APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Yihua Yue,Jian Tian,Jiechao Ma,Shui Yang,Wen Li,Jiale Huang,Qingbiao Li,Guowu Zhan
Herein, Ga-ZnZrO x &ZSM-5 bifunctional catalysts were designed for CO 2 thermal hydrogenation to aromatics, particularly, aiming to enhance the selectivity of high-value BTX ( i.e. , benzene, toluene, and xylene). It was evident that the exterior surface properties and acidity of ZSM-5 can be effectively tailored by in-situ silicon deposition originating from the rice husk template. Catalytic performance assessments demonstrate an optimized catalyst achieving 88.1 % aromatics selectivity (exclusive CO) in a single pass, with a notable 45.2 % BTX selectivity within total aromatics and a low CO selectivity of 23.6 %. This superior performance is attributed to the in-situ silicon deposition on ZSM-5 during one-pot synthesis and the optimized spacing between Ga-ZnZrO x and ZSM-5 facilitated by the rice husk platform. Furthermore, in-situ DRIFTS analysis identifies key reaction intermediates. This study offers an effective strategy for tuning zeolite acidity using rice husks, while modulating metal oxide-zeolite proximity on the bio-SiO 2 platform, thus boosting CO 2 conversion to aromatics.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Tao Cheng,Yaotao Cai,Yifan Su,JinTao Xu,Xiaohua Tian,Pan Wang,Jianming Pan
Surface post-imprinting modification (SPIM) refers to a technique involving chemical modifications at the imprinted recognition site aimed at improving the specificity of the recognition site. Among these factors, ensuring sites accessibility and selecting appropriate substrates are essential to precisely adjusting the recognition site. In this study, hydrophilic metal–organic frameworks (MOFs) materials were employed as substrates with active functional groups, combined with SPIM to construct hydrophilic dual-receptor post-imprinting modified polymers (D-MOFs@PMIPs) for the selective separation of water-soluble 5′-adenosine monophosphate (AMP). We concentrate on the in-situ synthesis of imprinted polymers on the hydrophilic Zr-MOFs nanosheets surface through the utilization of ester ammonolysis covalent interactions, metal–ligand interactions involving Zr 4+ and PO 4 3- , and the sequential assembly of the template AMP molecule. The pore structure of the MOFs and the Zr 4+ provide high site accessibility and abundant imprinting sites. Furthermore, by employing the SPIM strategy based on disulfide bond-thiol exchange, pyrimidine functional groups were introduced to enhance the affinity of the imprinting recognition sites for the highly specific separation of AMP. The static adsorption results reveal a half-equilibrium time t 1/2 of 0.990 h, with a maximum adsorption capacity of 141.7 μmol g −1 at 298 K. The adsorption equilibrium constant ( k d ) for D-MOFs@PMIPs towards AMP is 219.0 L/g −1 , which is significantly higher than other nucleoside compounds, indicating a higher selectivity of D-MOFs@PMIPs for AMP. Concurrently, D-MOFs@PMIPs adsorbed 73 % of AMP from River water, further demonstrating that using hydrophilic Zr-MOFs as a substrate and employing dual-receptor SPIM polymer nanosheets as adsorbents can be effective for the selective separation and separation of nucleoside compounds in complex biological samples.
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MOLECULAR IMMUNOLOGY
·
2024
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IF 3.2
Zhaohui Shi,Tianfeng Zhao,Dingbo Li,Chong Wang,Yanjie Luo,Yangshan Zheng
Allergic rhinitis (AR) is caused by immunoglobulin E (IgE)-mediated reactions to inhaled allergens, which leads to mucosal inflammation and barrier dysfunction. The transcription factor forkhead box C1 (FOXC1) has been identified to be associated with allergic inflammation. This study sought to uncover the role of FOXC1 in AR. A murine model of AR was induced by repeated intranasal ovalbumin (OVA) challenges. Results revealed that high FOXC1 expression was found in the nasal mucosal epithelium of AR mice. Nasal allergy symptoms, mucosal epithelial swelling, goblet cell hyperplasia and eosinophil infiltration in AR mice were attenuated after silencing of FOXC1. Knockdown of FOXC1 decreased the levels of T-helper 2 cytokines interleukin(IL)−4 and IL-13 in nasal lavage fluid, and serum OVA-specific IgE and histamine. Silencing of FOXC1 restored nasal epithelial integrity in AR mice by enhancing the expression of tight junctions (TJs) and adherence junction. Furthermore, knocking down FOXC1 increased tight junction expression and transepithelial electrical resistance (TEER) in IL-13-treated air-liquid interface (ALI) cultures of human nasal epithelial cells (HNEpCs). Mechanistically, silencing of FOXC1 induced DNA methylation of secreted frizzled-related protein 5 (SFRP5) promoter and increased its expression in the nasal mucosa of AR mice and IL-13-treated ALI cultures. FOXC1 overexpression transcriptionally activated DNA methyltransferase 3B (DNMT3B) in IL-13-treated ALI cultures. Knockdown of SFRP5 reversed the protection of FOXC1 silencing on epithelial barrier damage induced by IL-13. Collectively, silencing of FOXC1 reduced allergic inflammation and nasal epithelial barrier damage in AR mice via upregulating SFRP5, which may be attribute to DNMT3B-driven DNA methylation. Our study indicated that FOXC1 may represent a potential therapeutic target for AR.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Ketao Shi,Youbing Zhu,Zhen Xu,Nianming Jiao,Hui Wang
