MICROPOROUS AND MESOPOROUS MATERIALS
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2017
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IF 3.615
Wentian Ma,Kexin Li,Huiqin Guo,Liushui Yan,Yuhua Dai,Xubiao Luo,Yong Yao
Porous carbon microspheres with numerous spherical microstructures were successfully fabricated directly from waste Camellia oleifera shells by hydrothermal carbonization combined with annealing treatment and potassium hydroxide chemical activation technique in the assistance of phloroglucinol. Numerous aromatic carbon microspheres were constructed after hydrothermal carbonization due to the structure-directing effect of phloroglucinol. The spherical microstructures remain intact after suffering from potassium hydroxide chemical activation because the aromatic carbon framework was further graphitized by annealing treatment. The mesoporous carbon microspheres were successfully obtained from microporous carbon microspheres through the secondary potassium hydroxide chemical activation. As valuable porous materials, the as-prepared microporous and mesoporous carbon microspheres were successfully applied to the sustained-release of anticancer drug 5-fluorouracil. The as-prepared microporous and mesoporous carbon microspheres showed some obvious advantages such as low-cost, high-capacity, and strong biological affinity compared with traditional drug sustained-release agent.
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ENERGY
·
2024
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IF 9
Xian Shi,Wanni Liu,Xinyi Xing,Weiwei Shu,Rui Weng,Junhang Sun,Ying Guan,Hui Gao,Gaojin Lyu,Kai Huang,Zengyong Li,Mengya Ruan,Siquan Xu
5-hydroxymethylfurfural (HMF) is a platform compound with great potential, and solid acid-catalyzed lignocellulosic carbohydrate components into HMF is a viable biomass valorization strategy. Herein, hafnium-anchored dendritic mesoporous silica nanospheres (Hf-DMSNs) with three-dimensional center-radial structures were synthesized via an in-situ co-assembly method. Characterization revealed that the acid properties and particle size of Hf-DMSNs could be regularly customized and that they acted as bifunctional catalysts capable of driving glucose (190 °C, 3 h) and cellulose (210 °C, 4 h) to achieve the desired HMF yields of 71 % and 50 %, respectively. Owing to the appropriate acidity, high accessibility, and anchored active site, the recycling of Hf-DMSNs catalyst lasted for more than twenty times with slight activity loss, which is eye-catching. Meanwhile, the intermediates detected during the conversion process confirmed that the HMF formation from cellulose components under the Hf-DMSNs catalysis was a cascade reaction consisting of three basic steps: hydrolysis, isomerization, and dehydration. The findings in this study provide a reference for the utilization of biomass-derived carbohydrates into HMF via heterogeneous catalysis.
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MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Guanghou Wang,Xueqian Tang,Feixu Qin,Hongjin Wang,Hao Zhang,Hanyue Li,Lan Wei,Lixin Sun
Nauclea officinalis ( N. officinalis ), a medicinal plant of the genus Nauclea in the Rubiaceae family, is used to treat bronchitis, pneumonia and acute tonsillitis and enteritis in China. Extracts of N. officinalis include more than 60 alkaloids, which exert all kinds of pharmacological effects, such as antiproliferative, antiparasitic, antimicrobial, anticancer, and anti-inflammatory activities. In this study, an affinity ultrafiltration and high-performance liquid chromatography- tandem mass spectrometry (AUF-LC-MS/MS) approach was constructed and validated, and was applied to rapidly screen COX-2/5-LOX inhibitors in N. officinalis extracts (NOE). To gain a more comprehensive and profound understanding of the anti-inflammatory mechanism of N. officinalis . Central Composite Design (CCD) of Response Surface Method (RSM) was used to optimize extraction conditions for potential COX-2/5-LOX inhibitors from NOE. Next, COX-2/5-LOX dual targeted inhibitors were screened from NOE using AUF-LC-MS/MS, and the biological activity of the screened ligands was demonstrated by enzyme inhibition assay. Finally, the preferred binding modes for these COX-2/5-LOX inhibitors were then determined by molecular docking, and compared with active drugs celecoxib and zileuton, respectively, to further explore ligand active binding sites and intersections between ligands and target proteins. The optimum extraction conditions were follows: ethanol concentration of 79 %, liquid − solid ratio of 11.8 v / w and extraction time of 1.8 h. The results of COX-2 inhibition assay showed that angustine (AU) had the more stronger inhibition activity with an IC 50 of 20.49 μM, followed with IC 50 of angustidine (AD) and nauclefine (NF) were 35.89 and 60.45 μM, respectively. Among the three components, AU also exhibited the highest inhibition of 5-LOX with an IC 50 of 1.18 μM, followed by NF and AD at 2.75 and 4.35 μM, respectively. Owing to the synergistic effect of multiple components make NOE exhibit strong inhibitory activity, it is shown potent inhibitory activities with an IC 50 at 9.47 and 6.16 μg/mL for COX-2 and 5-LOX, respectively. This work has demonstrated that NF, AD, and AU are potential COX-2/5-LOX dual-target inhibitors, indicating that N. officinalis anti-inflammatory activities were partially based on these COX-2/5-LOX inhibitors. These research results can also be further used for developed or improved anti-inflammatory agents with more beneficial effects.
