ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Tianyun Jing,Shaokang Yang,Tingting Li,Yangyang Wan,Huimin Jia,Yonghai Feng,Yunpeng Zuo,Dewei Rao
Atomic scaling of cobalt-based catalysts is the feasible and sustainable approach for selective oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to produce bio-plastic monomer of 2,5-furandicarboxylic acid (FDCA) under mild conditions. Here, a high-efficiency dual single-atomic Co/Cu supported on nitrogen-doped carbon (a-Co/Cu-NC) is constructed. Leveraging exceptional oxygen activation ability, the Co/Cu dual-atomic-sites can accelerate the HMF oxidation, suppressing by-product formation mediated by reactive oxygen species (ROS) in low-oxygen environments. This leads to enhanced FDCA selectivity with a yield of 98% and a production rate of 298.8 mmol FDCA g metal −1 h −1 under ambient conditions. Comprehensive experiments and density functional theory (DFT) calculations demonstrate that long-range interactions between Co and Cu sites optimize reactant adsorption and lower energy barriers for •O 2 − and HMFCA formation.
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LANGMUIR
·
2024
·
IF 3.7
Yongzhi Xiong,Jianchun Jiang,Yajun Liu,Xialin Ji,Changzhou Chen,Kui Wang
The electrooxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) demonstrated its unique superiority, not only in reducing overpotential and improving energy conversion efficiency for green hydrogen production but also in utilizing abundant biomass resources and producing high-value-added chemicals. However, designing highly efficient electrocatalysts for HMF electrooxidation (HMF-EOR) with low cost and high performance for large-scale production remained a huge challenge. Herein, we introduced an easy one-step activation process to produce P-doped porous biochar loaded with multiple crystal surfaces exposed to CoP2O6 catalysts (CoP2O6@PC), which exhibited outstanding electrooxidation performance. To achieve a current density of 50 mA cm–2, only a low overpotential of 200 mV was needed for the electrooxidation of HMF in 1.0 M KOH + 10 mM HMF. This performance far surpassed that of other similar materials. CoP2O6@PC exhibited outstanding HMF-EOR performance with high conversion (nearly 100%), selectivity (97.1%), faradaic efficiency (95.3%), and robust stability. This work represents a promising strategy to fabricate macroscale and low-cost HMF-EOR electrocatalysts and achieve potential industrial applications of HMF-EOR.
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PubMed
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ANTI-CANCER DRUGS
·
2025
·
IF 2.2
Luo Kairan,Hu Wenbin
Intelligent hydrogels are promising in constructing scaffolds for the controlled delivery of drugs. Here, a dual thermo- and pH-responsive hydrogel called PCG [poly ( N -isopropyl acrylamide-co-itaconic acid)/chitosan/glycerophosphate (PNI/CS/GP)] was established as the carrier of 5-fluorouracil (5-FU) for triple-negative breast cancer (TNBC) treatment. The PCG hydrogel was fabricated by blending synthesized [poly ( N -isopropyl acrylamide-co-itaconic acid), pNIAAm-co-IA, PNI] with CS in the presence of GP as a crosslinking agent. The interaction between PCG hydrogel compositions was characterized by Fourier transforms infrared, NMR spectroscopy, and scanning electron microscopy. The PCG hydrogel presented an interconnected and porous structure with similar pore size, rapid swelling/deswelling rate in response to both temperature and pH change, and biocompatibility, upon which it was proposed as a great drug carrier. 5-FU had a dual thermo- and pH-responsive controlled release behavior from the PCG hydrogel and displayed an accelerated release rate in an acidic pH environment than in a neutral pH condition. The application of 5-FU-loaded PCG hydrogel exhibited a more promoted anticancer activity than 5-FU against the growth of TNBC cells both in vitro and in vivo . The outcomes suggested that the PCG hydrogel could be an excellent platform for local drug-delivery systems in the clinical therapy of TNBC.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xuan Gao,Zhihui Li,Shuxing Zhang,Dongsheng Zhang,Xinqiang Zhao,Baoquan Zhang,Yanji Wang
