INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Xiangbo Song,Jun Yue,Yuting Zhu,Chengyan Wen,Lungang Chen,Qiying Liu,Longlong Ma,Chenguang Wang
Efficient and one-pot conversion of biomass-derived carbohydrate into highly value-added 5-hydroxymethylfurfural (HMF) is a crucial reaction step for the valorization of biomass resources toward bio-based chemicals and fuels. In this work, a series of Sn/SAPO-34 catalysts were prepared through impregnation and evaluated in glucose conversion to HMF. The physicochemical properties of Sn/SAPO-34 catalysts were systematically characterized by SEM, XRD, N2 physisorption, XPS, solid-state 119Sn, 29Si, and 31P NMR, XRF, UV–vis, NH3-TPD, and pyridine-FTIR techniques. It was demonstrated that controlling the Sn loading amount could facilely adjust the acid strength and acid amount of the SAPO-34 zeolite. The incorporation of Sn species could induce the formation of a tetrahedrally coordinated Sn4+ site and Sn-OH site to improve the amounts of Brønsted and Lewis acid sites of the catalyst. However, modification with sufficiently high Sn loading could decrease the acid strength and performance of the catalyst owing to its structure damage. The 5%Sn/SAPO-34 catalyst (i.e., Sn loading calculated based on the mass ratio of SnCl4·5H2O as a precursor to the parent SAPO-34) was found to exhibit the superior catalytic performance under mild conditions and could afford an HMF yield of 64.4% at 98.5% glucose conversion in a biphasic 35 wt % NaCl-H2O/tetrahydrofuran (THF) system at 150 °C within 1.5 h. Additionally, a catalytic reaction pathway was proposed, involving the adsorption of glucose molecules by the −Cl group on the catalyst via a hydrogen bond, followed by glucose isomerization to fructose over the Lewis acid Sn4+ and Al3+ sites and, finally, fructose dehydration to HMF catalyzed by the Brønsted acid Sn-OH and Si-OH-Al sites. The activity of the catalyst decreased due to the leaching of the active site Sn after several consecutive cycles. This work provides insights into the improvement in the Sn-containing zeolite catalyst for tandem conversion of glucose to HMF.
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ChemCatChem
·
2021
·Vol. 13
·期 13
·3027-3036
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IF 5.686
Zhijian Wan,Youkun Tao,Hengzhi You,Xiang Zhang,Jing Shao
Graphical Ammonia decomposition : Ni nanoparticles with a mean size of ∼2.3 nm anchored on Na-ZSM-5 nanocrystals were prepared as a catalyst to effectively crack ammonia for CO x -free H 2 production. Ammonia has been increasingly recognised as an effective hydrogen carrier to produce clean hydrogen free of CO x emissions. This study reports the development of Ni-based catalysts to efficiently crack ammonia into hydrogen and nitrogen. A series of catalysts with different Ni loadings supported on Na-ZSM-5 zeolite nanocrystals were prepared with the assistance of 1,10-phenanthroline ligand. The coordination of Ni and the ligand led to the formation of uniform Ni nanoparticles with a mean size of ∼2.3 nm. These small Ni nanoparticles of the catalyst enabled a high activity in ammonia decomposition evaluated using a fixed-bed reactor. Using the zeolite support in its pristine sodium form provided the catalyst with desired basicity. This promotes a strong metal-support interaction, leading the catalyst to have high stability. The catalyst with 5 wt% Ni loading exhibited a high TOF of 3.51 s −1 with no performance degradation at 650 °C for 50 h.
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CHEMICAL ENGINEERING SCIENCE
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2021
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IF 4.311
Tingting Qi,Yingying Kang,Moses Arowo,Yong Luo,Guang-Wen Chu,Liangliang Zhang,Hai-Kui Zou,Baochang Sun,Jian-Feng Chen
In this study, hierarchical ZSM-5 zeolites are hydrothermally prepared using rotating packed bed (RPB) in premixing process (gelation stage). The impact mechanisms of RPB on the zeolite growth process are investigated. It is found that the zeolite precursor obtained by RPB contains abundant bubbles, and aluminosilicate aggregates in the precursor are broken and dispersed uniformly, which is beneficial for the uniform and fast growth of zeolite. Additionally, the effects of various RPB-premix process parameters, including rotation speed, premixing time, and liquid feed rate on the particle sizes of ZSM-5 are systematically investigated. The prepared ZSM-5 zeolites by RPB-premix route exhibit smaller particle sizes, narrower particle size distributions, larger specific surface areas, richer pore structure, and more acid amount compared with those by traditional premix treatment. Therefore, this study provides a novel approach for the synthesis of high-performance ZSM-5 zeolites.
