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JOURNAL OF POROUS MATERIALS · 2015 ·Vol. 22 ·期 3 ·577-584 · IF 1.108

Hierarchically structured SAPO-5 molecular sieve catalysts with tailored mesoporosity for alkylation reaction

Zhao Xinhong,Wen Juanjuan,Zhao Jiangbo,Li An,Li Guixian,Wang Xiaolai

Hierarchically structured SAPO-5 molecular sieve was synthesized by microwave-assisted ionothermal method in eutectic mixture solvent. Their porous texture and acid properties were characterized by nitrogen physisorption, SEM, TEM and NH 3 -TPD. The results show that the mesoporous volume of SAPO-5 can be tuned via simply varying the degree of supersaturation, the type of mineralizer or replacing partly succinic acid with sebacic acid. A lower degree of supersaturation and using ammonium fluoride as a mineralizer favor the synthesis of SAPO-5 with large mesoporous volume. Notably, the introduction of sebacic acid can lead to three-level micro-meso-macroporous structure (sample C1). Five typical samples were selected as catalysts and tested in the alkylation of benzene with benzyl alcohol. Among all catalysts, the sample C1, whose aspect ratio is the lowest, exhibited the best catalytic activity, giving a 91 % benzyl alcohol conversion. The diffraction peak intensity ratio of I 002 /I 100 was proposed to be a good indicator in fabricating a highly active SAPO-5 catalyst for this reaction.

CAS / MDL: 112945-52-5
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RSC Advances · 2016 ·Vol. 6 ·期 106 ·104398-104406 · IF 3.289

An investigation on the aqueous-phase hydrodeoxygenation of various methoxy-substituted lignin monomers on Pd/C and HZSM-5 catalysts

Cong Zhang,Jingbo Qi,Jing Xing,Si-Fu Tang,Liang Song,Yuanyuan Sun,Chuanhui Zhang,Hongchuan Xin,Xuebing Li

Aqueous phase catalytic upgrading of lignin monomers to hydrocarbons via hydrodeoxygenation (HDO) has been explored using a combination of Pd/C and HZSM-5 catalysts under 2 MPa of H2 (ambient temperature). Model monomers with varying numbers of methoxy groups, including phenol, anisole, guaiacol and 2,6-dimethoxy-phenol, were chosen as lignin model compounds. Mechanistic studies revealed cascade and parallel reaction pathways via hydrogenation and dehydration (hydrolysis) processes, which were catalyzed by Pd/C and HZSM-5, respectively. Hydrogenation was preferred at lower temperature, whereas higher temperature was favorable for the removal of oxygen-containing functional groups. The effect of methoxy groups on the HDO of these monomers was also investigated systematically. Basically, the conversion of multi-substituted monomers was tougher than that of mono-substituted ones, due to steric constraint and the inhibition of the electron-donating hydroxyl group. The selectivities to cyclohexane from phenol and anisole were improved significantly by increasing the temperature to 413 K. However, cyclohexanone was preferably produced over cyclohexane when using model compounds with multi-substituents (guaiacol and 2,6-dimethoxy-phenol), even at temperatures above 513 K. Comparative experiments were also conducted on the HDO of 1,2-cyclohexanediol with or without the presence of phenol, which clearly suggested that the further HDO of guaiacol and 2,6-dimethoxy-phenol was inhibited, probably due to the strong interactions between cyclohexanediol molecules and Brønsted acid sites.

