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CRYSTENGCOMM · 2020 ·Vol. 22 ·期 23 ·4005-4013 · IF 3.117

Engineering CuOx–ZrO2–CeO2 nanocatalysts with abundant surface Cu species and oxygen vacancies toward high catalytic performance in CO oxidation and 4-nitrophenol reduction

Baolin Liu,Yizhao Li,Shaojun Qing,Kun Wang,Jing Xie,Yali Cao

Highly dispersed surface Cu species and oxygen vacancies are important for CuOx–CeO2 catalysts in many reactions, but it is difficult to increase the concentrations of highly dispersed Cu species and oxygen vacancies simultaneously by only adding a Cu component. Herein, CuOx–ZrO2–CeO2 (CZC) nanocatalysts with different ratios of Cu/Zr have been effectively produced by a simple solvent-free synthetic strategy. The effect of Zr doping on the structure and reactivity of the CuOx–CeO2 catalysts has been investigated with the help of carbon monoxide (CO) oxidation and 4-nitrophenol (4-NP) reduction as model reactions. It is revealed that the introduction of Zr relieved the agglomeration of surface Cu species, produced more oxygen vacancies in the interior and Cu+ species on the surface of the catalyst, and increased the reducibility of CuOx–CeO2. The CZC catalysts show remarkably enhanced catalytic activity due to the abundant surface active sites and the improved redox properties provided by the suitable doping of Zr into CuOx–CeO2. This work not only offers a practicable way to reconstruct the distribution of active metals on the metal oxide support but also provides a high-efficiency strategy to prepare oxide catalysts with excellent catalytic performance.

✓ 已验证 DOI 高影响因子
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CHEMOSPHERE · 2018 · IF 4.427

Synergistic effects in iron-copper bimetal doped mesoporous γ-Al2O3 for Fenton-like oxidation of 4-chlorophenol: Structure, composition, electrochemical behaviors and catalytic performance

Zhuangpeng Huang,Zhiping Chen,Yuancai Chen,Yongyou Hu

Iron-copper bimetal supported on mesoporous γ-Al 2 O 3 with different Fe/Cu ratios was prepared via a modified evaporation-induced self-assembly method and employed to degrade 4-chlorophenol (4-CP) in a Fenton-like process. The X-ray photoelectron spectroscopy, X-ray diffraction spectrum and UV–vis diffuse reflectance spectroscopy results confirmed the co-doping of Fe 2+ /Fe 3+ and Cu + /Cu 2+ into the lattice of γ-Al 2 O 3 through the bonds of Al O Fe and Al O Cu. With the iron and copper co-doped in γ-Al 2 O 3 , three-fold oxygen vacancies (V 0 ) could be achieved compared with that of non-metal catalysts, which was favorable for the reduction of iron and copper species. The 1Fe3Cu-γ-Al 2 O 3 with a Fe/Cu mass ratio of 1:3 exhibited the highest activity on Fenton-like degradation of 4-CP due to the synergistic effects of Fe and Cu by facilitating the electron transfer in the recycles of Cu + /Cu 2+ and Fe 2+ /Fe 3+ based on the results of X-ray photoelectron spectroscopy, cyclic voltammetry and electro paramagnetic resonance analysis. The utilization efficiency of H 2 O 2 was as high as 86.0% when 4-CP almost disappeared (i.e., 99.7 percent of 0.78 mM 4-CP) at 240 min and pH 7.0, additionally, their dechlorination and TOC removal efficiencies were 92.0% and 81.6%, respectively. The catalyst also displayed a good performance after 5th cycles. Furthermore, a possible mechanism for activation of OH on the catalyst surface was also proposed.