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FUEL PROCESSING TECHNOLOGY
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2020
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IF 4.982
Zi Zeng,Jiaoyang Xie,Yue Guo,Ruiheng Rao,Bo Chen,Lihua Cheng,Ying Xie,Xinping Ouyang
Highly dispersed Fe Pd bimetallic catalyst supported on HZSM-5 (Fe-Pd/HZSM-5) was prepared by impregnation method for the hydrogenolysis of lignin. The correlation between the textural properties of the catalyst and its catalytic activity to lignin hydrogenolysis were investigated. The presence of Fe facilitates the dispersion of Pd, and the particle size decreases from 6.1 nm for 3.0 wt% Pd/HZSM-5 (Pd-3.0) to 2.5 nm for 9.0 wt% Fe-1.0 wt% Pd/HZSM-5 (FP-1.0). Fe is mainly existed in the oxidized state which means that electrons in Pd tend to transfer to FeO x , facilitating the activation of H 2 to form active H atoms. Due to the geometric and electronic synergistic effects , FP-1.0 bimetallic catalyst exhibits a good catalytic activity to lignin hydrogenolysis, contributing to as higher as 98.17% of lignin conversion and 27.92% of aromatic monomers yield under the optimal reaction conditions of 1 MPa H 2 at 320 o C for 120 min in ethanol-water solvent. FP-1.0 bimetallic catalyst with low cost and highly catalytic activity may be a potentially useful catalyst for selective hydrogenolysis of lignin.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2020
·
IF 4.551
Tingting Qi,Jing Shi,Xishuo Wang,Kun Dong,Yong Luo,Jiawei Teng,Guang-Wen Chu,Hai-Kui Zou,Baochang Sun
Hierarchical (micro/mesopore) ZSM-5 zeolites were hydrothermally synthesized in a rotating packed bed (RPB) which substantially enhances micromixing for the high viscosity reaction system. Herein, the effects of four operating processes with different micromixing intensity on nucleation/crystal growth process as well as physicochemical properties of ZSM-5 zeolites were investigated. Results indicate that enhancing micromixing by RPB in the zeolite synthesis could facilitate the formation of Al sites and shorten the nucleation and crystallization period. ZSM-5 samples prepared by RPB exhibit hierarchical structure, smaller average particle size, more uniform particle size distributions , larger specific surface areas, higher catalytic stability as well as more acid sites than those obtained by (stirring tank reactor) STR. While adopting the ZSM-5 samples prepared by RPB for catalyzing C4-olefin cracking reaction, the conversion of C4-olefin and yield of propylene are higher than those obtained by STR.
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Expert Opinion on Drug Delivery
·
2020
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IF 4.838
Pu Guo,Chao Pi,Shijie Zhao,Shaozhi Fu,Hongru Yang,Xiaoli Zheng,Xiaomei Zhang,Ling Zhao,Yumeng Wei
Background A novel nanoemulsion (CU/FU-LN) was developed as an oral 5-fluorouracil and curcumin co-delivery system for synergistic efficacy against liver cancer.Methods MTT assay, confocal laser scanning microscope, and H&E staining were utilized to establish the efficacy and safety of CU/FU-LN.Results The AUC(0-t) of CU/FU-LN was 8.85-fold and 8.59-fold greater than those of CU and FU, respectively. The IC50 of CU/FU-LN was 4.6-fold and 4.9-fold lower than those of FU and CU in HepG2 cells, respectively. In vivo anti-tumor trials, the tumor inhibition rate was significantly elevated by CU/FU-LN (49.29%), compared 24.84% and 4.72% for FU and CU, respectively. Ki-67 immunohistochemical analysis revealed that CU/FU-LN had an obvious anti-proliferation effect. The IC50 of CU/FU-LN in L02 cells was 1.51-fold and 2.60-fold higher than those of CU and FU, respectively. Certain vital organs in the mice of the CU/FU-LN group showed markedly fewer lesions than those of the CU, FU, and CU+FU groups. The CU/FU-LN treatment caused no significant change in mouse body weight relative to the control group (P > 0.05). Conclusions We successfully prepared a promising co-delivery platform for the synergistic treatment of liver cancer and it has a comparatively enhanced efficacy and mitigated toxicity.
