability for the direct epoxidation of propylene with H 2 and O 2 , which is associated with the intimate contact between the gold and titanium sites and the zeolite’s unique pore structure.
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高影响因子
Journal of Energy Chemistry
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2026
·
IF 15.6
Yun Tian,Menghao Jiang,Jinxing Long
Developing in-situ catalysts featuring good activity for lignin hydrogenolysis is highly desirable, yet remains a great challenge. In this work, we proposed an efficient strategy for selective hydrodeoxygenation of lignin to a versatile petrochemical of alkylcyclohexanol (ACH) using the in-situ Ru nanoparticles anchored on MgO-modified TS-1. The results demonstrated that, with HRO 5 -MgO 20 @TS-1 catalyst, a total monomer yield of 36.4% was shown from the one-pot cascade process of lignin hydrogenolysis and phenolics hydrodeoxygenation. Importantly, 55.8% of obtained monomers were identified as ACH (20.2% yield), which has been widely used as an oxygenated fuel, solvent, and intermediate for functionalized materials. Intensive catalyst characterizations using TEM, XPS, and XAFS revealed that the highly dispersed in-situ Ru 0 species, together with the suitable acid-base properties, are responsible for the superior catalytic performance of HRO 5 -MgO 20 @TS-1 in lignin depolymerization. In addition, a plausible reaction pathway for ACH formation has been proposed, according to the results of comparative characterization of raw and regenerated lignin, and the performance of lignin model conversion. Therefore, this work provides a new insight into producing value-added alkylcyclohexanol from the renewable lignin.
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高影响因子
CHEMICAL PAPERS
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2026
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IF 2.7
Gu Yu-Qing,Fan Cong-Xuan,Xing Shi-Feng,Zhu Hong-Jun
Modified TS-1 catalysts were prepared by treating TS-1 with different alkalis for the nitration of aldoxime, and the effect of alkali treatment on catalytic performance was investigated. TS-1 was modified using organic amines such as ethylamine (EA), triethylamine (TEA), and tetrapropylammonium hydroxide (TPAOH), as well as inorganic bases such as NaOH, KOH. The catalysts were characterized by XRD, FT-IR, UV-vis, N 2 adsorption etc., which showed that the volume of mesopores increased and the skeleton structure remained basically unchanged by the ethylamine-modified TS-1 and the TPAOH-modified TS-1. The highest yield of 1-nitropropane increased 78% when propionaldehyde oxime was catalyzed by the 0.1 mol/L ethylamine treated sample TS-1-EA-0.1. The enhanced catalytic performance of TS-1 after ethylamine treatment may be attributed to the matching between the pore size of modified TS‑1 and the molecular size of propionaldehyde oxime. Subsequently, TS-1-EA-0.1 was used to catalyze acetaldoxime and butyraldehyde oxime. The results revealed that this catalyst was suitable for acetaldehyde oxime as expected, but less effective for the oxidation of butyraldehyde oxime with a larger molecular diameter than propionaldehyde oxime to 1-nitrobutane. Graphical abstract
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2026
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IF 3.7
Yingdi Jiang,Wanbin Zhan,Chao Yang,Jing Zhang,Changjiu Xia,Gang Qian,Xuezhi Duan
The direct hydroxylation of benzene with hydrogen peroxide (H 2 O 2 ) over titanium silicalite-1 (TS-1) offers an environmentally benign route to phenol, though its efficiency is highly dependent on the solvent environment. By integrating experimental and theoretical approaches, this study reveals the underlying mechanism. Water uniquely boosts benzene conversion to 45.8% through synergistic effects. It serves as a proton-transfer mediator to lower the activation barrier (Δ G ), enhances the electrophilicity of Ti-active sites via increased maximum electrostatic potential (ESP max ), and leverages the hydrophobic pores of TS-1 to enrich benzene near the active sites. However, this this multifunctional enhancement also promotes over-oxidation, limiting phenol selectivity to 42.8%. In contrast, the organic solvents suppress consecutive oxidation and achieve high selectivity above 70% due to their larger HOMO-LUMO energy gaps ( E gap ). Yet they exhibit low activity owing to higher energy barriers, weaker electrophilicity, and competitive adsorption. This work further establishes quantitative correlations between catalytic performance and key descriptors such as Δ G , ESP max , and E gap , providing a predictive framework for rational solvent selection in TS-1 catalysis.
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高影响因子
ACS Catalysis
·
2026
·
IF 13.6
Xianming Zhao,Mengde Kang,Jian Zhou,Jing Li,Mei Ren,Xinya Zhang,Honghao Liu,Zhongcheng Tian,C. Richard A. Catlow,Songmei Sun,Cheng Lian,Marc Pera-Titus,Yongsheng Li
The direct oxidation of methane to methanol at room temperature is a highly sought-after but challenging reaction due to methane’s inert C−H bond and methanol overoxidation. Conventional approaches often require high temperature and pressure or special oxidants. Here, we report an AuxPdy/TS-1 composite photocatalyst with tunable Au/Pd ratios that achieves highly selective methane-to-methanol conversion at near-room temperature using water as the oxidant. An optimized Au0.1Pd0.05/TS-1 photocatalyst exhibits an activity of 64.7 mmol gAuPd−1 h−1 and a turnover frequency of 19.1 h-1 with 100% methanol selectivity under simulated solar light. This performance arises from the efficient electron-hole generation by encapsulated nanoalloy AuPd clusters, generating ·OH and ·CH3 radicals for methane activation and water oxidation, as evidenced by in situ EPR and DRIFT spectroscopy. DFT calculations show that Au sites preferentially mediate the formation of methanol via surface-bound *CH3 and *OH intermediates. Alloy-induced Pd→Au charge redistribution modulates CH4/H2O activation energetics and weakens methanol binding. This study demonstrates an efficient and mild route for highly selective methane utilization under mild conditions.
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高影响因子
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