APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xinlei Ji,Jia Kou,Gökalp Gözaydın,Xi Chen
Chitin biorefinery offers a unique opportunity to sustainably produce highly-valued organonitrogen compounds such as the versatile pharmaceutical precursor 3-acetamido-5-acetylfuran (3A5AF), bypassing the Haber process and mitigating the consumption of fossil feedstocks. However, the reported protocols engaged large quantities of toxic organic solvents and required harsh conditions. In this work, a highly efficient catalytic system has been developed in the nontoxic, biobased γ-valerolactone (GVL) solvent under relatively mild conditions. 3A5AF was selectively obtained with an unprecedent yield of 75.3% at 140 °C for 2 h by adding NH 4 SCN and HCl. The high yielding was exclusively promoted by a dissolution-dehydration effect. Based on the UPLC-TOF-MS and NMR analyses, the presence of NH 4 SCN has induced a very rapid NAG conversion possibly by coordinating with the acetamido group and the hydroxyl groups, and the 3A5AF product was obtained in a subsequent dehydration pathway from NAG with the Chromogen I and Chromogen III as the intermediates.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
·
IF 8.2
Xu Liu,Xiao Han,Yushuang Shang,Lijuan Wang,Jian Shen,Jiang Yuan
Adverse factors such as high levels of glucose, oxidative stress , inflammation, and bacterial infection impede diabetic wound healing and even worsen wounds. Owing to its outstanding anti-inflammatory and antioxidant properties as well as the potential to promote cell migration and proliferation, hydrogen sulfide(H 2 S) gas therapy is promising for chronic diabetic wound recovery. In this work, a multifunctional poly(γ-glutamic acid)(PGA) hydrogel encapsulated with keratin-based H 2 S donor(KTC), ciprofloxacin(Cip), and anthocyanins(Ant) was developed. The resultant hydrogel was capable of releasing H 2 S, thereby promoting cell proliferation and enhancing anti-inflammation and antioxidant activity . The release of antibiotic Cip was accelerated under a diabetic wound microenvironment, thereby enhancing the antibacterial activity of the hydrogel. The encapsulated Ant could serve as a pH monitor, sensitively indicating wound pH conditions in situ and indirectly reflecting wound infection. In vivo results in diabetic wound healing suggested that PGA/Ant/KTC/Cip hydrogel reduced inflammation and promoted angiogenesis and collagen deposition, thereby accelerating wound healing.
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高影响因子
WATER ENVIRONMENT RESEARCH
·
2021
·Vol. 93
·期 8
·1361-1369
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IF 1.946
Shengkai Xu,Jiaxin Yang,Rafaat Hussein,Guangqing Liu,Bensheng Su
In this study, the performance of ofloxacin (OFX) degradation in synthetic wastewater using synthesized MnO x -CeO x /γ-Al 2 O 3 as a heterogeneous ozonation catalyst was evaluated. The removal rates of OFX and chemical oxygen demand (COD) during 15-day continuous-flow experiments were 98.2% and 76.7% on average, respectively. An ozone index (mgCOD/mgO 3 ) of 1.09 with a high ozone utilization efficiency of 91.39% was achieved. The pseudo-first-order rate constant of ofloxacin degradation reached 15.216 × 10 −2 min −1 , which was five times that (3.085 × 10 −2 min −1 ) without catalysts. The results of gas chromatography-mass spectrometry (GC-MS) demonstrated that a variety of small-molecule organics occurred in the final oxidation products, such as 4-hydroxyl-4-methyl-2-pentanone and 2-oxoadipic acid in addition to homologs of OFX. The results of this study suggested that hydroxyl radicals played critical roles in the degradation and mineralization of OFX via four main pathways: (a) electrophilic addition of nitrogen; (b) breakdown of carbon-carbon double bonds; (c) hydrolysis of ether rings; and (d) halodecarboxylation of carboxyl groups. The biodegradability (BOD 5 /COD) of OFX after catalytic ozonation reached 0.54. Practitioner points Ofloxacin wastewater was treated using catalytic ozonation in a 15-day continuous experiment with MnO x -CeO x /γ-Al 2 O 3 as a catalyst. The ozone index reached 1.09 mgCOD/mgO 3 during ozonation of ofloxacin. The presence of the catalyst increased the reaction rate constant by a factor of five. 4-hydroxy-4-methyl-2-pentanone was the primary ofloxacin oxidation product.