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PubMed
高影响因子
Materials Today Chemistry
·
2021
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IF 8.301
Y. Hu,M. Li,Z. Gao,L. Wang,J. Zhang
Sulfonated carbon dots (SCDs) were synthesized from plant leaves via continuously hydrothermal treatment by hydrogen peroxide and sulfuric acid, used as catalyst for converting fructose to 5-hydroxymethylfurfural (HMF). Owing to nanosize effect and moderate acidic intensity, SCDs could thoroughly distribute in the solvent with an improved interfacial compatibility and selectively convert fructose to HMF. Under the optimal condition, the yield of HMF was 92.6% along with a fructose conversion of 100%, benefiting from a low activation energy of 52.9 kJ/mol when dimethylsulfoxide was used as solvent. The SCDs catalyst can be recovered, after six recycles, the fructose conversion and HMF yield were remained 66.1% and 56.2% under condition with incompletely conversion of fructose, respectively. This work provides a sustainable route to prepare carbon dots with a superior catalytic performance for converting biomass to important biobased platform chemicals.
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CATALYSIS LETTERS
·
2021
·Vol. 151
·期 8
·2436-2444
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IF 3.186
Hu Yaoping,Li Mingfu,Gao Zhijin,Wang Lei,Zhang Jian
Abstract Waste Polyethylene terephthalate plastic bottles were used as precursors to fabricate carbon dots (CDs) via air oxidation and sulfuric acid hydrothermal treatment. Owing to the nano-size effect and abundant acidic groups, CDs allowed their application as a novel solid acid for quasi-homogeneous catalytic dehydration of fructose to 5-hydroxymethylfurfural (HMF). Under the optimal condition, an ultra-high yield of HMF was 97.4% along with 100% fructose conversion at low temperature of 50 °C when [BMIM]Cl/ethanol was used as solvent. The CDs catalyst also displayed a prominent recyclability and was used for six recycles without massive loss in catalytic activity. Furthermore, 98.6% of HMF could be obtained from final products. The findings provide a novel sustainable route using recyclable plastics to synthesize carbon dots with a superior catalytic performance for conversion of biomass to important bio-based platform chemicals. Graphic Abstract
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POLYMER INTERNATIONAL
·
2020
·Vol. 70
·期 5
·612-618
·
IF 2.574
Yi Xu,Nan Yang,Yujia Liu,Zhengbai Li,Qiang He,Chao Li
5-Aminoindole is designed for aldehyde-functional benzoxazine (PHB-a) copolymerization due to the special reaction between the indole and aldehyde groups, and the copolymerization with benzoxazine monomers. The curing and mechanical behavior and thermal properties of the cured resins are investigated using Fourier transform infrared spectroscopy, 1 H NMR spectroscopy, differential scanning calorimetry, scanning electron microscopy, dynamic mechanical analysis, tensile tests and thermogravimetric analysis. The resulting networks show better processability and mechanical properties without obvious degradation in thermal performance. The low curing temperature (70 °C) of PHB-a is achieved after incorporation of 5-aminoindole. An elongation rate of 2.54% and a forcing break of around 72.3 MPa are achieved, while neat poly(PHB-a) is brittle and failed in the grips. Furthermore, its glass transition temperature is maintained up to 234 °C. These findings open a new way to realize low-temperature curing and to improve the mechanical properties of brittle polybenzoxazine resins under the premise of maintaining good thermal stability. © 2020 Society of Industrial Chemistry
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BIOCHEMICAL AND BIOPHYSICAL RESEARCH COMMUNICATIONS
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2020
·
IF 2.985
Yafei Wang,Huimin Liu,Jianmin Wu,Yunjian Liao,Daifeng Lu,Feng Dong,Hongxi Li,Zhitao Zhang,Yongyun Lian
Periprosthetic osteolysis (PIO) caused by wear particles is the main cause of implant failure, which is regulated by nuclear factor κ B receptor activator ligand (RANKL)/osteoprotegerin (OPG) system. At present, there is a lack of effective drugs to prevent or treat PIO. Previous studies have confirmed that DNA methylation is closely related to postmenopausal osteoporosis and can affect the expression of OPG and RANKL . However, the relationship between DNA methylation and PIO is not clear. In this study, we investigated the inhibitory effect of 5-Aza-2-deoxycytidine (AzadC) on osteolysis induced by titanium particles in a mouse model. This inhibition mechanism is achieved by changing the ratio of RANKL/OPG in the osteolysis model. In conclusion, there is a relationship between DNA methylation and PIO. AzadC has a certain inhibitory effect on osteolysis induced by titanium particles. Regulating DNA methylation may be a new way to treat PIO. Our findings lay a foundation for epigenetic understanding and intervention of osteolysis.