The metal coordination state and the corresponding acid property of zeolite closely relate to its catalytic performance. In this study, DBD-plasma (dielectric barrier discharge-plasma), a low-temperature and energy-efficient external activation method, was proposed to activate the NH4+-type ZSM-5 zeolite and to regulate the Al coordination. It was found that DBD treatment could efficiently decompose NH4+ species at 115 °C, far below that required for calcination (550 °C). Characterizations, including X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), 27Al magic angle spinning nuclear magnetic resonance (27Al MAS NMR), and pyridine-adsorption infrared spectroscopy (Py-IR), revealed that DBD-plasma treatment could inhibit zeolite framework destruction and retain more framework Al and mesoporous structure, thus improving the stability and enhancing the amount of medium-strong Brønsted acid sites. In n-hexane cracking, DBD-activated zeolite exhibited improved conversion and C2–C4 olefin selectivity due to the enhanced monomolecular cracking pathway induced by increased Brønsted acidity, while reducing aromatics and coke formation by suppressing side reactions. This paper presents an alternative method that is more energy-efficient, highly effective, and capable of regulating the metal coordination and acidity of ZSM-5 zeolite.
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Sustainable Chemistry and Pharmacy
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2025
·
IF 5.8
Yang Liu,Shuo Zhang,Tingwei Zhang,Yongcan Jin,Huining Xiao,Chaofeng Zhang
5-Hydroxymethylfurfural (HMF) is a versatile biomass-derived platform compound, but its production from glucose and cellulose remains challenging. In this study, several nano-metal oxides (Al 2 O 3 , TiO 2 , ZrO 2 , and SnO 2 ) with distinct Lewis acidities were combined with a trace amount of HCl to catalyze the conversion of glucose to HMF in a methyl isobutyl ketone (MIBK)/H 2 O–NaCl biphasic system. Without HCl, fructose was formed and accumulated in the aqueous phase due to insufficient Brønsted acidity, limiting further dehydration to HMF. The addition of HCl effectively overcame this bottleneck, with Al 2 O 3 and HCl showing the best synergy. Under optimized conditions, a HMF yield of 69.1 % was achieved at 180 °C, and Al 2 O 3 exhibited excellent recyclability. This work demonstrates a promising approach for combining homogeneous and heterogeneous catalysis for efficient conversion of renewable carbohydrates into platform chemicals.
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NEW JOURNAL OF CHEMISTRY
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2025
·Vol. 49
·期 24
·10338-10356
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IF 2.5
Fan Bai,Yanjiao Gao,Yongbo Xiao,Jingyi Yang,Jiaxin Chen,Jing Xiao
In recent years, advanced oxidation based on periodate (PI) has become a research focus for disposal of recalcitrant organics from water due to its efficient oxidizing ability. This study systematically investigated the degradation of reactive black 5 (RB5) by the Cu(II)-activated sodium periodate (NaIO4, SPI) system. The optimal reaction conditions were determined via Box–Behnken response surface methodology as [Cu(II)] = 1.013 ± 0.021 g L−1, [SPI] = 45 ± 2 μM, and pH = 5.7 ± 0.3, achieving a RB5 removal rate of 91.98% (R2 = 0.9901, prediction error <1%). The free radical quenching experiment confirmed that the dominant ROS in the system were ˙OH, 1O2, and IO3˙, and their contribution was IO3˙ > 1O2 > ˙OH. The coexistence anion experiments showed that Cl− (0.1–5.0 mM) and SO42− (0.1–5.0 mM) had almost no effect on the RB5 degradation efficiency, with inhibition rates lower than 1.99% and 3.58%, respectively, while CO32− (1.0 mM) and HCO3− (1.0 mM) led to a decrease of 20.8% and 14.17% in the RB5 degradation rate. In the presence of HA, the degradation efficiency of RB5 was maintained at 89.88–92.66%. The system maintained a removal rate of 73.33–87.66% for RB5 in the simulated actual water bodies (tap water/river water/brewery wastewater). Energy-assisted experiments showed that the activation energy of the reaction was significantly reduced and the kobs values were increased by 10.3 times when the temperature was increased to 40 °C, and the reaction time could be shortened to 2 min (removal rate >98%) after ultraviolet (365 nm, 20 W) coupling. In summary, this study is expected to support the related PI-based advanced oxidation process in stubborn pollutant treatment.