✓ 已验证 DOI 高影响因子
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JOURNAL OF ORGANIC CHEMISTRY · 2020 · IF 4.335

Regioselective Reversal Cyclization To Access either Eight-Membered Sulfur-Containing Heterocycle-Fused γ-Pyrones or 2-(1,4-Dithianyl)-4-pyrones from the Same Precursors

Ling Tang,Qin Yang,Jianfang Zhang,Guisheng Deng

A regioselective reverse strategy for the construction of eight-membered sulfur-containing heterocycle-fused γ-pyrones and 2-(1,4-dithianyl)-4-pyrones starting from 2-diazo-γ-pyrones and dithioacetals was achieved for the first time. The process combines C–S bond formation via sulfur ylides and C–C bond formation via electron transfer to afford the target molecules in a facile manner with 100% regioselectivity and in excellent isolated yields (up to 90%).

✓ 已验证 DOI 高影响因子
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Bioresource Technology Reports · 2018 · IF 0

Pretreatment of bamboo shoot shell with surfactant OP-10 in the acidified media for enhancing the biosynthesis of ethyl (S)-4-chloro-3-hydroxybutanoate

Bing-Qian Wang,Bo Peng,Jian-Fei Sun,Chu Wang,Ke Jiang,Jing-Hao Ma,Peng-Qi Zhang,Yu-Cai He

An effecti v e combination pretreatment of bamboo shoot shell (BSS) using Emulsifier OP-10 (0.5%, w/v) in the acidified media (pH 4.0) by autoclaving (120 °C, 40 min) was conducted. After BSS slurry without detoxification was enzymatically hydrolyzed for 96 h, glucose (25.2 g/L) and xylose (7.5 g/L) were obtained from 50 g/L BSS at high yields. HPLC results showed that no potential inhibitors (furfural and 5-hydroxymethylfurfural) formed. In the hydrolysates , an effective biocatalytic synthesis of ethyl ( S )-4-chloro-3-hydroxybutanoate (100% yield; >99% e.e. ) from 1000 mM ethyl 4-chloro-3-oxobutanoate was developed without the extra addition of cofactors within 24 h. In summary, this combination strategy involving biomass pretreatment, enzymatic saccharification , and bioreduction can be developed for producing chiral alcohols.

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ChemCatChem · 2024 ·Vol. 16 ·期 21 ·e202401010 · IF 3.8

Synthesis of Chabazite Zeolite via Faujasite Conversion Using 1-(1-Methylpropyl)-4-aza-1-azoniabicyclo[2.2.2]octane Hydroxide as Cost-Effective Structure-Directing Agent

Ziwei Wu,Han Sun,Quanzheng Deng,Lu Han,Penggang Lv,Haijun Chen,Hongchang Duan,Kake Zhu

Graphical Mono-quaternary 1-(1-methylpropyl)-4-aza-1-azoniabicyclo[2.2.2]octane hydroxide is proposed to direct the Faujasite-to-Chabazite inter-zeolite conversion to generate 35–258 nm CHA crystals with Si/Al ratio of 7.2. The Cu-CHA zeolite exhibits superior hydrothermal stability and catalytic performance in standard NH 3 -SCR process. Cu-exchanged chabazite zeolite is the state-of-the-art used on-board catalyst for NO x selective reduction by ammonium (NH 3 -SCR), and the zeolite is currently generated in the presence of N , N , N -trimethyl-1-adamantylammonium hydroxide, serving as organic structure-directing agent (OSDA). The expensiveness of this OSDA increases the catalyst production cost, while its low degradability brings about environmental concerns in post treatment of waste water. Here, a new type OSDA, 1-(1-methylpropyl)-4-aza-1-azoniabicyclo[2.2.2]octane hydroxide, is proposed to direct Faujasite-to-Chabazite inter-zeolite conversion and generate chabazite with Si/Al ratio up to 7.2. The obtained zeolite possesses high hydrothermal stability for the high crystallinity, siliceous framework and low concentrations of Si(2Si, 2Al) sites. The Cu-form catalyst exhibits better catalytic performance in standard NH 3 -SCR process for the tiny crystallite size (35–258 nm) and formation of highly dispersed copper sites. The synthesis offers a new type of OSDA to fabricate zeolites and expands the toolkit to regulate their physicochemical properties.