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PubMed
高影响因子
Catalysts
·
2020
·Vol. 10
·期 3
·311
·
IF 3.52
Jing Shao,Shuyuan Cheng,Zhaoxu Li,Bichun Huang
A ZSM-5 zeolite with a hierarchical pore structure was synthesized by the desilication-recrystallization method using tetraethyl ammonium hydroxide (TEAOH) and cetyltrimethylammonium bromide (CTAB) as the desilication and structure-directing agents, respectively. The MnOx/ZSM-5 catalyst was synthesized by the ethanol dispersion method and applied for the low-temperature selective catalytic reduction of NOxwith NH3. The results showed that NOxconversion of the hierarchical MnOx/ZSM-5 catalyst could reach 100% at about 120 °C and could be maintained in the temperature range of 120–240 °C with N2selectivity over 90%. Furthermore, the hierarchical MnOx/ZSM-5catalyst presented better SO2resistance performance than the traditional catalyst in the presence of 100 ppm SO2at 120 °C. XRD, SEM, TEM, XPS, BET, NH3-TPD, and TG were applied to characterize the structural properties of the MnOx/ZSM-5 catalysts. These results showed that the MnOx/ZSM-5 catalyst had micropores (0.78 nm) and mesopores (3.2 nm) leading to a larger specific surface area, which improved the mass transfer of reactants and products while reducing the formation of sulfates. The better catalytic performance over hierarchical MnOx/ZSM-5 catalyst could be attributed to the higher concentration of Mn4+and chemisorbed oxygen species and higher surface acidity. The improved SO2resistance was related to the catalyst’s hierarchical pore structure.Keywords:hierarchical pore structure;MnOx/ZSM-5;NH3-SCR;SO2resistance
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Ji Guo,Zhongli Ji
The filtration efficiency of coalescent filter elements used in gasoline and diesel oil dehydration in refineries is unsatisfactory and not sufficient to meet downstream water-content requirements. Thus, it was necessary to improve the internal filter medium of traditional oil-water coalescent filter elements. Zeolite membrane is a kind of material with superhydrophilicity and strong adsorption for and permeability to water. In this study, ZSM-5 zeolite membrane with superhydrophilic properties was successfully prepared by an in situ hydrothermal synthesis. Two experiments with zeolite membranes were performed, including membrane filtration and membrane coalescence tests. Membrane filtration tests showed that it possessed strong adsorption for and permeability to water and that the oil-water filtration efficiency for 32 # turbine oil, kerosene, and corn oil were all >95 %. In the second part of this study, composite filtration was carried out using the membrane as well as hydrophilic glass fiber and hydrophobic polypropylene (PP) membranes. Membrane coalescence test demonstrated that, when the oil contained a phenol/water combination, the water rejection rate of the composite filtration with ABACBA (A, PP fiber; B, glass fiber; and C, molecular sieve membrane) was 90.8 %, with the downstream water content controlled within 100 mg/L and the quality factor increased from 0.18 to 0.23, relative to other systems. These experimental results showed potential for improving the current oil-water coalescent filters.
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