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ACS Applied Energy Materials
·
2021
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IF 6.024
Caihong Xue,Dandan Jin,Hui Nan,Haomin Wei,Huiyuan Chen,Chao Zhang,Shiai Xu
Poly(vinylidene fluoride) (PVDF) gel polymer electrolytes (GPEs) show great potential for application in lithium-ion batteries (LIBs) due to their outstanding characteristics. However, the inferior thermal stability and low ionic conductivity limit their practical application. Herein, γ-LiAlO2 was synthesized and applied in a polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP)-polybenzimidazole containing an ether bond (OPBI)-polyoxyethylene (PEO) (PHOP-LAO) GPE for improving its thermal stability and ionic conductivity properties. The ionic conductivity of PHOP-LAO is 4.83 mS cm–1, which increased by 210% compared with that of the PHOP sample. It is worth noting that the thermal shrinkage of the PHOP-LAO membrane is greatly reduced (less than 1% at 230 °C for 1 h). PHOP-LAO shows outstanding thermal stability, which is beneficial for the safety of LIBs. When the PHOP-LAO GPE was applied to LIBs with Li1.04Ni1/3Co1/3Mn1/3O2 as a cathode, the LIBs exhibit remarkable and stable cycling performance with a discharge capacity retention rate of 85% after 500 cycles at a 2 C rate and maintain a power capability retention rate of up to 77% of the initial capability at the high rate of 10 C (50 °C). PHOP-LAO thus shows great potential for achieving ultra-stable and safe LIBs in the future.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Jiankang Wang,Taiping Xie,Guokang Han,Quanxi Zhu,Yajing Wang,Yuan Peng,Songli Liu,Zhongping Yao
Cost-effective and low-toxicity of MnO 2 is regarded as a promising alternative to Co-based catalyst for peroxymonosulfate (PMS) activation to degrade recalcitrant organic pollutants. However, the sluggish Mn(IV)/Mn(III) redox cycling and limited specific surface area greatly hampered its wide application. To solve this challenge, a mesoporous γ-Fe 2 O 3 @MnO 2 magnetic catalyst with SiO 2 assistance (s-γ-Fe 2 O 3 @MnO 2 ) was synthesized. Physicochemical characterization confirmed part MnO 2 was coated on γ-Fe 2 O 3 surface while the other existed independently. Furthermore, BET surface area of s-γ-Fe 2 O 3 @MnO 2 was more than two times that of the counterpart without SiO 2 assistance (ws-γ-Fe 2 O 3 @MnO 2 ). s-γ-Fe 2 O 3 @MnO 2 exhibited enhanced PMS activation capacity with 97.6% phenol removal efficiency within 80 min, superior to other samples. Various influencing parameters on phenol oxidation were optimized. Reactive oxygen species (ROS) scavenging experiment and electron paramagnetic resonance (EPR) validated co-existence of hydroxyl radicals (·OH) and sulfate radicals (SO 4 · − ) as well as singlet oxygen ( 1 O 2 ) during PMS activation. However, phenol degradation was a non-radical oxidation process dominated by 1 O 2 . A rational reaction mechanism was proposed. Fe(II) promoted Mn(IV)/Mn(III) redox cycling and the enlarged surface area derived from SiO 2 mediated templating synthesis were responsible for the enhanced phenol degradation. This strategy can give a guidance for synthesis of highly efficient catalyst for sewage remediation.