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Materials Today Chemistry
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2025
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IF 6.7
Shuo Zhang,Xue Yang,Longyongxue Ma,Junwei Ma,Hongtao Gao
The conversion of biomass into value-added chemicals is crucial for addressing resource shortages and mitigating environmental degradation. 5-Hydroxymethylfurfural (HMF), a promising biomass-derived platform compound, can be selectively oxidized to produce high-value 2,5-furandicarboxylic acid (FDCA). In this study, an amorphous bimetallic hydroxide, Ni 1 Co 2 -LDH, was synthesized for the effective electrocatalytic oxidation of HMF. Electrochemical experimental results indicate that Ni–Co dual sites synergistically participate in the oxidation of HMF. Co sites promote the transformation of the aldehyde (CH O) group to the carboxyl group, while Ni sites speed up the reaction rate of 2,5-furandicarboxylic acid (FDCA) generation. The construction of such a bimetallic site enables the Ni 1 Co 2 -LDH catalyst to exhibit a low onset potential (1.20 V vs. RHE) and high selectivity (100 %) in HMFOR. At 1.30 V (vs. RHE), the catalyst achieves a Faradaic efficiency of 90.5 % and an FDCA yield of up to 95.6 %. Furthermore, Ni 1 Co 2 -LDH exhibits exceptional structural and catalytic stability, maintaining an FDCA yield above 95.0 % after five consecutive electrochemical cycles. These findings highlight the potential of Ni 1 Co 2 -LDH, synthesized via a hydrothermal method, as an efficient anode catalyst for the sustainable production of high-value chemicals from biomass-derived compounds.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2025
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IF 2.1
Yaqi Han,Fumin Xue,Wenguo Xing,Huanhuan Yin,Xiangchuan Wang,Shuai Yu
Solid–liquid equilibrium solubilities of 2-mercapto-5-methyl-1,3,4-thiadiazole (MMTD) in 12 kinds of monosolvents (i.e., methanol, ethanol, n-propanol, i-propanol, n-butanol, i-butanol, ethyl formate, methyl acetate, ethyl acetate, propyl acetate, butyl acetate, and amyl acetate) were determined by a gravimetric method with the temperature range from 283.15 to 323.15 K. In alcoholic solvents, the solubility order is ethanol > methanol > n-propanol > i-propanol > n-butanol > i-butanol. In ester solvents, the solubility of MMTD ranking is methyl acetate > ethyl acetate > propyl acetate > butyl acetate > amyl acetate > ethyl formate. The solubility of MMTD increased with increasing temperature. Four thermodynamic models (i.e., the modified Apelblat model, the λh model, the Wilson model, and the Jouyban model) were selected to correlate the solubility data. The RAD and RMSD values were less than 0.0254 and 0.000536, respectively. The Wilson model had the best-fitting effect. The KAT-LSER model and Hansen solubility parameters were used to explain the solvent effect in this work. The Hirshfeld surface, molecular electrostatic potential surface, and free energy of solvation were used to explain the interactions between molecules. Dissolution properties of MMTD were calculated by the Wilson model. The dissolution process of MMTD is endothermic, entropy driven, and spontaneous.
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JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Yimin Cai,Seraj A. Ansari,Kuirong Fu,Beichen Zhu,Haoyang Ma,Lixi Chen,Steven D. Conradson,Song Qin,Haiying Fu,Prasanta K. Mohapatra,Lihua Yuan,Wen Feng
Selective extraction of highly radiotoxic actinides(III) is an important and challenging task in nuclear wastewater treatment . Many proposed ligands containing S or P atoms have drawbacks including high reagent consumption and possible secondary pollution after incineration. The present work reports five novel pillar[5]arene-based extractants that are anchored with picolinamide substituents of different electronic nature by varying spacer. These ligands reveal highly efficient separation of actinides(III) over lanthanides(III). Specifically, almost all of these ligands could extract Am(III) over Eu(III) selectively at around pH 3.0 (SF Am/Eu > 11) with fast extraction kinetics. Variation of the pyridine nitrogen basicity via changing para-substitution leads to an increase in the distribution ratios by a factor of over 300 times for Am(III) with an electron-withdrawing group compared to those with an electron donating group. Investigation of complexation mechanism by slope analysis, NMR, IR, EXAFS , and DFT techniques indicates that each ligand binds two metal ions by pyridine nitrogen and amide oxygen. Finally, these ligands do not show obvious decrease in both extraction and separation ability after being exposed to 250 kGy absorbed gamma radiation . These results demonstrate the potential application of pillar[5]arene-picolinamides for actinide(III) separation.