Developing cost-effective and inherently safe methods for accelerating the sustainable production of value-added chemicals from biomass presents a promising solution to the current energy crisis. This study introduces heterogeneous copper species anchored on a γ-Al 2 O 3 catalyst (Cu/γ-Al 2 O 3 ) with high dispersibility and small Cu particle size, synthesized via a straightforward incipient-wetness impregnation method. This method facilitates the selective anaerobic dehydrogenation of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) in the absence of any oxidant or hydrogen acceptor. An HMF conversion of 69.8 % and a DFF yield of 44.9 % were attained at 130 °C over a 12-h period. Extensive characterizations were conducted to elucidate the correlation between the catalyst’s structure and its dehydrogenation activity. The findings indicated that strong L-acid sites, elevated Cu dispersions, small Cu particle size and an increased number of Cu + active sites were conducive to enhanced dehydrogenation reactivity. The Cu/γ-Al 2 O 3 catalyst demonstrated superior catalytic efficiency and stability. A possible reaction mechanism is suggested, integrating DFT calculations with experimental observations. This research offers valuable insights into the selective conversion of HMF to DFF and encourages further exploration into the dehydrogenation of biomass alcohols into high-value chemicals under oxidant-free conditions.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Ting He,Shanshan Zhang,Yang Zhu,Jiangwei Chen,Xiaoyun Wang,Qingguo Li,Rizhi Chen,Wenbo Pei,Xin Chen,Haibao Duan,Zhaoliang Cui
Extracorporeal CO 2 removal (ECCO 2 R) is a type of extracorporeal life support (ECLS) technology. It aims to remove carbon dioxide (CO 2 ) from small flow of the blood and correct hypercapnia and related acidosis. The ECCO 2 R system removes CO 2 retained in the patient’s body through the gas-blood exchange membranes, which in use, blood flows on the outside of the membrane, and the inside of the membrane is for gas flow. Existing ECCO 2 R system generally improves the emission rate of CO 2 by the increase of the gas flow rate. However, there is a problem that O 2 is simultaneously taken out, which will reduce the blood O 2 concentration. Therefore, the gas-blood exchange membranes should not only increase the CO 2 removal rate by the improvement of CO 2 /O 2 selectivity, but also retain more O 2 in the blood and then maintain the oxygen saturation of the blood. In present work, a method was proposed to fabricate COF-5/Pebax mixed matrix membranes (MMMs) on the PMP surface for enhancing CO 2 /O 2 selectivity, which was increased from 0.96 to 5.57. The CO 2 removal ability of COF-5/Pebax MMM was tested by blood circulation, and it was found that the CO 2 removal effect was increased 10.9% than that of the pristine membranes. The O 2 concentration was maintained at a higher level, about 1.69 times that of the pristine membranes. In contrast to the pristine PMP membrane, blood compatibility of COF-5/Pebax MMMs was improved because protein adhesion decreased by 44.75%. The results of cytotoxicity test and rabbit pyrogen test exhibited that the prepared COF-5/Pebax MMM presented great biosafety. Overall, the proposed COF-5/Pebax MMM has good performance in ECCO 2 R system and attractive potential for medical application.
