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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Reaction rate enhancement by reducing surface diffusion barriers of guest molecules over ZSM-5 zeolites: a structured illumination microscopy study

Shichao Peng,Hua Li,Wenjuan Liu,Junyi Yu,Zhaochao Xu,Mao Ye,Zhongmin Liu

Mass transfer of guest molecules is crucial for zeolite catalysis. Compared to intracrystalline diffusion, the surface barriers in zeolite catalysis have been less understood. Taking furfuryl alcohol oligomerization catalyzed by ZSM-5 zeolites as model reaction, here we present a single-crystal level study and gain insight into the surface barriers induced spatiotemporal evolution of oligomer products using structured illumination microscopy (SIM). It is shown that, as a result of the enhanced accessibility to zeolite crystals, promoting the surface permeability leads to the increase in catalytic reaction rate that is characterized as the generation rate of oligomer products.

研究领域: 催化化学 · 材料科学 · 物理化学 · 纳米催化 · 多相催化 · 分子筛催化 · 原位表征技术
✓ 已验证 DOI 高影响因子
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2024 ·Vol. 31 ·期 16 ·24398-24411 · IF 0

Structural/surface characterization of transition metal element–doped H-ZSM-5 adsorbent for CH3SH removal: identification of active adsorption sites and deactivation mechanism

Xie Yuxuan,Peng Xiao,Song Xin,Ning Ping,Sun Xin,Ma Yixing,Wang Chi,Li Kai

CH 3 SH is a potential hazard to both chemical production and human health, so controlling its emissions is an urgent priority. In this work, a series of transition metal-loaded H-ZSM-5 adsorbents (Si/Al = 25) (Cu, Fe, Co, Ni, Mn, and Zn) were synthesized through the wet impregnation method and tested for CH 3 SH physicochemical adsorption at 60 °C. It was shown that the Cu-modified H-ZSM-5 adsorbent was much more active for CH 3 SH removal due to its abundant strong acid sites than other transition metal-modified H-ZSM-5 adsorbents. The detailed physicochemical properties of various modified H-ZSM-5 adsorbents were characterized by SEM, XRD, N 2 physisorption, XPS, H 2 -TPR, and NH 3 -TPD. The effects of metal loading mass ratio, calcination temperature, and acid or alkali modification on the performance of the adsorbent were also investigated, and finally 20% Cu/ZSM-5 was found to have the best adsorption capacity after calcined at 350 °C. Additionally, the Cu/ZSM-5 adsorbent modified by sodium bicarbonate could expose more active components, which improved the adsorbent’s stability. However, the consumption and reduction of the active component Cu 2+ and the accumulation of sulfate during the adsorption process are the main reasons for the deactivation of the adsorbent. In addition, the simultaneous purging of N 2  + O 2 can effectively restore the adsorption capacity of the deactivated adsorbent and can be used as a potential strategy to regenerate the adsorbent. Graphical

研究领域: 环境科学 · 材料化学 · 催化 · 吸附技术 · 化学工程
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ACS Applied Energy Materials · 2022 · IF 6.959

Performance Improvement of Li6PS5Cl Solid Electrolyte Modified by Poly(ethylene oxide)-Based Composite Polymer Electrolyte with ZSM-5 Molecular Sieves

Changfei Zou,Li Yang,Kaili Luo,Lei Liu,Xiyuan Tao,Lingguang Yi,Xianhu Liu,Zhigao Luo,Xianyou Wang

All-solid-state lithium metal batteries (ASSLMBs) with argyrodite-type Li6PS5Cl solid electrolyte (SE) show potential to replace current commercially available lithium-ion batteries by virtue of their potentially high energy density and safety. However, the interface incompatibility between sulfide solid electrolyte and lithium metal leads to an increase in interfacial resistance and the rapid growth of lithium dendrites, which greatly impede its commercial application. To alleviate the above problems, here a cell construction model has been put forward, in which composite polymer electrolytes (CPEs) with high ionic conductivity and good interface compatibility against lithium metal are employed as the interphase between Li6PS5Cl solid electrolyte and lithium metal. CPEs can prevent direct contact between lithium anode and Li6PS5Cl, and a soft CPE layer can solve the problem of high interfacial resistance caused by bad contact between the Li6PS5Cl solid electrolyte and the lithium metal anode. As a result, the symmetric cells Li/CPEs/Li6PS5Cl/CPEs/Li show stable polarization voltage over 140 h at a current density of 0.2 mA at 60 °C. Compared with the rapidly decaying capacity of the LiFePO4/Li6PS5Cl/Li cell, the initial discharge capacity of LiFePO4/Li6PS5Cl/CPEs/Li is 93.74 mAh/g, and after 15 cycles at 0.5 C, the capacity retention rate is still 75.1%. Therefore, the successful design of this cell structure based on the interface modification of Li6PS5Cl solid electrolyte provides good prospects for the commercial application of ASSLMBs.

