ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Yu Yin,Chunhui Ma,Wei Li,Sha Luo,Zhanshuo Zhang,Shouxin Liu
Facilitated isomerization of cellulose hydrolysis intermediate glucose without unexpected byproducts, which is the rate-determining step in the production of high-value-added biofuels, enables the efficient production of 5-hydroxymethylfurfural (5-HMF) from cellulose. In this work, considering the essential role of the acidity control and shape selectivity of a zeolite catalyst, a NiO-loaded mesoporous NiO/poly(vinyl pyrrolidone) (PVP)-phosphotungstic acid (HPA)@SBA-15 nanoreactor was prepared. This SBA-15 nanoreactor with a pore size of 5.47 nm reduced the concentration of byproducts formic acid (FA) and levulinic acid (LA) through shape selection for intermediates. Well-defined NiO nanoparticles (Ni-to-carrier mass ratio was 1:1) provided the NiO/PVP-HPA@SBA-15 nanoreactor a high Lewis acidity of 99.29 μmol g–1 for glucose catalytic isomerization, resulting in an increase in total reducing sugar (TRS) yield by 5 times. Such a nanoreactor remarkably improved the reaction efficiency of 5-HMF production from cellulose (a 5-HMF selectivity of 95.81%) in the 1-butyl-3-methylimidazolium chloride ([BMIM]Cl)/valerolactone (GVL) biphasic system.
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FUEL
·
2023
·
IF 7.4
Yibo Zhang,Wei Wang,Chunlai Liu,Peihang Shen,Zelong Liu,Jianglei Hu,Fengwei Shi
In this work, we successfully synthesized a novel composite (HPW@MOF-199/SBA-15C, PMS-15C) in which MOF-199 encapsulated HPW catalyst (named HPW@MOF-199) was confined in SBA-15C, which is the carboxy-functionalized SBA-15. Physicochemical properties of the composites PMS-15C were systemically characterized by N 2 adsorption–desorption isotherms, wide-angle and low-angle XRD, XPS, FT-IR, SEM, and TEM. The results exhibited that HPW@MOF-199 had been successfully synthesized and embedded into the SBA-15C pores by COOH on the surface of SBA-15C. Meanwhile, the composites PMS-15C exhibited high activity and excellent reuse properties in the esterification reaction of acetic acid and ethanol, and no evidence of aggregation, leaching, or inactivation of HPW@MOF-199 during repeated use. The good dispersion of HPW within the MOF-199 cage and the interaction between HPW@MOF-199 and SBA-15C may be responsible for the good catalytic activity as well as the high stability of PMS-15C.
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高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Runqing Liu,Hongping Wu,Hongwei Yu,Zhanggui Hu,Jiyang Wang,Yicheng Wu
Four new Bi(III) phosphates, K 6 Bi 13 (PO 4 ) 15 , K 5 Bi(P 2 O 7 ) 2 , and A 5 Bi 5 (PO 4 ) 4 (P 2 O 7 ) 2 (A= K, Rb) with the different condensed P-O groups have been successfully synthesized via the solid-state reactions. The single crystals X-ray diffractions show that they crystallize in the different space groups (K 6 Bi 13 (PO 4 ) 15 : C 2; K 5 Bi(P 2 O 7 ) 2 : P 1 ¯ ; K 5 Bi 5 (PO 4 ) 4 (P 2 O 7 ) 2 and Rb 5 Bi 5 (PO 4 ) 4 (P 2 O 7 ) 2 : P 2 1 / c ). The structure of K 6 Bi 13 (PO 4 ) 15 can be described as a three-dimensional (3D) network composed of the Bi-O polyhedra and PO 4 tetrahedra with K atoms filling in the space to balance the residual charges. K 5 Bi(P 2 O 7 ) 2 features 2D [BiP 4 O 14 ] ∞ layers built by the BiO 6 octahedra and P 2 O 7 dimers and the adjacent [BiP 4 O 14 ] ∞ layers are bridged by the K atoms. A 5 Bi 5 (PO 4 ) 4 (P 2 O 7 ) 2 (A = K, Rb) contain two different condensed P-O groups, PO 4 tetrahedra and P 2 O 7 dimers, which are connected by Bi-O polyhedra to construct the complicated 3D framework with K/Rb atoms located in the tunnels. Note that, the compounds that simultaneously contain two different types of P-O groups are still rare in phosphates. Detailed structural comparisons of Bi 3+ -containing phosphates indicate that the Bi/P ratios have a significant effect on the condensed degrees of PO 4 groups. Furthermore, TG-DSC, IR, UV-Vis-NIR diffuse reflectance spectra and SHG test for title compounds have also been reported.
