Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yuan Bao,Weijia Pu,Yiwei Zhang,Yahui Xiao,Yong Liu
Ni-Co nano-alloys confined by in-situ formed N-doped porous carbon overlayer have been prepared through chelation of metal cations with citric acid and urea followed by carbonization for hydrodeoxygenation of 5-hydroxymethylfurfural (HMF) into 2, 5-dimethylfuran (DMF). The results indicated that the Ni-Co nano-alloys were formed and homogeneously distributed within the N-doped porous carbon overlayer. The electronic effect of the Ni-Co nano-alloys significantly boosted hydrodeoxygenation activity of the Co 2 Ni 1 @NC catalyst and simultaneously inhibited further hydrogenation and opening of furan ring. The N-doped porous carbon overlayer around Ni-Co nano-alloys not only facilitated to disperse and stable Ni-Co nano-alloys through strong metal-support interaction, but also protected the Ni-Co nano-alloys from aggregation. Therefore, the Co 2 Ni 1 @NC catalyst offered superior catalytic performance with the HMF conversion of 100 % and DMF selectivity of 93.0 %. Moreover, the Co 2 Ni 1 @NC catalyst displayed excellent stability without significant activity loss after five recycles due to the spatial confinement of N-doped carbon overlayer.
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MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 4
·1-8
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IF 5.705
Yang Yiwen,Zeng Yanbo,Tang Chuangui,Zhu Xudong,Lu Xing,Liu Lingyu,Chen Zhidong,Li Lei
The authors describe an electrochemical sensor for the determination of 5-hydroxytryptamine (5-HT; serotonin). It is based on the use of platinum nanoparticles (PtNPs) coated with molecularly imprinted silica (MIS). The MIS-coated PtNPs were prepared from 5-HT, PtNPs, phenyltrimethoxysilane and tetraethoxysilane that act as template, support, functional monomer and cross-linker, respectively. The MIS-coated PtNPs were characterized by Fourier transfer infrared spectroscopy and transmission electron microscopy. The MIS-coated PtNPs were drop-cast onto a glassy carbon electrode (GCE) to obtain an electrochemical sensor for 5-HT which exhibited fast response and high recognition ability for 5-HT. The imprinting factor of this electrode for 5-HT is 4.12, which is higher than that for its analogs. Under optimized conditions and at a typical working potential of 0.29 V (vs. Hg/Hg 2 Cl 2 ), the electrode has a linear response in the 0.05–80 μM 5-HT concentration range and a 0.02 μM detection limit. The electrode was successfully applied to the determination of 5-HT in human serum samples.
Molecularly imprinted silica-coated platinum nanoparticles were prepared using surface imprinting technique. A glassy carbon electrode modified with the surface imprinted material exhibits fast response in detecting 5-hydroxytryptamine, a low detection limit, good selectivity, reproducibility and stability.
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ANTIMICROBIAL AGENTS AND CHEMOTHERAPY
·
2018
·Vol. 62
·期 2
·
IF 4.256
Cheng Wang,Gaomei Zhao,Song Wang,Yin Chen,Yali Gong,Shilei Chen,Yang Xu,Mengjia Hu,Xinmiao Wang,Hao Zeng,Aiping Wang,Dengqun Liu,Yongping Su,Tianmin Cheng,Fang Chen,Junping Wang
The increasing incidence of multidrug-resistant Acinetobacter baumannii (MDRAb) infections worldwide has necessitated the development of novel antibiotics. Human defensin 5 (HD5) is an endogenous peptide with a complex architecture and antibacterial activity against MDRAb. In the present study, we attempted to simplify the structure of HD5 by removing disulfide bonds. We found that the Cys2-4 bond was most indispensable for HD5 to inactivate MDRAb, although the antibacterial activity of the derivative was significantly attenuated. We then replaced the noncationic and nonhydrophobic residues with electropositive Arg to increase the antibacterial activity of HD5 derivative that contains a Cys2-4 bond, obtaining another derivative termed HD5d5. The in vitro antibacterial assay and irradiation-wound-infection animal experiment both showed that HD5d5 was much more effective than HD5 at eliminating MDRAb. Further investigations revealed that HD5d5 efficiently bound to outer membrane lipid A and penetrated membranes, leading to bacterial collapse and peptide translocation. Compared to HD5, more HD5d5 molecules were located in the cytoplasm of MDRAb, and HD5d5 was more efficient at reducing the activities of superoxide dismutase and catalase, causing the accumulation of reactive oxygen species that are detrimental to microbes. In addition, HD5 failed to suppress the pathogenic outer membrane protein A of Acinetobacter baumannii (AbOmpA) at concentrations up to 50 μg/ml, whereas HD5d5 strongly bound to AbOmpA and exhibited a dramatic toxin-neutralizing ability, thus expanding the repertoire of drugs that is available to treat MDRAb infections.