研究领域: 化学工程 · 催化反应
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MACROMOLECULAR BIOSCIENCE · 2016 ·Vol. 17 ·期 4 ·1600262 · IF 3.68

Use of 5-Fluorouracil Loaded Micelles and Cisplatin in Thermosensitive Chitosan Hydrogel as an Efficient Therapy against Colorectal Peritoneal Carcinomatosis

Qin Yun,Si Song Wang,Shan Xu,Jin Ping Yang,Juan Fan,Ling Lin Yang,Yue Chen,Shao Zhi Fu,Jing Bo Wu

Colorectal peritoneal carcinomatosis (CRPC) is a common systemic metastasis of intra-abdominal cancers. Intraperitoneal chemotherapy against CRPC is at present the preferred treatment. The aim of this study is to develop a novel hydrogel drug delivery system through the combination of 5-fluorouracil (5-FU) loaded polymeric micelles and cisplatin (DDP) in biodegradable thermosensitive chitosan (CS) hydrogel. The prepared CS hydrogel drug is a free-flowing solution at room temperature and forms a stationary gel at body temperature. Therefore, a CRPC mouse model is established to investigate the antitumor activity of CS hydrogel drug system. The results suggest that intraperitoneal administration of CS hydrogel drug can inhibit tumor growth and metastasis, and prolong survival time compared with other groups, thus improving the chemotherapeutic effect. Ki-67 immunohistochemical analysis reveals that tumors in the CS hydrogel drug group has lower cell proliferation in contrast to other groups ( P < 0.001). Furthermore, hematoxylin-eosin staining of liver and lung tissue indicates that the CS hydrogel drug has also a certain inhibitory effect on colorectal cancer metastasis to the liver and lung. Hence, the work highlights the potential clinical applications of the CS hydrogel drug.

研究领域: 肿瘤学 · 药剂学
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ACS Applied Materials & Interfaces · 2021 · IF 9.229

Effect of Coordination Environment Surrounding a Single Pt Site on the Liquid-Phase Aerobic Oxidation of 5-Hydroxymethylfurfural

Wanzhen Zhu,Yu Meng,Chaoxin Yang,Jun Zhao,Hongliang Wang,Wei Hu,Guangqiang Lv,Yingxiong Wang,Tiansheng Deng,Xianglin Hou

As the frontier in heterogeneous catalyst, a monomer and positively charged active sites in the single-atom catalyst (SAC), anchored by high electronegative N, O, S, P, etc., atoms, may not be active for the multispecies (O2, substrates, intermediates, solvent etc.) involved liquid-phase aerobic oxidation. Here, with catalytic, aerobic oxidation of 5-hydroxymethylfurfural as an example, Pt SAC (Pt1-N4) was synthesized and tested first. With commercial Pt/C (Pt loading of 5 wt %) as a benchmark, 2,5-furandicarboxylic acid (FDCA) yield of 97.6% was obtained. Pt SAC (0.56 wt %) gave a much lower FDCA yield (28.8%). By changing the coordination atoms from highly electronegative N to low electronegative Co atoms, the prepared Pt single-atom alloy (SAA, Pt1-Co3) catalyst with ultralow Pt loading (0.06 wt %) gave a much high FDCA yield (99.6%). Density functional theory (DFT) calculations indicated that positively charged Pt sites (+0.712e) in Pt1-N4 almost lost the capability for oxygen adsorption and activation, as well as the adsorption for the key intermediate. In Pt1-Co3 SAA, the central negatively charged Pt atom (−0.446e) facilitated the adsorption of the key intermediate; meanwhile, the nearby Co atoms around the Pt atom constituted the O2-preferred adsorption/activation sites. This work shows the difference between the SAC with NPs and the SAA during liquid-phase oxidation of HMF and gives a useful guide in the future single-atom catalyst design in other related reactions.