研究领域: 材料科学 · 电化学 · 能源存储 · 固体离子学 · 电池技术 · 界面工程
✓ 已验证 DOI 高影响因子
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MEDICINAL CHEMISTRY RESEARCH · 2018 ·Vol. 28 ·期 2 ·133-142 · IF 1.607

Novel anti-cancer agents: design, synthesis, biological activity, molecular docking, and MD simulations of 2, 3, 4, 5-tetrahydro-1H-pyrido-[4,3-b]indole derivatives

Feng Yu,Teng Xingxing,Gu Jinhua,Yu Bangwei,Luo Yan,Ye Lianbao

In the previous research, our group designed and synthesized 2,3,4,5-tetrahydro-1 H -pyrido-[4,3-b] indoles, which showed high anti-tumor activity. In this study, a series of novel 2,3,4,5-tetrahydro-1 H -pyrido-[4,3-b] indole derivatives were designed by introducing an alkyl or aralkyl and a sulfonyl group, which are considered as the pharmacophores of some antitumor drugs based on the combination principles, and synthesized. The antiproliferative activity of all the target compounds were evaluated against Hela, A549, HepG2, and MCF-7 cell lines using the MTT assay in vitro. The results were represented by IC 50 values. All compounds showed moderate to excellent antiproliferative activity with IC 50 values between 0 μM and 100 μM against cancer cells. The proliferations of Hela, A549, HepG2, and MCF-7 cell lines were inhibited in a dose-dependent manner, and the cytolytic activity was markedly inhibited at the same time. The IC 50 values of intermediate 3 inhibited against Hela, A549, HepG2, and MCF-7 cell lines were 52.75, 50.30, 60.31, and 54.39 μM, respectively, which were higher than the new compounds that we expected. The compounds 4a – 4d bearing sulfonyl, substituted by electron donating group, showed moderate to significant antiproliferative activity, in which compound 4c was the best with the IC 50 values of 13.71, 9.42, 15.06, and 14.77 μM, and these results suggested that the introduction of sulfonyl could increase the antiproliferative activity of 2,3,4,5-tetrahydro-1 H -pyrido-[4,3-b]indole. Compounds 4e – 4g bearing alkyl, phenyl, and arylated alkyl produced good antiproliferative activity and the IC 50 value of 4 g was lower than 30 μM. The target compounds were more potent against A549 compared to the other three cell lines. Molecular docking studies revealed the binding orientations of all the synthesized compounds in the active site of c-Met. Moreover, molecular dynamics simulations have been performed to evaluate the binding stabilities between the synthesized compounds and their receptors.

研究领域: 药物化学 · 肿瘤学 · 计算生物学
✓ 已验证 DOI 高影响因子
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FUEL · 2025 · IF 7.5

A tandem system of Cr/HZSM-5 and bismuth-modified CeZrO2 for coupling of ethane dehydrogenation to selective H2 combustion

Ying Li,Haibo Zhao

Ethylene production via chemical looping oxidative dehydrogenation (CL-ODH) of ethane faces a critical challenge in balancing conversion efficiency and selectivity due to competing oxygen species requirements. Here, we present a bifunctional composite catalyst (CrH/BiCZ) by physically integrating a Cr-HZSM5 (Cr-H) dehydrogenation (DH) catalyst with a Bi 2 O 3 -Ce 0.4 Zr 0.6 O 2 (Bi-CZ) selective hydrogen combustion (SHC) catalyst. This tandem system decouples ethane activation and hydrogen combustion, promoting the DH process of ethane through the in situ hydrogen combustion of the SHC catalyst. The Ce-Zr solid solution in Bi-CZ acts as an oxygen reservoir, enabling complete H 2 combustion within 3 min and suppressing carbon deposition. This rapid hydrogen combustion shifts the reaction equilibrium towards ethylene production. At 650 °C, the optimized CrH/BiCZ catalyst achieves 84.1 % ethylene selectivity at 43.0 % ethane conversion, and maintains exceptional stability over 36 redox cycles. This work establishes a scalable chemical looping strategy for efficient ethylene synthesis.