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Molecular Catalysis
·
2025
·
IF 4.9
Shengxin An,Shuaibo Zhao,Jingting Jin,Tao He,Yuhao Wang,Na Kong,Jie Zhou,Wenzhi Li
Great expectations have been placed on bimetallic co-modified zeolite for the direct oxidation of methane to methanol. In this work, H-ZSM-5 zeolite was modified with bimetallic copper and zinc via ion-exchange method. Numerous experiments were conducted and the methanol yield of 44,302.70 μmol·g cat −1 ·h −1 was obtained over 1Cu/2Zn-ZSM-5 catalyst. A series of characterization analyses confirmed that the introduction of Zn increased the proportion of active Cu species bound to extra-framework oxygen by altering the electronic state of copper. The bis (μ-oxo) dicopper ligand was identified as the active site for methane oxidation. The possible reasonable reaction pathway was the free radical reaction. This work provides a valuable guidance for the preparation of co-modified zeolite catalysts for the direct oxidation of methane to methanol.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Liyan Wang,Zhaokun Wang,Liang Chu,Mu Yang,Ge Wang
The design of transition metal nitrides with excellent oxygen evolution reaction and 5-hydroxymethylfurfural oxidation reaction (HMFOR) is of great significance to achieve the goal of "carbon peaking and carbon neutrality". Herein, Fe-doped bimetallic nitride Fe x Co 1-x ) 4 N was prepared by a simple electron regulation strategy. The introduction of Fe changes the electronic structure of Co and optimizes the adsorption energies of *OH, reduces the potential barrier for the generation of *OOH as a potential-determining step and thus increases the intrinsic OER activity of Co 4 N. In addition, Fe substitution of some of the Co atoms gives (Fe x Co 1-x ) 4 N a higher electrochemical active surface area, which accelerates the electron transfer efficiency and improves the electrical conductivity. The overpotential for (Fe x Co 1-x ) 4 N-0.9 to reach a current density of 10 mA cm −2 in 1 M KOH is only 271 mV. When in 1 M KOH + 50 mM HMF condition, (Fe x Co 1-x ) 4 N-0.9 requires only 1.37 V to reach a current density of 10 mA cm −2 . This work provides practical guidance for developing bifunctional transition metal electrocatalysts with excellent OER and HMFOR activity.
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CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Hongyu Qu,Wende Hu,Xiangcheng Li,Rui Xu,Xiao Han,Junjie Li,Yiqing Lu,Yingchun Ye,Chuanming Wang,Zhendong Wang,Weimin Yang
Selective hydrogenolysis of biomass-based platform compounds is of great importance for the production of chemicals and fuels. Herein, we reported that the catalyst of Ni-C 3 N 4 supported on H 2 activated carbon (HC) synthesized by a simple coordination-impregnation-pyrolysis method is efficient for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF); the yield of 94.2% can be obtained in a batch reactor and the lifetime of greater than 120 h can be achieved in fixed-bed experiment. It is demonstrated that Ni nanoparticles coated by graphitic C 3 N 4 shell were highly dispersed on the surface of HC and the Ni loading is as low as 0.86 wt%, beneficial to the anti-sintering of Ni nanoparticles during the reaction. Both XPS characterizations and theoretical calculations reveal that Ni 3 N is the intrinsic active component for the hydrogenolysis , which exhibits efficient activity for the dissociation of C–O bond. This work opens up a new avenue to develop catalysts with single non-noble metal component for the efficient conversion of biomass-based chemicals.