研究领域: 催化化学 · 材料科学 · 理论计算化学
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ChemCatChem · 2013 ·Vol. 5 ·期 6 ·1517-1523 · IF 5.181

Improved para-Xylene Selectivity in meta-Xylene Isomerization Over ZSM-5 Crystals with Relatively Long b-Axis Length

Yan Liu,Xiaozhao Zhou,Xinmei Pang,Yinying Jin,Xiangju Meng,Xiaoming Zheng,Xionghou Gao,Feng-Shou Xiao

Graphical Join the chain gang: Chain-like ZSM-5 crystals that are synthesized in the presence of starch show higher p -xylene selectivity in m -xylene isomerization than normal, mesoporous, and sheet-like ZSM-5 crystals. ZSM-5 zeolite crystals with controllable b- axis length (sheet-like, S-ZSM-5; chain-like, C-ZSM-5) have been synthesized by using urea and starch as additives in the starting aluminosilicate gels. X-ray diffraction (XRD) patterns and scanning electron microscopy (SEM) images show that these zeolite samples have good crystallinity. Transmission electron microscopy (TEM) images show that there is a strong chemical interaction between the stacked crystals in C-ZSM-5 samples. N 2 sorption isotherms indicate that C-ZSM-5 crystals are mesoporous. Catalytic tests for the formation of p -xylene from m- xylene isomerization show that, compared with other zeolite catalysts, C-ZSM-5 catalysts give both high conversion and improved p -xylene selectivity, which are attributed to the combination of relatively long b -axis length and the present mesoporosity in the crystals. The improvement of p -xylene selectivity in catalytic m- xylene isomerisation is of great importance for selective industrial production of p -xylene in the future.

研究领域: 化学工程 · 材料科学
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Journal of the Taiwan Institute of Chemical Engineers · 2019 · IF 3.834

Direct synthesis of metal-organic frameworks catalysts with tunable acid–base strength for glucose dehydration to 5-hydroxymethylfurfural

Yunlei Zhang,Bing Li,Yanan Wei,Changhao Yan,Minjia Meng,Yongsheng Yan

Developing a green and economically viable approach for the direct synthesis of metal-organic frameworks (MOFs) catalysts with multifunctional active sites remains the key step for their applications in heterogeneous catalysis field. Herein, we report a green (aqueous solutions), mild (90 °C, atmospheric pressure), and modulated hydrothermal (MHT) approach to synthesize UiO-66-type MOFs catalysts with acid–base bi-functional sites, which were obtained via the coordination of monosodium 2-sulfoterephthalate and 2-aminoterephthalic with zirconium (Zr) ions. More importantly, a series of acid, base and acid–base catalysts with varied acid–base strengths can be readily prepared, by simply varying the ratio of organic ligands for preparing MOFs. The synthesized catalysts were characterized and their performances in glucose dehydration to produce 5-hydroxymethylfurfural (5-HMF) have been evaluated. The developed approach in this work has clearly depicted a roadmap for the facile synthesis of MOFs catalysts to facilitate their potential use in acid–base catalysis.

研究领域: 化学工程 · 催化科学
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Journal of Cleaner Production · 2025 · IF 10

Electrochemical dimerization of furfural and 5-hydroxymethylfurfural into aviation fuel precursors: Optimization and mechanistic insights

Jiahui Chen,Xian Pan,Xinchi Zhang,Xin Zhou,Shiliang Wu,Youn-Sang Bae,Ismagil Shakirovich Khusnutdinov,Feng Gong,Tao Li,Huiyan Zhang,Rui Xiao

Furfural and 5-hydroxymethylfurfural are prominent biomass-derived aldehydes, offering substantial potential for sustainable fuel production. The electrochemical dimerization of these bio-derived aldehydes is investigated in this study as a novel and mild approach to carbon-chain elongation (>C6), leading to the formation of viable precursors for aviation kerosene. Compared with conventional electrochemical hydrogenation, this approach directly promotes C–C coupling without additional reagents or harsh conditions. Systematic investigations of electrode materials, applied potentials, and electrolysis duration enabled precise control over product selectivity. Notably, a Pb/CF electrode demonstrated superior catalytic performance, achieving 77.7 % selectivity for hydrofuroin from furfural and 89.8 % for 5,5′-bis(hydroxymethyl) hydrofuroin from HMF. Mechanistic analyses revealed that moderate hydrogen adsorption capacity on electrode surfaces enhances aldehyde coupling and suppresses competing hydrogenation pathways. Consequently, this mild electrochemical route offers clear advantages over thermochemical upgrading, including operational simplicity, environmental compatibility, and integration with renewable energy sources. These findings not only underscore the feasibility of electrochemical dimerization for biomass upgrading but also establish a robust basis for developing sustainable aviation fuels.

