RENEWABLE ENERGY
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2023
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IF 8.7
Shanshuai Chen,Puxiang Yan,Xiaona Yu,Wanbin Zhu,Hongliang Wang
The development of a highly active and robust catalyst for the conversion of lignin, the largest volume of renewable aromatic resource in nature, to value-added aromatics is of great importance in sustainable chemistry. However, the condensation of lignin depolymerization intermediates into recalcitrant macromolecules restricts high yields of desired products, and this remains a great challenge in lignin valorization. Here, a serious of bifunctional Ru–ZnO/SBA-15 catalysts were synthesized for lignin conversion to aromatics. Roles of Ru and ZnO in these catalysts for lignin conversion were in-depth analyzed. The effect of the ratio of Ru to ZnO was studied. Other reaction conditions including temperature and time were systematically optimized. More than 51.3% yields of aromatics were obtained over Ru–10ZnO/SBA-15 at 240 °C for 4 h. Structure-activity relationship research of the catalyst revealed that the high yield of product could be attributed to the following three reasons: 1) the Lewis acidic sites on Ru/SBA-15 are significantly improved after ZnO modification, and thus promotes the C–O bond cleavage ; 2) the oxophilic ZnO is beneficial to absorb the substrate and reaction intermediates, and therefore enhances the hydrodeoxygenation activity of the adjacent Ru; 3). The interaction between Zn and Ru in Ru–ZnO/SBA-15 changes Ru electronic properties and leads to the formation of highly active catalytic sites with high electron density. These results indicated that the bifunctional Ru–ZnO/SBA-15 catalyst with high catalytic activity could be a good choice for lignin conversion to high-yield aromatics.
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
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2022
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IF 5.062
Fei Wang,Xuyang Li,Xialin Hu,Wenya Zhuang,Jiewei Lai,Wenchao Wang,Xuanrong Sun,Hong Wang,Qingyong Li
FLQY2 is a camptothecin derivative modified by FL118 and proved to be good antitumor activity in vitro . However, its poor solubility leads to the low therapeutic efficacy in vivo . Here, the injectable FLQY2 lyophilized powder was prepared with Kolliphor® HS 15 (HS 15), which was called HS 15-FLQY2. The preparation process of HS 15-FLQY2 was optimized by orthogonal design and the lyophilization process was investigated by single factor experiment. Moreover, the formulation was characterized, the pharmacokinetics study and the antitumor activity were carried out in vivo . As the results, HS 15-FLQY2 (1:1500, w/w) containing 5% mannitol as cryoprotectant showed good appearance and 70% entrapment efficiency. HS 15-FLQY2 revealed low particle size (<16 nm), better homogeneity (PDI <0.2) and remained stable for 24 h in water. In addition, the data of the DSC , XRD and FTIR demonstrated that FLQY2 was distributed within micelles . In vivo , the bioavailability of HS 15-FLQY2 (i.p.) was improved significantly compared with oral CD-FLQY2 (a cyclodextrin inclusion complex of FLQY2). In addition, HS 15-FLQY2 demonstrated higher tumor inhibition effect than capecitabine , confirming the possibility of treatment cancer by the delivery of FLQY2.
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RENEWABLE ENERGY
·
2022
·
IF 8.634
Xiaocui Wei,Yanan Liu,Yang Cao,Jin Li,Xianghao Meng,Zhao Zhang,Zhongyi Jiang
The catalytic pyrolysis of biomass is a sustainable approach for biofuel production, contributing to replacing fossil resources with renewable resources . The ZSM-5 zeolite remains an attractive catalyst in the catalytic pyrolysis of biomass, and how to reduce the product diffusion resistance and regulate the surface acidity of ZSM-5 should be explored more deeply. Herein, a hierarchical gallium-modified ZSM-5@SBA-15 catalyst is fabricated through coating a mesoporous layered SBA-15 shell on a hollow ZSM-5 core with gallium modified on the surface, which is effective for increasing hydrocarbon production during the catalytic pyrolysis of biomass process. The synergistic effect of hollowness, mesoporosity, and activity in the hierarchical gallium-modified ZSM-5@SBA-15 catalysts is found to affect the yield and quality of bio-oil. Accordingly, the hierarchical gallium-modified ZSM-5@SBA-15 catalyst with 11 wt% Ga loading exhibits a superior deoxygenation ability, and the relative content of hydrocarbons in bio-oil reach to 49.76 area% which is much higher than that of ZSM-5 (35.30 area%). Furthermore, a possible catalytic pyrolysis mechanism of biomass was also proposed to clarify the potential application of hierarchical gallium-modified ZSM-5@SBA-15 catalysts.