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Food Bioscience
·
2025
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IF 5.9
Cheng Yang,Pei-Zhi Dong,Zhou-Ning Jiang,Yanan Li,Yue-Hong Pang
The illegal addition of phosphodiesterase-5 (PDE-5) inhibitors in functional food poses significant food safety risks and health issues, requiring a sensitive and effective enrichment and detection method. Herein, a magnetic COFs (Fe 3 O 4 @TpDBA) was prepared by a layer-by-layer growth strategy. TpDBA was synthesized through the condensation of 1,3,5- Triformylphloroglucinol (Tp) and 4,4′-diamino-(1,1′-biphenyl)-3,3′-dicarboxylic acid (DBA). Fe 3 O 4 @TpDBA was used as an adsorbent for magnetic solid-phase extraction (MSPE) of PDE-5 inhibitors (sildenafil, tadalafil, and vardenafil), which enabled their efficient enrichment within 2 min. The lower binding energy value obtained through molecular docking calculations indicates stronger binding ability. The prepared Fe 3 O 4 @TpDBA exhibited high chemical stability (resistant to acid, alkali and organic reagents) and good reusability (10 adsorption/desorption cycles). Coupled with high-performance liquid chromatography-tandem mass spectrometry, Fe 3 O 4 @TpDBA-MSPE exhibited great potential in PDE-5 inhibitors. The developed method was optimized and validated, exhibiting a wide linear range and low limits of detection. Moreover, it was successfully applied to the determination of three PDE-5 inhibitors in five functional foods.
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Advanced Energy Materials
·
2024
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IF 24.4
Yanyan Zhang,Guangtong Hai,Zhuoshen Huang,Zhimeng Liu,Xiubing Huang,Ge Wang
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMFOR) is an effective route to produce value-added chemicals with low energy consumption. In this work, efficient electrocatalysts are prepared by varying the amount of Ce doping and CeO 2 modification on NiFe layered double hydroxide (NiFe–LDH) nanosheets supported on carbon cloth (CC). Through Ce doping and heterogeneous interface construction, the electronic structure and coordination chemistry of NiFe–LDH are greatly changed. Compared to CeO 2 modification and the synergistic effect of Ce-doping and CeO 2 modification, CC@NiFeCe(3%)-LDH with only Ce-doping show excellent charge transfer ability, higher HMF conversion (95.73%), 2,5-furandicarboxylic acid (FDCA) selectivity (93.31%), and Faraday efficiency (99.47%) at only 1.44 V RHE . Density-functional theory calculations and X-ray fine structure spectroscopy demonstrate that Ce doping, compared with CeO 2 modification and their synergistic effects, significantly facilitates the electron transport and optimizes intermediate adsorption by effectively lowering the activation energy for the transformation of 5-formyl-2-furancarboxylic acid (FFCA) and encourage the conversion of FFCA to FDCA. Overall, this work systemically investigates the HMFOR behaviors of CC@NiFe–LDH under Ce doping, CeO 2 modification, and their synergetic effect, which provides some guidance on the development of high-performance electrocatalysts for HMFOR performance.
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ENZYME AND MICROBIAL TECHNOLOGY
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2019
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IF 3.553
Liuyan Gu,Haibo Yuan,Xueqin Lv,Guangsheng Li,Rigang Cong,Jianghua Li,Guocheng Du,Long Liu
5-Methylpyrazine-2-carboxylic acid (MPCA) is an important pharmaceutical intermediate and is used in the production of hypoglycemic agents and lipid-lowering drugs. This work aimed to develop a whole-cell biocatalytic process for the efficient synthesis of MPCA from 2, 5-dimethylpyrazine (DMP). Firstly, a whole-cell biocatalyst Escherichia coli strain was constructed by plasmid-based expression of xylene monooxygenase (XMO), benzyl alcohol dehydrogenase (BADH), and benzaldehyde dehydrogenase (BZDH) from Pseudomonas putida ATCC 33015, resulting in MPCA titer of 5.0 g/L. Then, the reaction conditions were optimized and the MPCA titer was further increased to 9.1 g/L. Next, the Ribosome Binding Site (RBS) Calculator v2.0 was used to predict and compare the translation initiation rates of the RBS sequences preceding xylM and xylA genes, encoding the two subunits of XMO. By optimizing the RBS sequences preceding xylA , the MPCA titer was increased to 10.2 g/L and the yield of MPCA on DMP reached 0.665 mol/mol. Finally, to achieve plasmid-free production of MPCA, we integrated the genes encoding for XMO, BADH and BZDH in the genome by using CRISPR/Cas9 and further fine-tuned the copy number ratios of xylM and xylA in the genome, improving the MPCA titer to 15.6 g/L and the yield of MPCA on DMP to 1.0 mol/mol. This work developed a high-yield and plasmid-free biocatalysis process for the environmentally friendly production of MPCA with 100% substrate conversion, and paved the way for the commercial production of MPCA in the future.