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RENEWABLE ENERGY
·
2020
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IF 6.274
Han Chen,Qiong Xu,Du Zhang,Wenzhu Liu,Xianxiang Liu,Dulin Yin
A series of mesoporous nickel catalysts with different molar ratios of citric acid and nickel nitrate were synthesized via a simple two-step method by solid-state grinding and in-situ reduction; these catalysts were further employed for the catalytic transfer hydrogenation of levulinate esters to γ-valerolactone (GVL) with 2-propanol as the hydrogen donor. The effects of C 6 H 8 O 7 /Ni molar ratios , catalyst dosage, reaction temperature and time on the catalytic performance were investigated. An excellent GVL selectivity of 99.1% and an ethyl levulinate (EL) conversion of 100% could be achieved at 180 °C in 6 h over Ni-1.0 catalyst with a 1.0:1 M ratio of C 6 H 8 O 7 /Ni. The characterization results showed that the Ni-1.0 catalyst was composed of mesoporous metallic Ni bulk and a surface Ni–NiO composite, and the acid sites of NiO played a synergistic catalytic role in producing GVL from EL. The superior mesoporous structure and large surface area of Ni-1.0 increased the atomic utilization rate of nickel metallic active centers. Moreover, Ni-1.0 catalyst could be easily separated and reused ten times, with an EL conversion above 95% remaining in each recycle. This work provids a highly efficient and environmentally friendly catalytic procedure for the conversion of biomass into GVL, a fuel additive compound.
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International Journal of Nanomedicine
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2020
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IF 5.115
Shuping Wei,Chaoli Xu,Yidan Zhang,Zhongqing Shi,Min Wu,Bin Yang
Objective To investigate the antifibrotic effect of the combination of a PPARγ agonist-loaded nanoparticle-microbubble complex with ultrasound (US) exposure on renal interstitial fibrosis (RIF). Materials and Methods Polylactide-co-glycolide (PLGA) nanoparticles were used to load PPARγ agonist (rosiglitazone, RSG) and prepare PLGA-RSG nanoparticles (PLNPs-RSG); then, a novel complex between PLNPs-RSG and SonoVue microbubbles (MBs) (PLNPs-RSG-MBs) was prepared. The size distribution, zeta potentials, RSG-loading capacity and entrapment efficiency were measured, and the release of RSG was assessed using a UV-vis spectrophotometer. The in vitro cytotoxicity and in vivo systemic toxicity assays were performed. The cellular uptake assessment was performed using a confocal laser scanning microscope (CLSM). The in vivo biodistribution assessment was performed using fluorescence imaging with a near-infrared (NIR) imaging system. Furthermore, this complex was administered to a unilateral ureteral obstruction (UUO) rat model with the assistance of US exposure to investigate the antifibrotic effect. Results This PLNPs-RSG-MBs complex had a size of 2199.5± 988.1 nm and a drug-loading efficiency of 28.5%. In vitro cytotoxicity and in vivo systemic toxicity assays indicated that the PLNPs-RSG-MBs complex displayed excellent biocompatibility. In addition, the complex showed high cellular uptake efficiency in vitro and kidney-targeting ability in vivo. In a UUO rat model, the combination of the PLNPs-RSG-MBs complex with US exposure significantly reduced collagen deposition and successfully attenuated renal fibrosis. Conclusion The combination of the PLNPs-RSG-MBs complex with US exposure may be a promising approach for the treatment of RIF.