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MOLECULES
·
2018
·Vol. 23
·期 4
·756
·
IF 3.098
Ming-Xia Song,Zhen-Yuan Wang,Shi-Hui He,Sheng-Wang Yu,Shi-Long Chen,Dong-Fu Guo,Wen-Hao Zhao,Xian-Qing Deng
In this study, a novel series of 4-(2-(alkylthio)benzo[d]oxazol-5-yl)-2,4-dihydro-3H-1,2,4-triazol-3-ones (4a–m) was designed and synthesized. The anticonvulsant activities of these compounds were evaluated by using the maximal electroshock seizure (MES) and subcutaneous pentylenetetrazole (scPTZ) seizure models in mice. The neurotoxicity of these compounds was evaluated using the rotarod neurotoxicity test. The majority of compounds showed anti-MES activities at 100 or 300 mg/kg. Compound4gwas considered to be the most promising, based on its potency against MES- and PTZ-induced seizures with ED50values of 23.7 and 18.9 mg/kg, respectively. The TD50value of4gwas 284.0 mg/kg, which resulted in a higher protective index (PI = TD50/ED50) value than that of carbamazepine and valproate. In an ELISA test, compound4gsignificantly increased the γ-aminobutyric acid (GABA) content in mouse brain. In addition, pretreatment with thiosemicarbazide (an inhibitor of the GABA synthesizing enzyme) significantly decreased the activity of4gin the MES model, which suggests that the mechanism through which compound4gelicits its anticonvulsive action is at least in part through increasing the GABA level in the brain.Keywords:anticonvulsant;maximal electroshock;pentylenetetrazole;benzoxazole;triazolone
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RSC Advances
·
2017
·Vol. 7
·期 5
·2415-2425
·
IF 3.108
Ying Yang,Lin Zhu,Feng Xia,Baoyou Gong,Anjian Xie,Shikuo Li,Fangzhi Huang,Shaohua Wang,Yuhua Shen,David T. Weaver
In this study, a novel drug-loaded inorganic nanoparticle–biomolecule hybrid hydrogel shell containing fluorouracil (5-FU)/reduced graphene oxide (rGO)/Brassica chinensis extract (Bce) on tumor cells was firstly constructed through a facile one-step method. The Bce stems from a natural green vegetable for improving the bio-compatibility of 5-FU/rGO/Bce hydrogel and presents multi-functions in this system. As both a reducing and a cross-linking agent for GO, Bce is beneficial for the fast formation of a rGO/Bce hybrid hydrogel at body temperature (37 °C) before laser irradiation, as well as being an excellent photo-sensitizer for inducing the generation of cytotoxic singlet oxygen (1O2) to kill tumor cells by means of laser radiation. The rGO in the hybrid hydrogel possesses photothermal characteristic for the hyperthermia antitumor. After loading anticancer drugs, the formed 5-FU/rGO/Bce hybrid hydrogel shells encapsulated on the tumor cells in situ exhibit three competitive advantages, i.e., retaining the high concentration of drugs around tumor cells to enhance the localized antitumor effect, reducing the side effects by hindering drugs from migrating to normal tissue, and displaying effectively synergetic chemo/photo-thermal/photodynamic therapies. This study provides a new strategy to exploit the multi-functions of hybrid hydrogel materials for effective biomedical applications.
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yuke Wu,Shaoyu Yuan,Ting Wang,Hu Yan,Zihao Qin,Yu Qiu,Yunchao Feng,Xianhai Zeng
The transfer hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF) using ethanol as the hydrogen donor represents a green and efficient route for biomass valorization. In this work, a carbon-coated CuCo catalyst was designed to catalyze this transformation, achieving a high DMF yield of 96.4 % at 180°C within 6 h. Isotopic labeling indicated that transfer hydrogenation proceeded via a metal-mediated mechanism, while combined experimental and theoretical observations revealed that the formation of CuCo alloy optimized the adsorption modes of HMF. Specifically, the adsorption of the aldehyde group in HMF changed from η 1 to di-σ C,O configuration, weakening the C=O bond and thus facilitating hydrodeoxygenation. Notably, the CuCo alloy weakened the adsorption strength of HMF on the catalyst surface, preventing competitive adsorption from inhibiting ethanol dehydrogenation. These optimized adsorption interactions ensured the smooth progress of ethanol dehydrogenation and HMF hydrogenation, enabling CuCo catalyst to exhibit excellent performance in the transfer hydrogenation reaction.
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