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MATERIALS CHEMISTRY AND PHYSICS
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2022
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IF 4.778
Xijun Li,Sifan Zhang,Lihua Zhu,Jun Liu,Huan Zhang,Ning Zhao,Bing Hui Chen
Herein, a series of the Pt-based bimetallic catalysts (PtM x /SBA-15) are gained by using ultrasonic incipient wetness impregnation method (M = Co, Cu, Ni or Zn). The experimental results show that the catalytic performance (including catalytic activity (turnover frequency-TOF), selectivity to crotyl alcohol) of PtCo x /SBA-15 for catalyzing crotonaldehyde selective hydrogenation is the best among PtM x /SBA-15. Additionally, the ratio of Pt/Co in the PtCo x /SBA-15 catalysts is changed to successfully synthesize PtCo/SBA-15, PtCo 2 /SBA-15, PtCo 5 /SBA-15. It demonstrates that the selectivity of the PtCo x /SBA-15 catalysts for crotonaldehyde selective hydrogenation to crotyl alcohol is significantly improved with the increase of the Co content. The PtCo 5 /SBA-15 catalyst provides 83.8% conversion of crotonaldehyde, 94.3% selectivity to crotyl alcohol and TOF of 910.5 h −1 under mild reaction conditions (3.0 MPa H 2 , 80 °C and 2.0 h). And PtCo 5 /SBA-15 has much better catalytic performance (higher catalytic activity and selectivity to crotyl alcohol) than PtCu 5 /SBA-15, PtNi 5 /SBA-15 and PtZn 5 /SBA-15. The reasons are as follows: (1) PtCo alloy forms, which is conducive to crotonaldehyde adsorption and activation; (2) there is an appropriate synergy effect between Pt and Co, greatly improving the capacity of the catalyst activating hydrogen under mild conditions; (3) the electron transfers from Co to Pt, resulting in the increase of Pt electron density and decrease of Co electron density, then the Co sites are advantageous to C O group adsorption and activation and Pt sites for H 2 adsorbing and activating; (4) with the increase of the Co proportion in PtCo x /SBA-15, the synergy effect between Pt and Co in PtCo alloy strengthens and thus increases the selectivity of C O group hydrogenation.
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Journal of Oleo Science
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2022
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IF 1.628
Wenyi Chen,Maomao Kou,Lin Li,Bing Li,Jianrong Huang,Shudong Fan,Li Xu,Nanjing Zhong
In this study, SBA-15 was functionalized by organic groups (-CH3, -C4H9, -C8H17, -CH2CH2NH2, -C6H5, et al.), and then Lecitase® Ultra (LU) was immobilized onto the modified SBA-15 for soybean oil degumming. The hydrolysis activity, degumming performance, reusability in degumming, and the composition of phospholipids in the gum, of the immobilized LU samples, were carefully studied. Hydrolysis activities over 1800 U/g were obtained from all the immobilized LU samples. The highest activity of up to 4554.17 U/g was observed from the 3-ureidopropyl group-modified SBA-15-supported LU. Most of the immobilized LU samples removed the phospholipids effectively from crude soybean oil (initial phosphorous content 314.23 mg/kg), with a residual phosphorus content of less than 10 mg/kg. The reusability of the immobilized LU samples in the degumming process was evaluated. No loss of activity was observed from the methyl and N-(2-aminoethyl)-3-aminopropyl group-modified SBA-15-supported LU samples after five cycles of reuse. In addition, 3-aminopropyl and 3-glycidyloxypropyl group-modified SBA-15-supported LU samples retained over 90% of their initial activity; N-phenylaminomethyl and 1-isocyanatopropane group-functionalized SBA-15-supported LU samples retained approximately 80% of their initial activity. The phospholipids in the gum were analyzed. The n-octadecyl and N-(2-aminoethyl)-3-aminopropyl group-functionalized SBA-15-supported LU samples were selective for lysophosphatidylethanolamine (LPE) preparation, and LPE percentages up to 37.14 and 38.80% were obtained, respectively. The N-phenylaminomethyl group-modified SBA-15-supported LU showed selectivity toward lysophosphatidylcholine (LPC) production, with an LPC percentage of up to 38.5%.