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Experimental and Therapeutic Medicine
·
2021
·Vol. 22
·期 2
·1-11
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IF 2.447
Jingli Zhang,Lingling Zhu,Hong Shi,Huizhe Zheng
Previous studies have demonstrated that microRNAs (miRNAs/miRs) serve a vital role in the pathogenesis of Sjögren's syndrome (SS). The present study aimed to investigate the role of miR‑155‑5p in SS and determine its underlying molecular mechanism. An inflammatory lesion model was established by stimulating salivary gland epithelial cells (SGECs) with interferon‑γ (IFN‑γ). The apoptosis of SGECs was measured by using flow cytometry. Levels of proinflammatory factors were detected by reverse transcription‑quantitative PCR and ELISA, respectively. Immunofluorescence was used for p65 staining. Dual‑luciferase reporter assay was performed to verify the interaction between miR‑155‑5p and arrestin β2 (ARRB2). The protein levels in the NF‑κB signaling pathway were assessed by western blotting. The results of the present study demonstrated that treatment with IFN‑γ increased miR‑155‑5p expression, in addition to inducing apoptosis and inflammation in SGECs. Furthermore, overexpression of miR‑155‑5p promoted IFN‑γ‑induced apoptosis and inflammation in SGECs. Overexpression of miR‑155‑5p also increased Bax protein expression, enzyme activities of caspase 3 and caspase 9, release of inflammatory cytokines interleukin‑6 and tumor necrosis factor‑α, and decreased Bcl‑2 protein expression in IFN‑γ‑treated SGECs. By contrast, all of the effects aforementioned were reversed following miR‑155‑5p knockdown. These results demonstrated that miR‑155‑5p activated the NF‑κB signaling pathway, where treatment with the NF‑κB inhibitor, pyrrolidine dithiocarbamate, reversed the effects of miR‑155‑5p overexpression on the inflammatory factors in IFN‑γ‑induced SGECs. miR‑155‑5p was demonstrated to target ARRB2 and negatively regulated its expression levels, such that overexpression of ARRB2 reversed the effects of miR‑155‑5p overexpression on the inflammatory response, apoptosis and the NF‑κB signaling pathway in IFN‑γ‑treated SGECs. Collectively, results from the present study suggest that miR‑155‑5p may activate the NF‑κB signaling pathway by negatively regulating ARRB2 to promote salivary gland damage during SS pathogenesis. This suggests that miR‑155‑5p may serve to be a potential target for the treatment of SS.
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
·
2019
·Vol. 93
·期 2
·391-401
·
IF 1.986
Yi Huilin,Wan Yanchun,Zhang Yang,Wang Yujun,Fei Weiyang,Luo Guangsheng
This study describes a novel and facile route for fabricating highly uniform γ-alumina microspheres with controllable size, morphology, and pore structure by integrating the sol–gel route for alkoxide with “temperature/pH-induced gelation” in a coaxial microchannel. Taking advantage of the controllability of the microfluidic devices and Al–O–Al chains formed by the sol–gel route of aluminum alkoxide, the uniformity of the microspheres was assured, and the mechanical strength of the microspheres was greatly improved to 18–27 N/mm 2 . The effects of the continuous phase composition and two-phase flow rate on the size, morphology, and pore structure of the obtained microspheres were investigated. When triocylamine (TOA) was added to the continuous phase and the two-phase flow rate ratio was larger than 188, the as-prepared microspheres had a smooth surface and good sphericity; otherwise, the microspheres had poor spheriticy and included many ravines on the surface, which can be explained by the mutual influence of long-lasting movements of molecular chains resulted from low gelation speed and inner circulation of the droplets. Under different continuous phase compositions, the average pore diameter, pore volume, and specific surface area ranged from 7 to 12 nm, 0.89 to 1.58 mL/g, and 293.7 to 387.7 m 2 /g, respectively.
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CARBOHYDRATE POLYMERS
·
2019
·
IF 6.044
Qingqing Yu,Weijun Yang,Qianqian Wang,Weifu Dong,Mingliang Du,Piming Ma
In this work, functionalized cellulose nanocrystal (fCNC) was obtained by the grafting of 3-methacryloxypropyltrimethoxysilane coupling agent (γ-MPS) onto CNC. Then acrylic pressure sensitive adhesive (PSA) incorporated with various contents of CNC or fCNC was successfully synthesized by an in-situ emulsion polymerization , and the effects of CNC or fCNC on the sol molecular weight, latex properties, thermal properties, viscoelastic properties, and adhesive performance of the acrylic PSA were investigated. The results illustrated a coinstantaneous improvement of tack, shear strength and peel strength with increasing the loading of both CNC and fCNC. Interestingly, fCNC showed much more improvement than CNC on adhesive performance of acrylic PSA. The fCNC-1/acrylic PSA showed tack of 27#, shear strength of 70 h, and peel strength of 13.4 N/25mm, which were 12.5%, 4%, and 106% higher than those of CNC-1/acrylic PSA and 35%, 100%, and 163% higher than those of neat acrylic PSA, respectively. The superior adhesive performance of the fCNC/acrylic PSA films was supposed to be attributed to better compatibility and dispersion of fCNC in the acrylic copolymer. Thus, this work presents a feasible strategy for utilization of CNC in adhesives and coatings.