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ANALYTICAL CHEMISTRY · 2013 · IF 5.695

Hydrophilic Material for the Selective Enrichment of 5-Hydroxymethylcytosine and Its Liquid Chromatography–Tandem Mass Spectrometry Detection

Yang Tang,Jie-Mei Chu,Wei Huang,Jun Xiong,Xi-Wen Xing,Xiang Zhou,Yu-Qi Feng,Bi-Feng Yuan

5-Methylcytosine (5-mC), an important epigenetic modification involved in development, can be converted enzymatically to 5-hydroxymethylcytosine (5-hmC). 5-hmC is considered an intermediate of active DNA cytosine demethylation and makes itself serve as an epigenetic mark. 5-hmC content in most mammalian cells is low and the quantification of 5-hmC by liquid chromatography–mass spectrometry (LC–MS) frequently suffers from ion suppression by the presence of unmodified nucleosides. To circumvent this problem, we developed a method to selectively transfer a glucosyl group to the hydroxymethyl moiety of 5-hmC and form a more hydrophilic residue (β-glucosyl-5-hydroxymethyl-2′-deoxycytidine, 5-gmdC) by using T4 β-glucosyltransferase. The more hydrophilic 5-gmdC can be selectively enriched by using NH2-silica via hydrophilic interaction prior to liquid chromatography–tandem mass spectrometry (LC–MS/MS) analysis, which eliminates the ion suppression and significantly improves the detection sensitivity and accuracy. Using this method, we successfully quantified 5-hmC content in genomic DNA of three human cell lines and seven yeast strains. To the best of our knowledge, this is the first report about the existence of 5-hmC in the model organism of yeast. In addition, the contents of 5-hmC in two yeast strains of Schizosaccharomyces pombe are even higher than those of 5-mC, indicating that 5-hmC may play important roles on the physiological functions of yeast.

研究领域: 表观遗传学 · 分析化学 · 生物化学
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Frontiers of Chemical Science and Engineering · 2024 ·Vol. 18 ·期 8 ·1-12 · IF 4.3

Solid-conversion synthesis of three-dimensionally ordered mesoporous ZSM-5 catalysts for the methanol-to-propylene reaction

Chun Weilong,Yang Chenbiao,Wang Xu,Yang Xin,Chen Huiyong

A facile synthesis of hierarchical ZSM-5 with the three-dimensionally ordered mesoporosity (3DOm ZSM-5) was achieved by solid conversion (SC) of SiO 2 colloidal crystals to high-crystalline ZSM-5. The products of 3DZ5_S/C and 3DZ5_S, which were severally transformed from the carbon-padded SiO 2 colloidal crystals and the initial SiO 2 colloidal crystals, exhibited not only a similar ordered structure and acidity but also higher crystallinity and more balanced meso-/micropore combination in comparison with 3DZ5_C obtained by the conventional confined space crystallization approach. All three synthesized 3DZ5 catalysts showed improved methanol-to-propylene performance than the commercially microporous ZSM-5 (CZ5), embodied in five times longer lifetime, higher propylene selectivity and S propylene / S ethylene ratio ( P/E ), and superior coke toleration with lower formation rate of coke ( R coke ). Moreover, the 3DZ5_S catalyst in situ converted from SiO 2 colloidal crystals presented the highest selectivities of propylene (42.51%) and light olefins (74.6%) among all three 3DZ5 catalysts. The high efficiency in synthesis and in situ utilization of SiO 2 colloidal crystals demonstrate the proposed SC strategy to be more efficiently and eco-friendly for the high-yield production of not only 3DOm ZSM-5 but also other types of hierarchical zeolites.