✓ 已验证 DOI 高影响因子
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INORGANIC CHEMISTRY COMMUNICATIONS · 2025 · IF 5.4

Cyclometalated Ir(III) complexes based on 3,8-di(1H-pyrazol-4-yl)-1,10-phenanthroline: Acid/base-induced luminescence transformation and Cu2+-induced luminescence switching

Yi-Heng Wang,Yang Liu,Jin Tong,Shu-Yan Yu

The cyclometalated Ir(III) complex, Ir(ppy) 2 (phen-dipzH 2 ) ( Ir-1 ), was synthesized using the ligand 3,8-di(1H-pyrazol-4-yl)-1,10-phenanthroline (phen-dipzH 2 ) and the auxiliary ligand 2-phenylpyridine (ppy). Crystal structure analysis reveals that each {Ir(ppy) 2 } + unit is coordinated by a neutral phen-dipzH 2 ligand in Ir-1 . The packing arrangement of Ir-1 displays aromatic stacking interactions and [C–H…N] hydrogen bonding interactions between the [Ir(ppy) 2 (phen-dipzH 2 )] + cations. In solution, Ir-1 exhibits emission switching induced by acid/base changes, with the emission wavelength shifting from 562 nm (yellow color) in the neutral state to 618 nm (pink color) under acidic conditions and to 528 nm (gray color) under basic conditions. These shifts are attributed to the protonation and deprotonation of the pyrazole units, which is confirmed by 1 H NMR spectra. Additionally, Ir-1 demonstrates high selectivity and sensitivity toward Cu 2+ ions, with a detection limit as low as 9.47 μM compared to other metal ions. The acid/base-responsive phosphorescence of Ir-1 has also been successfully utilized in the development of paper strip-based devices for urea detection.

✓ 已验证 DOI 高影响因子
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COMPARATIVE BIOCHEMISTRY AND PHYSIOLOGY C-TOXICOLOGY & PHARMACOLOGY · 2024 · IF 3.9

Environmental endocrine disrupting chemical 4-tert-butylphenol induced calcium overload and subsequent autophagy impairment via miRNA-363/CACNA1D Axis in epithelioma papulosum cyprini cells

Jiawen Cui,Zhenda Liang,Yuhao Liu,Zhiyu Hao,You Tang,Li Zhou,Xiaohua Teng

Environmental endocrine disrupting chemical 4-tert-butylphenol (4-tBP), a widely-utilized surfactant in various industries, poses potential risks to aquatic organisms. Our previous sequencing results suggested that 4-tBP-induced common carp liver injury might be associated with Ca 2+ signaling and autophagy. However, the intricate involvement of these pathways in 4-tBP-induced cytotoxic mechanisms remained unexplored. To bridge these knowledge gaps, this study focused on epithelioma papulosum cyprini (EPC) cells, a significant cell type in fish biology. Initial observations showed that 4-tBP induced a dose-dependent perturbation in Ca 2+ levels. Further investigations, with siRNA and L-type Ca 2+ channel agonist (BAY K8644), identified L-type calcium channel gene CACNA1D as a critical regulator of 4-tBP-induced Ca 2+ overload. Predictive analysis using miRanda platform suggested a potential interaction between miR-363 and CACNA1D, which was subsequently verified through dual-luciferase reporter gene assays. We then established miR-363 mimic/inhibitor models, along with miR-363 and CACNA1D co-suppression models in EPC cells. Through TEM observation, immunofluorescence assay, Ca 2+ staining, and qRT-PCR analysis, we evaluated the role of miR-363/CACNA1D axis in modulating the effects of 4-tBP on Ca 2+ signaling and autophagy. Results showed that miR-363 inhibitor exacerbated 4-tBP-induced increase in CALM2, CAMKII, Calpain2, and p62 expression and also led to decrease in ATG5, ATG7, and LC3b expression. In contrast, miR-363 mimic notably alleviated these changes. Notably, siRNA CACNA1D effectively modulating miR-363 inhibitor's effect. Our study revealed that 4-tBP induced Ca 2+ overload and subsequent autophagy impairment via miR-363/CACNA1D axis. These findings illuminated a profound understanding of molecular mechanisms underlying 4-tBP-induced cytotoxicity and spotlighted a potential therapeutic target.