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CHEMOSPHERE
·
2019
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IF 5.108
Rongji Cui,Suxia Ma,Jie Wang,Shujun Sun
The catalytic gas-phase H 2 O 2 oxidation of NO was achieved over Fe-based catalysts supported on montmorillonite K10, γ-alumina and ZSM-5. ESR tests illustrate that the three catalysts can catalyze decomposition of H 2 O 2 yielding highly reactive hydroxyl radicals , of which Fe/K10 has the fastest rate, followed by Fe/γ-alumina. Fe 3+ in Fe/K10 and Fe/γ-alumina show lower density of electron cloud due to a strong interaction between Fe 3+ and the support, which benefits the electron transfer from the H 2 O 2 to Fe 3+ , thus favoring the production of hydroxyl radicals. Fe species exist on the surface of Fe/K10 mainly in the form of Fe 2 O 3 , whereas Fe species of Fe/γ-alumina and Fe/ZSM-5 exist mainly in the form of Fe 3 O 4 , and it is found that Fe 2 O 3 is more active than Fe 3 O 4 in catalytic gas-phase H 2 O 2 oxidation of NO. Interestingly, Fe/ZSM-5 has the lowest efficiency in generating hydroxyl radicals, its NO removal efficiency is 90%, which is much higher than 47.5% for Fe/γ-alumina and 62.3% for Fe/K10. In-situ IR results suggested that Fe/ZSM-5 are dual functional in oxidation of NO, that is, whether both Fe ion sites and Brønsted acid sites collectively provide the catalytic functionality. In the meantime, a possible reaction mechanism on catalytic gas-phase H 2 O 2 oxidation of NO over Brønsted acid sites is proposed.
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APPLIED CATALYSIS A-GENERAL
·
2018
·
IF 4.521
Zhenzhen Lin,Mengting Luo,Yindi Zhang,Xiaoxue Wu,Yanghe Fu,Fumin Zhang,Weidong Zhu
Heterogeneous catalytic conversion of biomass-derived methyl levulinate (ML) to γ-valerolactone (GVL) is highly attractive as a sustainable route to mitigating the dependence on nonrenewable fossil resources. However, this route is limited by its low selectivity toward GVL and severe reaction conditions. Here, we present a synergistic catalytic process that offers exclusive GVL selectivity with complete ML conversion under mild conditions (80 °C, 0.5 MPa of H 2 pressure). This is achieved over a dual-functionalized catalyst of Ru nanoparticles (Ru-NPs) and Brønsted acid SO 3 H groups in a Cr-based metal-organic framework (MIL-101). The Ru-NPs served as metal sites for the hydrogenation of ML to methyl-3-hydroxyvalerate (MHV) and the acidic SO 3 H moieties promoted the cyclization of MHV to generate GVL via lactonization. In contrast, GVL production was significantly suppressed over the physically mixed congener (2.0 wt% Ru/MIL-101 + MIL-101-SO 3 H). This result demonstrates an unrivalled advantage of the dual integration of metal/acid sites in a single MOF crystal, and the relative amount of sulfonic acid groups in the catalyst can exert significant influence on the overall catalytic performances. The activation energies for the hydrogenation and lactonization steps with the developed catalyst were 29.5 and 42.1 kJ/mol, respectively, which are much lower than those observed with the traditional 5.0 wt% Ru/AC catalyst.
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