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JOURNAL OF POROUS MATERIALS
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2022
·Vol. 29
·期 5
·1399-1410
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IF 2.523
Zhang Xin,Chen Fei,Li Yuejin,Duan Yongzheng,Liu Guoxia
In this study, lanthanum-modified the shell–core magnetic nanocomposites with Fe 3 O 4 core and homogeneous mesoporous silica shell (La-SBA-15@Fe 3 O 4 -x) were prepared. The preparation, morphology, composition and magnetic properties of La-SBA-15@Fe 3 O 4 were investigated by TEM, SEM, XRD, VSM and BET. The results suggested that the SBA-15 have successfully encapsulated Fe 3 O 4 and the magnetic particles were decorated by lanthanum. The adsorption experiments were carried out to explore effect of La-SBA-15@Fe 3 O 4 on removal of phosphorus from aqueous solution. The kinetic study of adsorption process was investigated to describe the relationship between adsorption rate and adsorption equilibrium and the Langmuir and Freundlich isotherm models were employed to illustrate adsorption isotherm.
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Advanced Healthcare Materials
·
2023
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IF 10
Dongyan Shao,Ting Bai,Bobo Zhu,Xiaojia Guo,Kai Dong,Junling Shi,Qingsheng Huang,Jie Kong
Natural killer (NK) cells have emerged as an important contributor to cancer immunotherapy, but their antitumor efficacy remains suboptimal. While cytokine-based priming shows promise in enhancing NK-cell activity, its clinical translation faces many challenges, including co-activation of multiple cytokines, poor pharmacokinetics, and limited mechanistic understanding. Here, we developed a polymeric micelle-based IL-15/IL-2 codelivery system (IL-15/2-PEG-PTMC) for NK-cell activation. In vivo studies demonstrated that the half-life of IL-15 and IL-2 as well as the recruitment of NK cell within tumor tissue was significantly increased after PEG-PTMC loading. Coupled with the coactivation effect of IL-15 and IL-2 conferred by this polymeric micelle-based system, it noticeably delayed the growth of tumors in mice compared to conventional NK cell activation approach, that was free IL-15 and IL-2. We also surprisingly found that cholesterol metabolism was highly involved in the NK cell activation by IL-15/2-PEG-PTMC. Following stimulation with IL-15/2-PEG-PTMC or IL-15, NK cells underwent a series of cholesterol metabolism reprogramming, which elevated the cholesterol levels on the NK cell membrane. This in turn promoted the formation of lipid rafts and actived immune synapse, effectively contributing to the enhancement of the NK cell's anti-tumor activity. We believe this will open a new avenue for improving the efficacy of NK cell immunotherapy by regulating cholesterol metabolism. This article is protected by copyright. All rights reserved
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COMPOSITES PART B-ENGINEERING
·
2020
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IF 7.635
Beibei Ma,Rijia Lin,Hui He,Qinghua Wu,Shuixia Chen
Hydrothermal is common process for synthesizing well-ordered mesoporous silica, however, it costs time and energy simultaneously. To improve the efficiency of synthesis process, it is necessary to propose a facile synthesis strategy with less time and energy requirement. In this study, an innovative non-hydrothermal method using NH 3 ∙H 2 O as catalyst after ripening step is developed to prepare SBA-15 with short mesochannels (SSBA-15) for the first time. The synthesis period of SSBA-15 framework was extremely shortened within 40 min under the optimized conditions (30 min of ripening step and 25% of NH 3 ∙H 2 O concentration), while obtained material exhibits well-ordered hexagonal pore structure and fine particle morphology of SSBA-15 (pore length of 250 ± 50 nm and mesopore size of 9.8 nm). This method can also be employed to synthesize conventional SBA-15 successfully. Moreover, the application of SSBA-15 as support of solid amine adsorbents on CO 2 adsorption and well-fitting of experimental CO 2 adsorption data with Avrami and intraparticle diffusion models reveal that the adsorbents combine the advantages of micro-mesoporous structure, short mesochannel and amine reagents (high affinity of CO 2 ), resulting in enhanced molecular diffusion, fast adsorption kinetics and high CO 2 adsorption capacity . Notably, the solid amine adsorbents exhibited excellent regeneration ability during ten adsorption-desorption cycles. This work opens up new opportunities in efficient preparation of materials that require hydrothermal process.