✓ 已验证 DOI PubMed 高影响因子
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MICROCHIMICA ACTA · 2019 ·Vol. 186 ·期 7 ·1-10 · IF 5.479

A composite prepared from gold nanoparticles and a metal organic framework (type MOF-74) for determination of 4-nitrothiophenol by surface-enhanced Raman spectroscopy

Zhang Yanshu,Hu Yufei,Li Gongke,Zhang Runkun

Core-shell nanoparticles (NPs) consisting of a gold core and a metal-organic framework shell (type MOF-74) were synthesized via one-pot synthesis. The NPs exhibit highly sensitive and stable SERS activity for the detection of 4-nitrothiophenol, with a specific band at 1337 cm −1 . The method has a linear response in 0.10–10 μmol·L −1 analyte concentration range and a lower detection limit of 69 nmol·L −1 . The potential application of this novel SERS substrate was evaluated by two model reactions involving 4-nitrothiophenol. The first involves in-situ SERS monitoring of the surface plasmon-induced nitration of aromatic rings without adding conventional acid catalyst. The second involves the photocatalytic reduction of 4-nitrothiophenol to 4-thioaminophenol in the presence of Au/MOF-74 under 785-nm laser irradiation. The plasmon-assisted dimerization of 4-nitrothiophenol to form 4,4′-dimercaptoazobenzene can also be monitored simultaneously. Schematic presentation of a nanoparticle SERS substrate consisting of gold core and MOF-74 shell, which was applied to detection of 4-nitrothiophenol. The Au/MOF-74 was successfully used for in-situ monitoring of two model reactions involving 4-nitrothiophenol by SERS.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Oncotarget · 2017 · IF 5.168

A novel synthetic derivative of quercetin, 8-trifluoromethyl-3,5,7,3′,4′-O-pentamethyl-quercetin, inhibits bladder cancer growth by targeting the AMPK/mTOR signaling pathway

Ting Tao,Caimei He,Jun Deng,Yanjun Huang,Qiongli Su,Mei Peng,Meiling Yi,Kwame Oteng Darko,Hui Zou,Xiaoping Yang

Quercetin is a naturally existing compound and shows attractive anticancer properties for a variety of solid tumors including glioma, bladder cancer, hepatocellular carcinoma, breast cancer, hematological malignancies and prostate carcinoma. However, these anticancer properties have not been clinically approved due to unclear mechanistic information and its low bioactivity. In our previous study, we elucidated that quercetin activates AMPK pathway which is the major mechanism for its unique anticancer effect in bladder cancer. In the present study, we are trying to enhance its bioactivity by chemical modification using fluorination approach to prepare novel chemical entities, based on the principle of intermediate derivative method (IDM). The compound we obtained is named 8-trifluoromethyl-3,5,7,3′,4′-O-pentamethyl- quercetin (TFQ), characterized by NMR spectra and mass spectrum (MS). The results from MTT and cologenic assay in two human and one murine bladder cancer cell lines showed that TFQ exhibits more potent inhibition on the three bladder cancer cell lines than quercetin (Que) although this enhanced effects is not very dramatic. Furthermore, we found that the survival of normal bladder cells PEBC was not significantly suppressed by TFQ compared with Que. Western blot analysis showed that TFQ possess more potent AMPK activation than Que. The downstream of AMPK was further examined by western blot. TFQ treatment is able to inactivate mTOR signaling pathway with the regulation of mTOR, 4EBP1 and P70S6K. These results demonstrated that the fluorinated quercetin derivative TFQ inhibits bladder cancer cell growth through the AMPK/mTOR pathway. Altogether, our findings suggest that TFQ could serve as a new potential therapeutic agent for bladder cancer more effective than Que.