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FUEL
·
2024
·
IF 6.7
Mei Ren,Jun Li,Manhong Huang,Donghui Chen,Xuelian Chen,Qi An,Songmei Sun
The escalating environmental issues resulting from waste plastic necessitate innovative decomposition methods that optimize conversion rates and product selectivity. In this study, we demonstrate that linear low-density polyethylene (LLDPE) can be effectively hydrothermolyzed into C1 − C4 compounds with a selectivity of 100 % in the presence of trace water on H-ZSM-5 catalyst under a relatively low temperature of 220 °C. Water plays a dual role here as both a solvent and a reactant. It was found the density of Brønsted acid sites is crucial for LLDPE decomposition, serving as the primary active centers for cracking LLDPE chains. In-situ EPR studies indicate a synergistic mechanism of free radical and carbenium ion pathways in LLDPE depolymerization. Density Functional Theory (DFT) simulations show that the depolymerization starts with the cleavage of a C–C bond in polyethylene, instigated by a hydrogen radical from the Brønsted acid site, leading to various intermediate stages for the formation of tert -butanol, acetone and acetic acid from two potential pathways. The presence of water is crucial in these pathways, aiding bond breakages and the creation of oxygenated products in the Brønsted acid site. This study represents a substantial leap forward in sustainable methodologies for upcycling plastic waste.
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RENEWABLE ENERGY
·
2024
·
IF 9
Ya-Peng Du,Xin-Yu Tian,Xiao-Ping Zheng,Yu Chai,Yu-Cang Zhang,Yan-Zhen Zheng
In this study, an innovative method for the high-efficiency production of 5-hydroxymethylfurfural (5-HMF) from cellulose were developed, overcoming the inherent recalcitrant physicochemical properties of cellulose. The method initiated with the ultra-high-pressure homogenization (UHPH) of a cellulose and formic acid mixture. This pre-treatment could highly enhance the 5-HMF yield compared with the reported pretreatment method. Following this, a catalytic system comprising a metal-based ionic liquid , 1-butyl-3-methylimidazole chloroaluminate ([BMIM][AlCl 4 ]) and acetic acid, was utilized to transform the pre-treated cellulose into 5-HMF. Reaction parameters such as temperature, duration, DMSO concentration, cellulose substrate amount, and the balance of ILs and organic acids were optimized to obtain the highest yield of 5-HMF. Besides, a combination of experimental characterization methods with quantum chemical calculations, aiming to elucidate the pre-treatment mechanisms was conducted. The integration of formyl groups into the cellulose structure and the intense shear forces applied during UHPH were observed. These factors contributed to disrupting the cellulose's chemical stability, reducing particle size, and shifting cellulose's structure towards a blend of crystalline cellulose and amorphous forms with decreasing crystallinity. These changes collectively heightened the reactivity of cellulose for subsequent catalytic transformations, fostering more effective interactions between the catalyst and substrate and thereby elevating the efficiency of cellulose conversion to 5-HMF.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2024
·
IF 4.3
Qian Zhang,Ruo Yu Yin,Zhi Huang,Yan-ying Liu,Jun-ming Hong
The development of high-efficiency catalysts for peroxymonosulfate (PMS) activation is critical for pollutant treatment in environmental applications. In this research, a Co organic framework (CoHHTP) combined with graphene oxide (GO) (CoHHTP/GO) with a 2D structure was prepared for PMS activation to treat the azo dye Reactive Black 5 (RBK5). The combination of CoHHTP and GO via oxygen groups resulted in the high activity of CoHHTP/GO, and almost 100 % performance was achieved within 30 min under various pH, temperature, PMS loading, and catalyst loading conditions. The maximum RBK5 removal efficiency was obtained with a catalyst loading of 3.0 g L −1 , PMS loading of 0.5 mM, temperature of 25 °C, and pH of 6 with a pseudo-first-order kinetics k value of 0.1903 min −1 . The activation energy of the CoHHTP/GO/PMS/RBK5 system was calculated to be 14.34 kJ mol −1 . Meanwhile, radicals and nonradicals, including SO 4 ·− , ·OH, ·O 2 − , and 1 O 2 , were proven to be generated and involved in RBK5 degradation. Moreover, RBK5 degradation pathways were identified through experimental research and density functional theory calculation.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Pui-Kei Lee,Co Vanessa Anna,Yang Yang,Murphy Lam Yim Wan,Hani El-Nezami,Danyue Zhao