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JOURNAL OF APPLIED PHYSICS
·
2020
·Vol. 127
·期 11
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IF 2.286
Xu Xiang,Zou Yu,He Junjie,Zeng Yanning,Yu Caili,Zhang Faai
Mesoporous silica nanoparticles/polymer hybrid materials were prepared via metal-free surface-initiated atom-transfer radical polymerization (SI-ATRP). Self-synthesized mesoporous SBA-15 with surface hydroxyl groups was modified with (3-aminopropyl)-triethoxysilane, followed by anchoring of the ATRP initiator α-bromoisobutyryl bromide onto the surface via amide reaction. The SI-ATRP of methyl methacrylate was then carried out with fluorescein (FL) as a photocatalyst and trimethylamine (TEA) as an electron donor under irradiation with blue light. Thus, polymer chains grew directly from mesoporous walls. The hybrid materials were characterized by gel permeation chromatography, N 2 adsorption/desorption measurements, and thermogravimetric analysis. The effects of the ligand/photocatalyst molar ratios, solvent, and the monomer/initiator molar ratios on grafting density, molecular weight, and molecular-weight distribution were investigated. The results show that a higher TEA/FL ratio led to a higher reaction rate and better controllability of the polymerization but also to a lower grafting density. These properties were also affected by the solvent. With an increasing monomer/initiator molar ratio, the grafting rate, molecular weight, and grafting density exhibited increasing trends.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Junhua Zhang,Yao Liu,Shibo Yang,Junnan Wei,Liang He,Lincai Peng,Xing Tang,Yonghao Ni
Biorefinery for the purpose of producing biofuels, chemicals, and materials has received much attention. Furfural alcohol (FOL) and levulinate ester (LE) are important biomass-derived platform chemicals, and they are produced from sugar-based furfural (FAL). Unfortunately, the two products are often obtained separately in different reaction systems, which is undesirable; furthermore, it is of significant practical interest to control their selectivity so that the desired product can be accumulated in high yields. Herein, we present an efficient method for the highly selective conversion of FAL to FOL or isopropyl levulinate (IPL) in a one pot system using isopropanol as the hydrogen source and ZrO2@SBA-15 as a bifunctional catalyst with both Lewis acid and Brønsted acid sites. Under optimized reaction conditions, high yields of FOL and IPL in up to 90.4% and 87.2%, respectively, were obtained. Based on the experimental results, a kinetic model describing the catalytic conversion of FAL into FOL and IPL process has been established, which has a good correlation (R2 > 0.92) between the measured and predicted data. The developed kinetics can provide an effective tool to monitor the process and tailor the process conditions to obtain the desired product.
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JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Jichang Lu,Jian Fang,Zhizhi Xu,Dedong He,Siyou Feng,Yubei Li,Gengping Wan,Sufang He,Hua Wu,Yongming Luo
Supported MoS 2 based materials are widely used as heterogeneous catalysts. In this work, we propose a rapid and facile method (ultrasound-induced impregnation assisted by microwave thermal treatment) to synthesize mesoporous silica (SBA-15)-supported, few-layer, ordered and K-promoted MoS 2 nanosheets with different K/Mo ratios. The prepared catalysts are characterized by various physical and chemical techniques. Their catalytic performance is evaluated by methyl mercaptan (CH 3 SH) synthesis from CO/H 2 /H 2 S. The results show that our catalysts exhibit a much higher CO conversion and selectivity to CH 3 SH than the catalysts prepared using the conventional impregnation and reported in the literature. The good performance arises because of two main factors: MoS 2 nanosheets of only 2–4 layers and K promotion. Experimental characterizations and (density functional theory) calculations show that the former is the typical nano-size effect, and the latter stabilizes C S bonds when activating COS molecules.
