Bioengineered
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2018
·
IF 1.639
Yanshun Kang,Xiaolin Xu,Huiran Pan,Jing Tian,Weihua Tang,Siqi Liu
In this report, the decolorization features of extracellular enzymes and mycelia separately prepared from Aspergillus sp. TS-A CGMCC 12,964 (120 h) were investigated. The fermentation broth of TS-A degraded 98.6% of Mordant Yellow 1 (50 mg/L) at an initial pH 6 within 1 h with over 70% of the dye (50 mg/L) degraded by extracellular enzymes and 18.8% removed by live mycelia. The degradation products of the dye were analyzed by UV-Vis and FTIR spectra. The decolorization rates of extracellular enzymes and mycelia were examined under different contact periods, dye concentrations and pH values. The extracellular enzymes exhibited excellent degradation activity under weak acidic conditions. In addition, biosorption models of mycelia fitted well the Langmuir isotherm model and the pseudo-second-order kinetic equation. Although the decolorization process was achieved through the synergistic effects of mycelia and extracellular enzymes, decolorization was dominated by the biodegradation activity of the extracellular enzymes from TS-A.
研究领域:
环境科学
·
微生物学
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DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 6
·1-16
·
IF 2.4
Li Tong,Liu Fuliang,Wang Xiaofang,Han Zhaohao,Jia Xiaoqiong,Wang Ping,Chu Qingyan,Sheng Yuxuan
The precise embedding of metal species within specific sites of zeolite frameworks and their unique microenvironments exert fascinating influences on catalytic performance. Herein, we report the rational design of a highly efficient Co-Cu@CTS-1 catalyst through the strategic incorporation of Co, Cu, and Ce into TS-1 zeolite, where Ce is doped at silicon atomic sites while Co and Cu are encapsulated within the zeolite cages. Mechanistic investigations reveal that the synergistic interplay among Co, Cu, and Ce is pivotal for catalytic activity: Co facilitates molecular oxygen activation to generate reactive oxygen species (O⁻), while Ce(III) enhances oxygen vacancy concentration, significantly boosting styrene conversion. Moreover, the distinctive electronic interaction between Ce and Cu markedly improves the selectivity toward styrene oxide. The optimized Co-Cu@CTS-1 catalyst exhibits exceptional performance in the aerobic epoxidation of styrene, achieving a remarkable conversion of 78.11% with 87.31% epoxide selectivity under mild conditions (80 °C, 2 h). Furthermore, the catalyst demonstrates outstanding stability, retaining 68.21% conversion even after 20 reaction cycles, underscoring its superior resistance to metal sintering and long-term durability. This work provides valuable insights into the rational design of multifunctional zeolite catalysts through precise metal positioning and microenvironment modulation. Graphical
研究领域:
催化化学
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材料科学
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环境化学
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高影响因子
CATALYSIS LETTERS
·
2019
·Vol. 150
·期 6
·1641-1649
·
IF 2.372
Luo Qianqian,Lu Tianliang,Xu Jun,Yang Xiaomei,Zhou Lipeng
Abstract Methyl pyruvate (MPA) was synthesized from dihydroxyacetone (DHA), the oxidation product of glycerol, over Sn-β and TS-1 hybrid molecular sieves at low temperature. Sn-β and TS-1 provide the active sites for conversion of DHA to methyl lactate (MLA) and oxidation of MLA to MPA, respectively. Synergism of Lewis acid sites on Sn-β and TS-1 realize the production of MPA from DHA. After optimization, 71% yield of MPA can be obtained under 50 °C. This is the first report for the synthesis of MPA from DHA directly. Graphic Abstract
研究领域:
催化
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绿色化学
·
化工
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高影响因子
ACS Applied Materials & Interfaces
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2025
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IF 8.2
Kaiwei Wang,Fumin Wang,Xubin Zhang,Mingshuai Sun,Yi Zhai,Yihao Wang,Hongyu Wang,Yang Qin,Hao Ruan
Nanosheet MFI zeolite with a shortened b-axis length is highly desirable for industrial applications due to the predominant mass transfer pathway provided by its larger straight channels along the b-axis. The introduction of specific additives into the precursor fluid of the zeolite can facilitate crystal anisotropic growth. However, the range of available additives is limited, and their role and underlying mechanisms remain poorly understood. Herein, the effect of three pyrrolidone compounds on the anisotropic growth of the TS-1 zeolite is unveiled within the crystallization engineering, such as 2-pyrrolidone, N-methylpyrrolidone, and N-vinyl-2-pyrrolidinone. The effects of different water content (H2O/SiO2 = 40, 100, and 160), pyrrolidone compound addition (x/SiO2 = 0.2, 0.6, 1, and 2), and seed liquid concentration on the nanosheet morphology of zeolite were studied. The TS-1 nanosheet zeolite synthesized using pyrrolidone compounds as an additive exhibits abundant high coordination titanium active sites and demonstrates excellent catalytic performance in olefin epoxidation. In this work, the crystals form a nanosheet zeolite in a nonclassical growth path. The ATS-100-1-1 sample had a thickness of 112 nm in the b-axis direction and an Lc/Lb aspect ratio of 20.08. The development of morphological engineering strategies can be extended to zeolites with other topological structures based on the intrinsic properties and interactions of additive molecules with different crystal faces.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