Schisandrin B (Sch B) is a predominant bioactive lignan from the fruit of a Chinese medicine food homology plant, Schisandra chinensis . Previously, we observed potent anti-tumor effect of Sch-B in colorectal cancer (CRC) and enhanced chemotherapy efficacy with fluorouracil (5-FU). However, their bioavailability and reciprocal interactions under CRC conditions are unclear. In this study, we first compared the bioavailability, metabolism and tissue distribution of Sch-B between non-tumor-bearing and xenograft CRC tumor-bearing mice. Next, we examined SchB-5-FU interactions via investigating alterations in drug metabolism and multidrug resistance. Using a validated targeted metabolomics approach, five active metabolites, including Sch-B and fluorodeoxyuridine triphosphate, were found tumor-accumulative. Co-treatment resulted in higher levels of Sch-B and 5-FU metabolites, showing improved phytochemical and drug bioavailability. Multidrug resistance gene (MDR1) was significantly downregulated upon co-treatment. Overall, we demonstrated the potential of Sch-B to serve as a promising chemotherapy adjuvant via improving drug bioavailability and metabolism, and attenuating MDR.
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ChemSusChem
·
2024
·
IF 7.5
Akkammagari Putta Rangapppa,Wenhua Xue,Anirban Chowdhury,Yixuan Liu,Jong-Min Lee,Jun Zhao
The photocatalytic conversion of biomass-based platform molecules, such as 5-hydroxymethylfurfural (HMF), holds significant importance for the utilization of biomass resources. This study focuses on the unique ability of atomically bridged indium (In) atoms that encourages inactive SnS2 surface and steer the selective HMF oxidation process under solar light. Experimental results suggest that In confined SnS2 structure provides not only favorable sites and electronic structures for the synergistic activation of HMF/O2 but also benefit in charge carrier dynamics, thus influencing the overall activity and selectivity of the SnS2 catalyst. In addition, in-situ spectroscopy and density functional theory (DFT) analysis uncovered the multifunctional role of In sites in promoting the key steps of the catalytic process, from ROS generation to regulated adsorption/activation of *HMF which serves as the rate limiting step of the overall HMF oxidation process. Consequently, the optimized In-SnS2-0.75 photocatalyst demonstrated excellent photo oxidation performance, reaching a high HMF conversion efficiency, yield, and selectivity of 91.2, 73 and 80% respectively, in just two hours of the reaction. This study highlights the strategic approach of rationally designed catalytic systems in order to tune the ROS and the product distribution of the HMF oxidation process.
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JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Jia Ding,Yuanhao Wu,Shurong Wu,Shengyu Zhou,Yulong Li,Chao Fan,Hanxiao Liu,Penghui Ren,Shengwei Deng,Jianguo Wang
The direct carbonylation of glycerol with CO 2 is an alternative route to produce high-valued glycerol carbonate, which however faces challenges like low catalytic conversion due to the thermodynamic equilibrium limitation. In this work, ZSM-5 membranes with different Si/Al molar ratios were prepared by hydrothermal method, and coupled with Ce–La–Co mixed metal oxide (CeLaCo-MMO) catalysts for enhancing the glycerol carbonylation performance by in situ water separation. The Si/Al ratio of ZSM-5 showed significant influences on the water permeance, separation selectivity, and catalytic performance for glycerol carbonylation, due to the precise concentration control of Na + gated water transport channels. The reaction-separation coupling process achieved a glycerol conversion of 40.1 %, which was about 4.5 times higher than the conventional batch reactor. The as-synthesized ZSM-5 membrane also exhibited good reusability performance in the cycling test. This work provides a new in-situ water separation strategy for boosting glycerol carbonylation performance without consuming chemical or physical dehydrating agents as compared to the investigations in the literature.
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