研究领域: 材料科学 · 催化化学 · 能源化学
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Materials Chemistry Frontiers · 2021 ·Vol. 5 ·期 18 ·7032-7040 · IF 6.482

Highly sensitive detection of paraquat with pillar[5]arenes as an aptamer in an α-hemolysin nanopore

Xiaojia Jiang,Mingsong Zang,Fei Li,Chunxi Hou,Quan Luo,Jiayun Xu,Junqiu Liu

Recently, biological nanopore-based techniques have attracted more and more attention in the field of single-molecule detection because they allow real-time, sensitive, high-throughput analysis. Herein, we report an engineered biological nanopore sensor by introducing a macrocyclic host molecule carboxylatopillar[5]arene (CP[5]A) that acts as an aptamer into the lumen of a mutant (E111R/K147R)7 αHL nanopore for detecting highly toxic paraquat (PQ) via host–guest interactions at the single-molecule level. By taking advantage of introducing positively charged arginine (Arg) into the lumen of the αHL nanopore, our engineered nanopore sensor exhibits higher stability. More importantly, this nanopore sensor shows high sensitivity, and the limit of detection (LOD) for PQ can reach a nanomolar level of 0.37 ppb. The CP[5]A-based nanopore sensing strategy developed in this work may bring inspiration for single-molecule detection and hold great potential in public health applications.

研究领域: 纳米技术 · 分析化学 · 生物技术 · 毒理学
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Materials Today Sustainability · 2023 · IF 7.8

Facile fabrication of a plate-like ZSM-5 zeolite as a highly efficient and stable catalyst for methanol to propylene conversion

W. Dai,L. Zhang,R. Liu,Z. Huo,W. Dai,N. Guan

Zeolite catalysts with high propylene selectivity and superior stability are highly desirable in the methanol to propylene (MTP) conversion. Herein, plate-like MFI zeolites with different Si/Al (Ga) ratios were successfully prepared via a fluoride assisted strategy and applied in the MTP reaction. The influences of the zeolite morphology, acid density, and strength on the MTP activity as well as the reaction mechanism were clarified by combining spectroscopic and catalytic results. The plate-like MFI zeolites with lower acid density could efficiently suppress the aromatic-based cycle and promote the olefin-based cycle and thus exhibited a remarkable catalytic performance in the MTP conversion. However, owing to occurrence of irreversible hydrolysis of the Si-OH-Ga group during the MTP conversion, the catalytic activity of the Ga-MFI catalyst was not recyclable. On the contrary, the plate-like ZSM-5 catalyst shows excellent stability and recyclability in the MTP conversion.

研究领域: 催化化学 · 能源化工 · 材料科学 · 石油化工 · 工业催化
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RSC Advances · 2014 ·Vol. 5 ·期 5 ·3792-3798 · IF 3.708

Solvothermal synthesis of hydroxyapatite nanostructures with various morphologies using adenosine 5′-monophosphate sodium salt as an organic phosphorus source

Chao Qi,Ying-Jie Zhu,Guan-Jun Ding,Jin Wu,Feng Chen

In this paper, we report a simple and green strategy for the synthesis of hydroxyapatite (HAP) nanostructures with various morphologies (including nanoparticles, microtubes, nanorods and nanorod-assembled flower-like hierarchical structures) using adenosine 5′-monophosphate sodium salt (AMP) as an organic phosphorus source by solvothermal treatment in different solvents. The effects of the solvents and the reaction time on the morphology of the product as well as the formation mechanism of HAP nanostructures are investigated. In this strategy, the AMP biomolecules act as an organic phosphorus source for the formation of HAP nanostructures, and the solvents have effects on the morphology of the product. This strategy is environmentally friendly and surfactant-free. The as-prepared products are characterized by X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM) and thermogravimetric analysis (TG).

研究领域: 材料科学 · 生物医学工程
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