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Separations
·
2024
·Vol. 11
·期 2
·39
·
IF 2.5
Zhenhua Sun,Qingxiang Shu,Qikun Zhang,Shaopeng Li,Ganyu Zhu,Chenye Wang,Jianbo Zhang,Huiquan Li,Zhaohui Huang
ZSM-5 zeolite is a kind of high-value-added porous aluminosilicate zeolite. The use of the coal gasification slag utilization process by-product desilication liquid as a silicon raw material to replace the current raw materials such as water glass will help reduce production costs and achieve high-value utilization of solid waste. ZSM-5 zeolites for volatile organic compounds (VOCs) adsorption were prepared by a one-step hydrothermal method using the desilication solution prepared from coal gasification slag as the main silicon source and sodium source. The effects of crystallization reaction time, the crystallization temperature, the Na2O/SiO2molar ratio, and the SiO2/Al2O3molar ratio on the relative crystallinity and the specific surface area of the ZSM-5 zeolite were investigated and optimized. The optical reaction conditions were as follows: a crystallization time of 12 h, a crystallization temperature of 170 °C, a Na2O/SiO2molar ratio of 0.2, and a SiO2/Al2O3molar ratio of 200. The optimal ZSM-5 zeolite synthesized is hexagonal, with regular grains, a relative crystallinity of 101.48%, a specific surface area of 337.48 m2·g−1, and a pore volume of 0.190 cm3·g−1. And the optimal ZSM-5 zeolite was composed of SiO2content of 97.52 wt%, Al2O3content of 1.58 wt%, Na2O content of 0.33 wt%, and SiO2/Al2O3molar ratio of 104.93. Na2O/SiO2molar ratio is 0.0033. The results of static adsorption experiments show that the static adsorption capacities of ZSM-5 zeolite forp-xylene, benzene, toluene, and butyl acetate were 118.85, 69.98, 68.74, and 95.85 mg·g−1, respectively, which can effectively adsorb VOCs. The synthetic process of the ZSM-5 zeolite is a simple preparation process and short in synthesis time. The results of this study not only help to realize the high-value utilization of silicon components in solid waste, but also provide an economical and effective way to synthesize VOCs adsorption materials.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2015
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IF 2.587
Jinxia Zhou,Tingyu Huang,Yuling Zhao,Zhi Xia,Zhanwei Xu,Songyan Jia,Jianji Wang,Z. Conrad Zhang
Ionic liquids have been widely studied as effective reaction media for the conversion of glucose or cellulose to 5-hydroxymethhylfurfural (5-HMF). However, the recovery of 5-HMF from ionic liquids, typically carried out by extraction, has been encountered with very low extraction efficiency, which limited the reusability of the solvents. Through this work, based on the model biphasic system that consists of 1-butyl-3-methylimidazolium chloride ([BMIM]Cl) as the ionic liquid phase and methyl isobutyl ketone (MIBK) as the extractant phase, the dominant force that suppresses the extraction efficiency of 5-HMF was identified as being the strong hydrogen bonding between 5-HMF and [BMIM]Cl. Solvent mediation with functional promoters have been established as a new strategy to shift this force, resulting in improved extraction efficiency of 5-HMF from the ionic liquid. For example, with ethanol as a promoter, the distribution coefficient of 5-HMF was about 10 times higher than that without a promoter.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2016
·
IF 4.179
Fan Wang,Ziliang Yuan,Bing Liu,Shaohua Chen,Zehui Zhang
In this study, a new ruthenium catalyst was used for the oxidation of biomass derived 5-hydroxymethylfurfural (HMF) under mild conditions, which was prepared by the exchange of Ru 3+ with H + in the structure of the zirconium phosphate (ZrP). The as-prepared ZrP–Ru catalyst showed high catalytic activity towards the oxidation of HMF, affording 100% of HMF conversion at 130 °C after 12 h under atmospheric oxygen pressure. 2,5-Furandicarboxylic acid (FDCA) and 2,5-diformylfuran (DFF) were detected to be the major oxidation products.