CAS / MDL: 10294-41-4
研究领域: 催化 · 化学工程 · 材料科学 · 反应工程 · 能量转换
✓ 已验证 产品关联 DOI 高影响因子
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Frontiers in Chemistry · 2021 · IF 5.221

Immobilized Crosslinked Pectinase Preparation on Porous ZSM-5 Zeolites as Reusable Biocatalysts for Ultra-Efficient Hydrolysis of β-Glycosidic Bonds

Liu Can,Zhang Liming,Tan Li,Liu Yueping,Tian Weiqian,Ma Lanqing

In this study, we immobilized pectinase preparation on porous zeolite ZSM-5 as an enzyme carrier. We realized this immobilized enzyme catalyst, pectinase preparation@ZSM-5, via a simple combined strategy involving the van der Waals adsorption of pectinase preparation followed by crosslinking of the adsorbed pectinase preparation with glutaraldehyde over ZSM-5. Conformal pectinase preparation coverage of various ZSM-5 supports was achieved for the as-prepared pectinase preparation@ZSM-5. The porous pectinase preparation@ZSM-5 catalyst exhibited ultra-efficient biocatalytic activity for hydrolyzing the β-glycosidic bonds in the model substrate 4-nitrophenyl β-D-glucopyranoside, with a broad operating temperature range, high thermal stability, and excellent reusability. The relative activity of pectinase preparation@ZSM-5 at a high temperature (70 °C) was nine times higher than that of free pectinase preparation. Using thermal inactivation kinetic analysis based on the Arrhenius law, pectinase preparation@ZSM-5 showed higher activation energy for denaturation (315 kJ mol−1) and a longer half-life (62 min−1) than free pectinase preparation. Moreover, a Michaelis–Menten enzyme kinetic analysis indicated a higher maximal reaction velocity for pectinase preparation@ZSM-5 (0.22 µmol mg−1 min−1). This enhanced reactivity was attributed to the microstructure of the immobilized pectinase preparation@ZSM-5, which offered a heterogeneous reaction system that decreased the substrate–pectinase preparation binding affinity and modulated the kinetic characteristics of the enzyme. Additionally, pectinase preparation@ZSM-5 showed the best ethanol tolerance among all the reported pectinase preparation-immobilized catalysts, and an activity 247% higher than that of free pectinase preparation at a 10% (v/v) ethanol concentration was measured. Furthermore, pectinase preparation@ZSM-5 exhibited potential for practical engineering applications, promoting the hydrolysis of β-glycosidic bonds in baicalin to convert it into baicalein. This was achieved with a 98% conversion rate, i.e., 320% higher than that of the free enzyme.

研究领域: 生物化学 · 酶学 · 催化 · 材料科学 · 生物技术
✓ 已验证 DOI PubMed 高影响因子
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Photodiagnosis and Photodynamic Therapy · 2020 · IF 2.894

Chemo-photodynamic therapy by pulmonary delivery of gefitinib nanoparticles and 5-aminolevulinic acid for treatment of primary lung cancer of rats

Tongtong Zhang,Jianwei Bao,Mengmeng Zhang,Yuanyuan Ge,Jianming Wei,Yu Li,Weixia Wang,Miao Li,Yiguang Jin

Lung cancer is a severe disease with high mortality. Chemotherapy is one major treatment for lung cancer. However, systemic chemotherapeutics usually distribute throughout the body without specific lung distribution so that serious side effects are unavoidable. Photodynamic therapy (PDT) is occasionally used for lung cancer treatment but photosensitizers are also systemically administered and the bronchoscopic intervention under anesthesia may hurt lung tissues. Here, we combined inhaled chemotherapeutics and photosensitizers for chemo-photodynamic therapy (CPDT) of primary lung cancer of rats with external laser light irradiation. Gefitinib PLGA nanoparticles (GNPs) were prepared. The anti-cancer effects of GNPs and/or a common photosensitizer 5-aminolevulinic acid (5-ALA) were explored on A549 cells (adenocarcinomic human alveolar basal epithelial cells) and primary lung cancer rats after intratracheal administration. External light irradiation was applied due to its higher safety compared to internal light irradiation that may result in injuries after a laser optic fiber was intubated into the lung. The remarkable synergistic effect of CPDT was confirmed although the single therapies were also effective, where the high anti-lung cancer effects were shown and some typical lung cancer markers, including CD31, VEGF, NF-κB p65 and Bcl-2, significantly decreased. Moreover, the treatments attenuated inflammation with the downregulation of TNF-α. The combination of pulmonary drug delivery and chemo-photodynamic therapy is a promising strategy for treatment of lung cancer.