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PubMed
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 12
·2778
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IF 4.2
Xi Zhu,Yong Guo,Baozhan Zheng
Efficient recovery of gallium (Ga) from vanadium slag processing residue (VSPR) solution is of great significance for environmental protection and resource utilization, but improving its selective adsorption against the coexisting Sc3+and In3+is still challenging. Herein, a novel adsorbent consisting of 4-amino-3-hydrazino-1,2,4-triazol-5-thiol (AHTZT)-modified graphene oxide (GO-AHTZT) was successfully synthesized that exhibits a higher adsorption selectivity for Ga3+in VSPR solution with coexisting Sc3+and In3+. Under optimal conditions, the adsorption capacity of GO-AHTZT for Ga3+can reach 23.92 mg g−1, which is 4.9 and 12.6 times higher than that for Sc3+(4.87 mg g−1) and In3+(1.90 mg g−1) adsorption, indicating the excellent anti-interference ability of GO-AHTZT against Sc3+and In3+. The process and mechanism of Ga3+adsorption onto GO-AHTZT was also studied and discussed in detail. By measuring the adsorption process and by characterizing the adsorbent before and after adsorption, we demonstrate that the selective interaction between the Ga3+- and N-containing groups in AHTZT is the main reason for the improved adsorption selectivity. This work opens up an avenue for the design and synthesis of highly selective adsorbents for Ga3+in complex VSPR solutions.
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Green Energy & Environment
·
2025
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IF 14.6
Runqing Xiao,Qingmao Yang,Yanjie Li,Wei Zhang,Gang Xiao,Chun Shen
Achieving high selectivity to 2,5-furandicarboxylic acid (FDCA) in the photocatalytic oxidation of 5-hydroxymethylfurfural (HMF) in aqueous solution advocates the principle of green and sustainable chemistry, but still remains a significant challenge. Herein, manipulating the reactive oxygen species (ROS) has been realized and dramatically promotes the selective photocatalytic oxidation of HMF in aqueous solution. High FDCA yield of 98.6% has been achieved after 3 hours of visible light irradiation over the as-prepared FeO x -Au/TiO 2 catalyst, being one of the leading photocatalytic performances. Furthermore, satisfactory FDCA yields of higher than 80% could be realized even in the outdoor environment under natural sunlight irradiation, regardless of sunny or cloudy weather. A combination study including physical characterization, kinetic analysis, radical trapping experiments and density functional theory calculations unveils the rate-determining step (oxidation of hydroxyl group) and respective contributions of the generated ROS ( 1 O 2 and •O 2 – ) in each step of the entire reaction network. The present work would push ahead the understanding of HMF photocatalytic oxidation and contribute to the rational design of high-performance photocatalysts.
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Journal of Integrative Agriculture
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2024
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IF 4.6
Jing Zuo,Yingying Quan,Yue Li,Dong Song,Jinpeng Li,Yuxin Wang,Li Yi,Yang Wang
Streptococcus suis is a significant zoonotic agent affecting both human and pig health and poses a substantial public health concern. The pathogenicity of S. suis is intricately linked to its ability to form biofilms and express virulence factors, which are regulated by the LuxS/AI-2 quorum sensing (QS) system. Herein, we uncover a novel therapeutic avenue by demonstrating that 5-fluorouracil (5-FU), an FDA-approved anti-cancer agent, effectively mitigates biofilm formation and attenuates the virulence of S. suis . Mechanistically, we observe a significant reduction in capsular polysaccharide and extracellular polysaccharide production upon 5-FU treatment, elucidating a potential mechanism for biofilm weakening. Additionally, 5-FU down-regulates virulence traits, diminishing S. suis ‘s ability to adhere to host cells and evade phagocytosis. Crucially, our study identifies the thymidylate synthase regulatory gene thyA as a key mediator of 5-FU’s effects on the LuxS/AI-2 QS system. Virtual molecular docking and gene knockout experiments provide compelling evidence that 5-FU modulates the LuxS/AI-2 QS system by targeting thyA . In vivo experiments further validate the therapeutic potential of 5-FU, showcasing a significant reduction in bacterial load and mitigation of tissue damage in a mouse model. In conclusion, our investigation unveils 5-FU as a potent disruptor of S. suis ‘s biofilm formation and virulence, offering a promising avenue for the control of this devastating pathogen.