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高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
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2020
·Vol. 44
·期 14
·11564-11582
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IF 3.741
Wei Liu,Hong Yuan
Summary Hydrogen is considered an ideal energy carrier. However, the use of fossil fuels to produce hydrogen depletes natural resources and causes environmental problems. Therefore, there is an urgent need to find alternative raw materials and technologies for the production of hydrogen. Waste cooking oil (WCO) is a renewable energy source that has emerged as a potential raw material for hydrogen production. This study describes the production of hydrogen and carbon nanotubes (CNTs) by catalytic cracking of a WCO model compound (WCOMC) performed in a lab-scale fixed bed using Ni-Co/SBA-15 catalysts. The phase, structure and reduction properties of the catalyst were analysed by using different characterisation methods. The effects of the nickel-cobalt metal content and the reaction temperature on both the hydrogen production and the quality of the CNTs were investigated. The deposited carbonaceous products were characterised to analyse their external appearance, internal structure, oxidation stability and graphitisation degree. The results indicated that the catalyst containing 20% Ni and 30% Co showed the highest activity. When reaction temperature was 800°C, the instantaneous volume fraction of hydrogen was close to 43.5 vol% and the content of hydrogen in the gas product was close to 66.5 vol%. A few multi-walled CNTs having a small diameter and some CNTs with an open-topped structure were deposited on 10%Ni-40%Co/SBA-15 and 30%Ni-20%Co/SBA-15, respectively. Thermogravimetric analysis and Raman spectroscopic analysis indicated that all CNTs showed high oxidation stability and a high degree of graphitisation.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2019
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IF 4.182
Lixue Gai,Qingda An,Zuoyi Xiao,Shangru Zhai,Haisong Wang,Weijie Cai,Zhongcheng Li
The configurations and compositions of an absorber play crucial role on the microwave absorption performance. Accordingly, the attenuation mechanism on the nanostructure with skillfully integrated components (e.g. dielectric loss and magnetic loss substances) is a highlight for constructing excellent absorbers. Herein, utilizing hierarchical succulent-like ZrSBA-15 as a template, the N-doped carbon layer containing Co nanoparticles embedded within ZrSBA-15 (Co-NCL@ZrSBA-15) composites were rationally constructed to acquire enhanced microwave absorption performance for the first time. The resultant Co-NCL@ZrSBA-15 composites exhibited high-performance microwave absorption capacity with low loading content of 25 wt % in a wax matrix. The minimum reflection loss (RL) value of −61 dB was achieved with the thickness of 2.0 mm at 16.8 GHz, and an effective frequency bandwidth (RL < −10 dB) was 4.4 GHz (13.6–18.0 GHz). Additionally, the minimum RL value are all less than −30 dB with thickness changing from 2.0 to 5.5 mm in the whole C, X and Ku absorbing band. Such excellent absorbing properties at lower filler loading and thin thickness endow the novel Co-NCL@ZrSBA-15 composites with gigantic potential for application in restrain electromagnetic wave pollution and interference.
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INTERNATIONAL IMMUNOPHARMACOLOGY
·
2023
·
IF 5.6
Na Li,Fanghan He,Yunxiao Shang
Obese asthma is a form of refractory asthma with inflammation as the underlying mechanism. The specific mechanism of action of anti-inflammatory growth differentiation factor 15 (GDF15) in obese asthma is unclear. The purpose of this study was to explore the effect of GDF15 on cell pyroptosis in obese asthma and to determine its mechanism of airway protection. Male C57BL6/J mice were fed with a high-fat diet, sensitized, and challenged with ovalbumin. Recombinant human (rh)GDF15 was administered 1 h before the challenge. GDF15 treatment significantly reduced airway inflammatory cell infiltration, mucus hypersecretion and airway resistant, and decreased cell counts and inflammatory factors in bronchoalveolar lavage fluid. Serum inflammatory factors decreased, and the increased levels of NLR family pyrin domain containing 3 (NLRP3), caspase-1, apoptosis-associated speck-like protein containing a caspase recruitment domain (ASC), and gasdermin-D (GSDMD-N) in obese asthmatic mice were inhibited. Furthermore, the suppressed phosphoinositide 3-kinase (PI3K)/AKT signal pathway was activated after rhGDF15 treatment. The same result was obtained by overexpression of GDF15 in human bronchial epithelial cells induced by lipopolysaccharide (LPS) in vitro, and the effect of GDF15 was reversed after the application of a PI3K pathway inhibitor. Thus, GDF15 could protect the airway by inhibiting cell pyroptosis in obese asthmatic mice through the PI3K/AKT signaling pathway.