研究领域: 肿瘤学 · 药学 · 生物医学工程 · 分子生物学
✓ 已验证 DOI PubMed 高影响因子
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS · 2022 ·Vol. 25 ·期 1 ·402-409 · IF 3.945

Excited state proton transfer in the triplet state of 8-hydroxy-5-nitroquinoline: a transient absorption and time-resolved resonance Raman spectroscopic study

Ran Wang,Fengjin Zhang,Xinghang Pan,Xuming Zheng,Jiadan Xue,Yong Du,Binbin Xie

8-Hydroxy-5-nitroquinoline (NO2-QN-OH) is an antimicrobial, anti-inflammatory and anticancer agent, and has been approved for use in the treatment of diseases. Its photosensitivity, however, cannot be overlooked. The photochemistry of 8-hydroxy-5-nitroquinoline in acetonitrile is investigated using transient absorption and time-resolved resonance Raman spectroscopies. By identifying the short-lived intermediates during the photoreaction, it is clear that the Tn state NO2-QN-OH is generated in 0.8 ps via an ultrafast ISC, followed by the IC in 8.5 ps to produce the T1 state. In neat acetonitrile, the T1 state NO2-QN-OH undergoes intramolecular proton transfer and tautomerizes to form T1 state NO2-QNH-O. To our knowledge, this is the first time that the intramolecular excited state proton transfer of hydroxyl-quinolines in an aprotic polar solvent is observed.

研究领域: 光化学 · 物理化学 · 光谱学
✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

Enhanced electricity production in single-chamber MFCs with air cathodes decorated by Fe–N–C catalysts derived from 5H-dibenz [b,f] azepine-5-carboxamide (Carbamazepine)

Wenyu He,Jinhui Wei,Ting Huang,Enren Zhang

For practical applications of microbial fuel cells (MFCs), 5H-dibenz [b,f] azepine-5-carboxamide (Carbamazepine, CBZ) was used as the organic precursor for the synthesis of catalysts composed of Fe–N–C complexes (named as Fe-CBZ-Cats) through a sacrificial support method. Characterizations by SEM, XPS and TEM-EDS elemental mapping show that the synthesized Fe-CBZ-Cats have porous structure and uniformly dispersed Fe/N/C complex centers which could play key roles in effective ORR . Linear scanning voltammetry (LSV) measurements show that the synthesized Fe-CBZ-Cats exhibits ORR activity comparable to commercial Pt/C catalysts under the same catalyst loading (2 mg cm −2 ). The maximum power density produced by cathode-limiting MFCs with Fe-CBZ-Cats air cathodes was 431 ± 23 μW cm −2 , higher than those in the control MFCs with Pt/C air cathodes (403 ± 13 μW cm −2 ) and activated carbon air cathodes (296 ± 24 μW cm −2 ). In addition, the toxicity tolerance of the synthesized Fe-CBZ-Cats is much higher than Pt/C.

研究领域: 环境科学 · 电化学 · 生物工程
✓ 已验证 DOI 高影响因子
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BIOORGANIC CHEMISTRY · 2020 · IF 4.831

Design, synthesis and biological evaluation of novel 7H-benzo [c] [1, 3] dioxolo [4, 5-f] chromen-7-one derivatives with potential anti-tumor activity