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Surfaces
·
2025
·Vol. 8
·期 4
·69
·
IF 2.9
Huajie Zhang,Yunhan Pu,Yanjun Li,Mingli Fu
The selective oxidation of methane to methanol under mild conditions remains a significant challenge due to its stable C-H bond and the propensity for overoxidation of products. Herein, we investigated the Fe- and Cu-modified ZSM-5 catalysts using H2O2as an oxidant for the selective oxidation of methane. It was found that the Fe/Cu ratio had a great impact on methanol yield. The Fe3Cu1displayed the highest methanol yield of 29.7 mmol gcat−1h−1with a selectivity of 80.9% at 70 °C. Further analysis revealed that Fe3Cu1showed the highest Fe3+and Cu+contents. The optimal dual valence cycle not only facilitates the efficient utilization of H2O2, promoting the activation of methane to •CH3at the Fe site, but also suppresses the deep oxidation caused by the Fenton-like effect of Fe/H2O2, thus maintaining the high yield and high selectivity of methanol.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
·
IF 21.1
Weizhen Xie,Chenting Yang,Quanwei Deng,Shigang Su,Lu Lin,Xing Tang
The selective hydrogenation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)tetrahydrofuran (BHMTHF) under mild conditions holds great significance for sustainable chemical production. However, this process remains hindered by challenges such as the instability of HMF in aqueous media and the insufficient efficiency of H 2 activation. Herein, a Pd catalyst supported on oxygen-vacancy–enriched MnO x -VC (Pd/MnO x -VC) is developed, featuring highly dispersed Pd/PdO heterostructures with abundant Pd–O–Mn interfacial active sites. Notably, Pd/MnO x -VC offered a high BHMTHF formation rates of 366.5 mol BHMTHF ·mol Pd −1 ·h −1 in water under mild conditions. Moreover, the catalyst was able to efficiently convert both purified and crude HMF at high concentrations (≥ 10 wt%), achieving BHMTHF yields exceeding 90 % in either batch or continuous-flow reactor under low temperatures (30–60 °C), underscoring its potential for industrial application. Mechanistic studies revealed that the relay activation of H 2 over Pd nanoparticles and adjacent Pd–O–Mn sites generates polarized H δ⁺ –H δ⁻ pairs, which primarily contributed to the outstanding activity of Pd/MnO x -VC. This work highlights the importance of interfacial site engineering in designing high-performance catalysts for HMF hydrogenation.
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ENERGY
·
2024
·
IF 9
Xiaohua Li,Junlong Wang,Yongbo Yu,Yu Cao,Shanshan Shao,Shiliang Wu
Inexpensive catalyst sources are of great importance in the conversion of biomass to economically valuable monocyclic aromatic hydrocarbons , and transition metals (Co, Ni, Fe and Mn) rich in catalytic effects in massive waste lithium battery cathode materials are not effectively reutilized currently. For this reason, the feasibility of employing the valuable metal oxides in the carbon-reduced waste lithium battery cathode materials (waste LiFePO 4 batteries, LFP, and waste LiNi x Co y Mn 1–x–y O 2 batteries, NCM) with HZSM-5 as coupled catalysts in the rape straw catalytic pyrolysis to produce aromatic hydrocarbons was explored. The carbon-reduced waste lithium battery cathode materials performed well at 5 wt% carbon loading, and the content of active components Fe 2 O 3 (SLFPC-5) and NiO (SNCMC-5) used for the reduction of large molecular oxygenates in biomass pyrolysis gas was increased by water leaching treatment. SLFPC-5 demonstrated superior bond-cutting performance, while SNCMC-5 exhibited strong deoxygenation performance. The selectivity of monocyclic aromatic hydrocarbons (MAHs) catalyzed by SLFPC-5/HZSM-5 and SNCMC-5/HZSM-5 was as high as 63.69 % and 79.19 %, with BTX yields of 14.58 wt% and 16.68 wt% respectively. This coupled catalytic system offers a low-cost source of catalysts for biomass catalytic pyrolysis and broadens the possibility of high-value recycling of wasted lithium batteries.
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