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PubMed
高影响因子
ENERGY & FUELS
·
2018
·
IF 3.024
Lincai Peng,Xueying Gao,Xin Yu,Hui Li,Junhua Zhang,Liang He
An integrated multistep catalytic process in a one-pot cascade model to realize conversion is preferred in terms of process economics and energy efficiency. Here, we present the noble-metal-free but highly effective catalytic transfer hydrogenation and acid-catalyzed conversion of biomass-derived furfural for direct production of biofuel alkyl levulinate using alcohols as the hydrogen donor and reaction medium. With optimization of the process variables, a high yield of alkyl levulinate at up to 85.3% could be captured under mild conditions in isopropanol medium with the combination of Zr-MCM-41 and Amberlyst-15 catalysts. The reaction proceeds via the catalytic transfer hydrogenation of furfural to furfuryl alcohol over Zr-MCM-41, which is then converted to alkyl levulinate by an Amberlyst-15 acid catalyst. The spent hybrid catalysts could be effectively recovered from the resulting reaction mixture and reused 5 times with little deactivation after plain regeneration treatment.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2019
·
IF 2.298
Kui Wu,Ya Jun Li
The solubility and solution thermodynamics of azacyclotridecan-2-one in different solvents are indispensable for the purification and performance improvement of crystalline products in industry. In this paper, the solid–liquid equilibrium of azacyclotridecan-2-one in 15 pure solvents (methanol, ethanol, n-propanol, isopropanol, n-butanol, isobutanol, n-pentanol, ethyl acetate, acetone, toluene, acetonitrile, dichloromethane, 1,2-dichlorobenzene, cyclohexanone, and tetrahydrofuran) from 273.15 to 323.15 K at atmospheric pressure was measured. The mole fraction solubility increased with the increase in temperature in all solvents studied. The modified Apelblat equation, Van’t Hoff equation, Buchowski–Ksiazczak λh equation, and nonrandom two-liquid (NRTL) activity coefficient model were used to correlate the experimental data. Consequently, some association parameters were obtained. As a result, the NRTL model provided the best fitting. The solubility data provide the basic data for the design and optimization of the azacyclotridecan-2-one crystallization process.
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高影响因子
Journal of Physical Chemistry C
·
2018
·
IF 4.484
Zhenzhen Wang,Haoyang Zhang,Lili Chen,Songsong Miao,Shujie Wu,Xiufeng Hao,Wenxiang Zhang,Mingjun Jia
In this work, a series of amine-modified ZrSBA-15-supported PtPd bimetallic catalysts with different Pt/Pd ratios were prepared and characterized by a variety of means. Introducing amino groups on the surface of ZrSBA-15 is beneficial for achieving high dispersion of PtPd nanoparticles (NPs) and can effectively prevent the overgrowth of PtPd NPs during the preparation process. The resulting hybrid catalysts exhibit very high catalytic activity and stability for H2 generation from aqueous ammonia borane (AB) and can also efficiently catalyze the reduction of p-nitrophenol to p-aminophenol using AB as the hydrogen source. Among them, the catalyst with the Pt/Pd ratio of 85/15 shows the highest activity for AB dehydrogenation under ambient condition, whereas the catalyst with the Pt/Pd ratio of 50/50 exhibits the highest efficiency for the reduction of p-nitrophenol with AB. These results suggest that highly efficient interface active sites could be constructed by optimizing the composition of bimetallic PtPd NPs and changing the chemical surrounding of mesoporous ZrSBA-15, which demonstrate effective synergistic catalysis for AB dehydrogenation and p-nitrophenol reduction.
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