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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Catalysis Science & Technology
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2025
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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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Frontiers of Chemical Science and Engineering
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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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高影响因子
APPLIED CATALYSIS A-GENERAL
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2025
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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
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储能技术
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Catalysts
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2026
·Vol. 16
·期 5
·417
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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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SCIENTIA HORTICULTURAE
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2024
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IF 3.9
Linmu Chen,Jingna Yan,Yiwen Miu,Rui Huang,Hao Wei,Lilei Wang,Cheng Zhang,Lianyu Yuan,Huarong Tong
The distinct qualities of etiolated leaves from chlorotic tea cultivars are significantly related to their developmental stages during harvesting. In this study, Hjy ( Camellia sinensis L. cv . Huangjinye) as a light sensitive etiolated tea variety had a higher concentration of theanine (99.36 mg/g) and lower total catechins (119.15 mg/g) than normal green tea plant. The shading treatment could turn the yellow leaves to green and alter the levels of catechins, caffeine, and theanine of tea shoots in Hjy. Additionally, the buds and 2nd leaves of Hjy tea shoots had the highest content of theanine, whereas the 3rd leaves contained the highest caffeine and total catechins. Moreover, the three different developmental stages of Hjy tea leaves had different levels of pigments, total free amino acids, total polyphenols, and soluble protein. Transcriptome and metabolome analyses identified a total of 58,175 genes and 414 metabolites in the three developmental stages, which were most enriched in photosynthesis, primary metabolism, lipid metabolism, and flavonoid metabolism. The multi-omics analysis revealed that the accumulations of L- glutamic acid and L-glutamine were up-regulated by GOGATs and GDHs and down-regulated by GSs, TS , and ALaDC. WRKY24, WRKY27, MYB105, and some other genes related to plant development and ion balance were highly correlated with L- glutamic acid biosynthesis. The decreased expressions of LARs and ANRs contributed to the reduction of catechin, epigallocatechin, and epigallocatechin gallate. WRKY35 , W RKY53, MYB62 , and some other genes related to photosynthesis, plant development, monooxygenases, and glycosylation exhibit roles in regulating catechins biosynthesis. This study provided the novel information about the Hjy tea plant, and the integrated strategy of multi-omics allowed a mechanistic understanding of the differential accumulation of L- glutamic acid and catechins during the development of etiolated tea leaves.
研究领域:
植物科学
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分子生物学
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农学
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茶学
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高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Yanan Jia,Lin Hao,Jun Zhang,Xing Zhang,Siying An,Ming Su,Huan Wang,Yufan Zhang
We describe a PCR-free, enzyme-free, and simple biosensing platform for the electrochemical monitoring of telomerase activity based on Au nanorods (AuNRs) as an electrocatalytic redox mediator, which enhances the electrochemical signal by catalyzing acetaminophen (AP). In this process, acid-functionalized ordered mesoporous carbon (OMC) was modified on a glassy carbon electrode (GCE) surface to offer -COOH sites. Moreover, the amino-modified S1 was fixed on the modified electrode by conducting an amide reaction. TS is extended to (TTAGGG) n repeat units in the presence of telomerase extract and dNTPs. One end (5′) is hybridized with S1 on the electrode, and the remaining end (3′) is combined with AuNRs-S2 probe. Clearly, the telomerase activity is relevant to the amount of connected AuNRs, resulting in different response signals. Therefore, with the telomerase extension triggered hybridization reaction, a large amount of AuNRs catalyst was introduced onto the surface of GCE as the sensing platform, thus achieving a sensitive electrochemical telomerase activity assay in the range of 20–2.15 × 10 6 HeLa cells mL −1 . This sensing platform shows that the limit of detection is 1.74 HeLa cells mL −1 , thus providing a promising method for the determination of telomerase activity and a powerful biosensor for accurate cancer monitoring and diagnosis.
研究领域:
生物传感器
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电化学
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癌症诊断
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纳米技术
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