Shiyang Zhou,Gangliang Huang

In this study, a series of novel 7 H -benzo [ c ] [1,3] dioxolo [4, 5- f ] chromen-7-one derivatives were obtained by structural modification of the lead compounds with Fissitungfine B. A total 15 compounds were designed, synthesized and evaluated as inhibitors of tumor. These target compounds have the novel chemical structures that named three six-membered rings including one lactone six-membered ring. In vitro assay, the results showed that the target compounds have a broad spectrum and strong of anti-tumor activity. Such as the target compound 4n to MCF-7 was IC 50  = 0.35 ± 0.01 μM, to A-549 was IC 50  = 0.37 ± 0.01 μM, to Hela was IC 50  = 0.56 ± 0.02 μM, to MDC-803 was IC 50  = 0.53 ± 0.02 μM and COLO-205 was IC 50  = 0.50 ± 0.02 μM in vitro . At the same time, in vivo anti-tumor activity assay results showed that the target compounds had a good inhibitory effect on tumor growth. Among them, the target compound 4n had the best anti-tumor activity, it could inhibit tumor growth well at a low dose. The target compound 4n could be used as a candidate drug for further research and development, in order to be used as early as application in the clinical treatment of tumors.

研究领域: 药物化学 · 肿瘤学 · 有机合成
✓ 已验证 DOI PubMed 高影响因子
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Catalytic Upgrading of Cellulose Pyrolysis Volatiles over Ce Modified Hierarchical ZSM-5 Zeolite: Insight into the Effect of Acid Properties on Light Aromatics and Catalyst Stability

Li-Yun Zhang,Jing-Pei Cao,Xue-Yu Ren,Xiao-Bo Feng,Jing-Xian Wang,Zi-Meng He,Tian-Long Liu,Zhen Yang,Xiao-Yan Zhao,Hong-Cun Bai

CeO2 receives extensive researches as an active component due to its providential catalytic center and favorable reducibility. Herein, a series of Ce-modified hierarchical ZSM-5 zeolites (FZ5) were prepared by HF (0.5 mol/L) etching followed by impregnation with different Ce loadings. The role of incorporating extra-framework Ce elements was assessed by catalytic upgrading of the cellulose pyrolysis volatiles to produce light aromatics (LAs). Introducing CeO2 could effectively regulate the acid properties of catalysts with an increase in Lewis acid sites and a decrease in Brönsted acid sites, which could significantly improve the catalytic performance. As a result, the selectivity toward LAs were significantly enhanced and the coke content dramatically decreased. The highest selectivity to LAs and the lowest coke content obtained over 1.0Ce-FZ5 zeolite (loading 1.0 wt % Ce) were 84.0% and 2.42 wt %, respectively. Additionally, the 1.0Ce-FZ5 catalyst exhibited excellent stability, maintaining nearly 90% carbon yield of LAs after the seventh regeneration test. CeO2 modification opened a simple and feasible way for promoting the LAs selectivity and catalyst stability during the reforming of biomass volatiles.

研究领域: 催化化学 · 生物质能源 · 材料化学 · 环境科学 · 能源化工
✓ 已验证 DOI 高影响因子
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JOURNAL OF MEDICINAL CHEMISTRY · 2024 · IF 6.8

Allosteric Activation of α7 Nicotinic Acetylcholine Receptors by Novel 2-Arylamino-thiazole-5-carboxylic Acid Amide Derivatives for the Improvement of Cognitive Deficits in Mice

Chenxia Yang,Ying Meng,Xintong Wang,Xin Li,Tong Yu,Weiming Liao,Wenjun Xie,Qianchen Jiang,Han Wang,Cheng Shi,Wenxuan Jiao,Xiling Bian,Fang Hu,Xiaowei Wang,Yani Liu,Liangren Zhang,KeWei Wang,Qi Sun

Enhancing α7 nAChR function serves as a therapeutic strategy for cognitive disorders. Here, we report the synthesis and evaluation of 2-arylamino-thiazole-5-carboxylic acid amide derivatives 6–9 that as positive allosteric modulators (PAMs) activate human α7 nAChR current expressed in Xenopus ooctyes. Among the 4-amino derivatives, a representative atypical type I PAM 6p exhibits potent activation of α7 current with an EC50 of 1.3 μM and the maximum activation effect on the current over 48-fold in the presence of acetylcholine (100 μM). The structure–activity relationship (SAR) analysis reveals that the 4-amino group is crucial for the allosteric activation of α7 currents by compound 6p as the substitution of 4-methyl group results in its conversion to compound 7b (EC50 = 2.1 μM; max effect: 58-fold) characterized as a typical type I PAM. Furthermore, both 6p and 7b are able to rescue auditory gating deficits in mouse schizophrenia-like model of acoustic startle prepulse inhibition.

研究领域: 神经科学 · 药物化学
✓ 已验证 DOI PubMed 高影响因子
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