Molecular Catalysis
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2025
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IF 4.9
Jinghui Lyu,Tao Liu,Shihao Wang,Jun Wei,Jinke Yao,Yiyong Zhao,Han Wu,Xianghao Zhang,Peikun Li,Zhizheng Wang,Qunfeng Zhang,Dahao Jiang,Qingtao Wang,Guofu Zhang,Chengrong Ding,Xiaonian Li
TS-1 zeolite is a catalyst known for its high selective oxidation performance and broad industrial applications. The titanium atom in the TS-1 often acts as the active center in catalytic reactions, especially in oxidation reactions, so increasing the titanium content in TS-1 is of great significance in chemical reactions and catalytic applications. This paper explores a Novel Boron Extraction and Titanium Incorporation Strategy to enhance the titanium content within the TS-1 framework. During the dry gel preparation process, boron species were introduced in situ into the framework of the TS-1 to form a framework boron-titanium-silicon TS-1-B with tetra-coordinated or tri-coordinated positions. TS-1-B is then treated with acid to remove the framework boron, while an appropriate amount of titanium precursor is introduced to fill the vacancy left by the removal of the framework boron. The results of XRD, FT-IR, UV–Vis, BET, NH 3 -TPD, XRF, and XPS showed that the titanium content of the tetracoordinate framework in the TS-1 was improved. The catalytic performances of TS-1-B, TS-1-BS, and TS-1-BST were comparatively evaluated through two representative reactions: propylene epoxidation and the direct synthesis of hydrogen peroxide from H₂ and O₂.
研究领域:
催化化学
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材料科学
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无机化学
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化学工程
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多孔材料
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DOI
高影响因子
ACS Catalysis
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2026
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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
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
·
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
Nature Synthesis
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2026
·
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
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2026
·
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
Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 12
·3077-3084
·
IF 6.569
Jiani Zhang,Huaizhong Shi,Yue Song,Wenjing Xu,Xianyu Meng,Jiyang Li
Titanium silicalite-1 (TS-1) zeolite, as a promising shape-selective catalyst, has excellent catalytic activity in many oxidation reactions. However, there are still challenges to rapidly synthesize TS-1 and achieve a high content of Ti in TS-1 without anatase TiO2. In this work, a high-efficiency strategy has been proposed by using 1,3,5-benzenetricarboxylic acid (H3BTC) as a crystallization modifier to rapidly synthesize enhanced-Ti TS-1 zeolite without extra-framework anatase TiO2. In such a synthetic system, a mixed liquid–solid precursor phase is formed within 4.5 hours, and then TS-1 crystals can be produced within one day based on the special combination mechanism of liquid-phase and solid-phase conversion. Ti species enter into the TS-1 framework by the transformation from the liquid phase to crystals as well as by the in situ transformation of the solid phase, which makes the content of framework Ti increase significantly, and the Si/Ti ratio can reach 48.5 without any anatase TiO2. In the epoxidation of 1-hexene with H2O2 as an oxidant, the conversion of alkene over the synthesized TS-1 was improved by 8.01% compared to the traditional TS-1 (18.11% vs. 10.10%). The high-efficiency strategy reported in this paper will provide new opportunities for further promoting the industrial application of TS-1 zeolite.
研究领域:
材料科学
·
催化化学
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高影响因子
CATALYSIS TODAY
·
2021
·
IF 6.766
Hai Wang,Liang Wang,Dong Lin,Xiang Feng,Xuefeng Chu,Lina Li,Feng-Shou Xiao
In situ release of hydrogen from liquid organic hydrogen carriers―such as methanol by steam reforming, offers a feasible way to potentially solve the problem of hydrogen storage and transport. Here we report that the titanosilicalite-1 (TS-1) zeolite support efficiently accelerates the Pt catalyzed methanol steam reforming (MSR), giving the hydrogen productivity at 639.7 mol H2 mol Pt −1 h −1 at 250 °C, which steadily outperforms the Pt nanoparticles supported on other carriers, including ZSM-5 zeolite, amorphous SiO 2 , and TiO 2 anatase. Further studies reveal that the electronic metal-support interactions (EMSIs) between Pt and TS-1 zeolite occurs, which modifies Pt nanoparticles surface charge state to accelerate the reaction. More importantly, the interactions could stabilize the Pt nanoparticles, achieving sinter-resistant Pt/TS-1 catalyst in the continuous MSR tests. This finding indicates the important role of heteroatoms in the zeolite framework for supported metal nanoparticles, which open a new way to guide the design of highly efficient heterogeneous catalysts in the future.
研究领域:
催化化学
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材料科学
·
能源化学
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高影响因子
危险品化学品经营许可证（带存储）