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Polymer Chemistry
·
2016
·Vol. 7
·期 19
·3268-3276
·
IF 5.687
Ye Chen,Leilei Rui,Lichao Liu,Weian Zhang
Supramolecular amphiphiles based on a pillar[5]arene with enhanced photodynamic therapy have been fabricated. Supramolecular amphiphiles based on host–guest complexation between a poly(ethylene glycol)-functionalized pillar[5]arene (PEG-P[5]A) and a pyridinium-terminated porphyrin derivative bearing a disulfide bond (TPPC6-SS-Py) could self-assemble into spherical micelles in aqueous solution with good colloidal stability as confirmed by transmission electron microscopy (TEM) and dynamic light scattering (DLS). Also, PEG-P[5]A/TPPC6-SS-Py micelles exhibited rapid release of porphyrin photosensitizers in a reducing environment. In addition, these micelles demonstrated nearly no toxicity in the dark but a higher photocytotoxicity upon light irradiation evaluated by the MTT assay. Flow cytometry and confocal laser scanning microscopy (CLSM) revealed a more effective cellular uptake property compared with free porphyrin. Therefore, novel reduction-responsive supramolecular amphiphiles with rapid drug release and superior cell internalization ability are constructed, which may provide a platform for drug delivery systems.
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MOLECULAR CRYSTALS AND LIQUID CRYSTALS
·
2016
·
IF 0.532
J. Wei,K. Liu,F. Lin,Y. Zhou,J. Zou,C. Lin
Through the sulfonation of protocatechuic acid, sodium 5-carboxy-2,3-dihydroxybenzenesulfonate (SPA) was synthesized. The structure of the sulfonated derivative was confirmed by FT-IR, MS, 1H NMR, 13C NMR, single crystal X-ray diffraction, and thermogravimetric analysis. The antioxidative activities of the derivative SPA were evaluated using 1,1-diphenyl-2-picrylhydrazyl (DPPH) scavenging method and reducing power determination, showing that SPA had strong antioxidative effects. Meanwhile DPPH scavenging progress by SPA was analyzed from dynamics experiments. Isothermal titration calorimetry (ITC) and circular dichroism (CD) were applied to investigate the interaction between the derivative SPA and human serum albumin (HSA).
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ANALYTICAL BIOCHEMISTRY
·
2017
·
IF 2.334
Lu Chen,Hui-Ting Lian,Xiang-Ying Sun,Bin Liu
A novel electrochemical sensor was presented for the determination of L-5-hydroxytryptophan (L-5-HTP) based on a graphene-chitosan molecularly imprinted film modified on the surface of glassy carbon electrode (GR-MIP/GCE). The morphology and composition of the imprinted film were observed in field emission scanning electron microscopy (FESEM), raman spectroscopy and fourier transform infrared (FTIR). The properties of the sensor were evaluated by electrochemical techniques. Under the optimal conditions, the peak currents of L-5-HIP were found to be linear in the concentration range of 0.05–7.0 μM, while the sensor also exhibited great features such as low detection limit of 6.0 nM (S/N = 3), superb selectivity against the structural analogues, good antidisturbance ability among coexisting components, excellent repeatability and stability. Moreover, the proposed method had been applied to the detection of L-5-HTP in human blood serum with a satisfactory recoveries ranging from 90.6% to 105.6%.
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JOURNAL OF MOLECULAR LIQUIDS
·
2017
·
IF 3.648
Jiang Xiao,Yongzhong Jia,Chenglong Shi,Xingquan Wang,Su Wang,Ying Yao,Yan Jing
A green and efficient liquid–liquid extraction system was developed for the separation of lithium isotopes by using hydrophobic ionic liquids (ILs = [C 4,6,8,10 mim] + [NTf 2 ] − ) as extraction organic phase and benzo-15-crown-5 (B15C5) as complexing agent. The maximum single-stage separation factor α of 6 Li/ 7 Li obtained in this study was 1.029 ± 0.001, indicating 6 Li was enriched in ionic liquid phase while 7 Li was concentrated in the aqueous phase. The lithium ion was extracted into the ionic liquid in the formation of 1:2 complex [Li + (B15C5) 2 ]. The negative data of thermodynamic parameters (∆ H 0 and ∆ G 0 ) suggest that the extraction system was a spontaneous exothermic process . In addition, effective lithium isotopes separation factor and the extraction efficiency of lithium ions can be gained in the condition of lower temperature with softer counter anions in the novel extraction system.
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