✓ 已验证 DOI PubMed 高影响因子
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Frontiers in Pharmacology · 2019 · IF 3.845

L-4, a Well-Tolerated and Orally Active Inhibitor of Hedgehog Pathway, Exhibited Potent Anti-tumor Effects Against Medulloblastoma in vitro and in vivo

Zhu Mingfei,Wang Hong,Wang Chenglin,Fang Yanfen,Zhu Tong,Zhao Weili,Dong Xiaochun,Zhang Xiongwen

Inhibition of aberrant Hedgehog (Hh) pathway had been proved to be a promising therapeutic intervention in cancers like basal cell carcinoma (BCC), medulloblastoma (MB), and so on. Two drugs (Vismodegib, Sonidegib) were approved to treat BCC and more inhibitors are in clinical investigation. However, the adverse effects and drug resistance restricted the use of Hh inhibitors. In the present study, 61 synthesized compounds containing central backbone of phthalazine or dimethylpyridazine were screened as candidates of new Hh signaling inhibitors by performing dual luciferase reporter assay. Among the compounds, L-4 exhibited an IC50 value of 2.33 nM in the Shh-Light II assay. L-4 strongly inhibited the Hh pathway in vitro and blocked the Hh pathway by antagonizing the smoothened receptor (Smo). Remarkably, L-4 could significantly suppress the Hh pathway activity provoked by Smo mutant (D473H) which showed strong resistant properties to existing drugs such as Vismodegib. Orally administered L-4 exhibited prominent dose-dependent anti-tumor efficacy in vivo in Ptch+/-; p53-/- MB allograft model. Furthermore, L-4 showed good tolerance in acute toxicity test using ICR mice. These evidences indicated that L-4 was a potent, well-tolerated, orally active inhibitor of Hedgehog pathway, and might be a promising candidate in development of Hh-targeted anti-cancer drugs.

✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2022 · IF 6.364

Fabrication of 4 at.% La3+ ion doped (TbxLu0.96−x)2O3 transparent ceramics by using NC-PLSH technology and characterisation of their magneto-optical properties

Huabei Qi,Ding Zhou,Xiaohui Li,Wei Jing,Weiwei Li,Jiayue Xu

Nanocrystalline powders and pressureless sintering (NC-PLSH) were used in a H 2 atmosphere to fabricate 4 at.% La 3+ doped (Tb x Lu 0.96−x ) 2 O 3 magneto-optical transparent ceramics. La 3+ was utilised as a sintering aid, and Lu 3+ was used as a phase stabiliser . A component of the (Tb x Lu 0.96−x La 0.04 ) 2 O 3 magneto-optical material was designed and investigated based on powder sinterability and green compact sintering. Transparent (Tb x Lu 0.96−x La 0.04 ) 2 O 3 ceramics were obtained by using a one-step sintering process in H 2 atmosphere, without the need for subsequent hot isostatic pressing . The in-line transmittance of the as-polished 4 at.% La 3+ :(Tb 0.8 Lu 0.16 ) 2 O 3 ceramic was 79% at 1400 nm. The measured Verdet constant at wavelengths of 633 nm and 1064 nm was 354 rad/(T·m) and 100.2 rad/(T·m), respectively. The required length of the (Tb 0.8 Lu 0.16 La 0.04 ) 2 O 3 ceramics was 63% less than that of Tb 3 Ga 5 O 12 ceramics.

✓ 已验证 DOI 高影响因子
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JOURNAL OF COORDINATION CHEMISTRY · 2013 · IF 1.801

Synthesis and biological evaluation of Cu(II), Zn(II), and Ni(II) 3-(4-nitrophenyl)acrylic acid complexes with diamines as potential urease inhibitors

Zhong-Ming Yang,Hui Zhu,Juan Sun,Shao-Song Qian,Meng-Na Cai,Hai-Liang Zhu

Five new Cu(II), Zn(II), and Ni(II) 3-(4-nitrophenyl)acrylic acid complexes were synthesized and evaluated for inhibitory activity on jack bean urease. All five complexes were structurally determined by single crystal X-ray analysis. Compared with the positive reference acetohydroxamic acid (IC50 = 13.25 μM), Cu(II) complexes 3 and 4 showed the strongest inhibitory activity against jack bean urease (IC50 = 1.23 and 1.17 μM). Ni(II) and Zn(II) complexes also exhibited inhibitory activities (IC50 = 10.09–13.10 μM).

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