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RSC Advances
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2020
·Vol. 10
·期 6
·3175-3183
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IF 3.119
Weiwen Chen,Zhikai Xie,Hui Liang,Xinhua Zhou,Wenbin Hu,Xugang Shu
In this paper, we report the successful preparation of a novel bifunctional heterogeneous catalyst Ptδ+/SBA-APTE-SA with a partial positively charged Ptδ+ electronic structure via post-synthesis modification of (3-aminopropyl)triethoxysilane (APTE), succinic anhydride (SA) and platinum precursors. The resulting catalyst showed superior catalytic performance for the hydrosilylation of 1,1,1,3,5,5,5-heptamethyltrisiloxane (MDHM) with allyloxy polyethylene glycol (APEG) compared to a heterogeneous platinum catalyst. In addition, our catalyst was suitable for the hydrosilylation of other alkenes. Furthermore, the catalyst displayed sufficient stability after being reused five times without noticeable inactivation. In terms of cycle number and atomic utilization efficiency, it has potential applications as a green hydrosilylation method for industry.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2021
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IF 3.171
Jinglei Cui,Qian Wang,Jianming Gao,Yanxia Guo,Fangqin Cheng
Rare earth elements (REE) are strategic resources and the recycling of REE in alternative resources is urgent and gets increasingly attention. However, the separation of REE in these alternative resources is still a challenge due to the low concentration of REE and multi coexisted ions in acidic system. In this study, the species distribution of REE within the pH 0–8.0 was calculated. The SBA-15 originated from coal fly ash was modified by two steps with (3-aminopropyl) triethoxysilane (APTES) and diethylenetriaminepentaacetic dianhydride (DTPADA) to obtain DTPADA-SBA-15 adsorbent, which was applied to the selective adsorption of REE. The results showed that DTPADA-SBA-15 possessed excellent adsorption performance on the selective adsorption of REE, including Eu, Gd, Tb, Nd and Sm, in acidic solution (pH 2) with multi competing ions. The FT-IR and Zeta potential characterization verified that the chemical adsorption through the coordination of O in DTPADA-SBA-15 with REE was dominant at lower pH value. The study of adsorption kinetics indicated that the adsorption of rare earth metal ions followed pseudo-second-order kinetic, of which the adsorption process followed the Langmuir isotherm model.
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CATALYSIS LETTERS
·
2021
·Vol. 152
·期 5
·1495-1505
·
IF 3.186
Zhang Yue,Wang Li,Ma Qingqing,Wang Nan,Pan Zhiyong
SBA-15 was modified via post-treatment with (NH 4 ) 2 SiF 6 and (NH 4 ) 3 AlF 6 solution (NSF-T and NAF-T) and applied as support of Pd catalysts for the hydrogenation of 2-ethyl-anthraquinone (EAQ). The characterization results revealed that F could be incorporated into the framework of SBA-15 by forming Si–F bond and the amount of F increased as the molar ratio of F in treating solution to Si species in SBA-15 (F/Si) increased from 0.1 to 0.4 for NSF-T and 0.3 to 0.6 for NAF-T. At the same F/Si, the incorporated amount of F was larger with NSF-T than with NAF-T, and the latter could simultaneously create acid sites in catalysts. The hydrophobicity of catalysts could be effectively improved by incorporating F into SBA-15 supports, which favored the catalytic performance. The catalyst on SBA-15 treated by NSF with F/Si of 0.3 exhibited the high initial activity (0.24 molH 2 ·gPd −1 ·min −1 ) and selectivity (95.5%). Graphic Abstract
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PLANTA
·
2021
·Vol. 254
·期 5
·1-10
·
IF 4.116
Wang Jiadian,Su Ping,Gao Linhui,Zhang Yifeng,Wang Jian,Tu Lichan,Zhao Yujun,Lu Yun,Yin Yan,Huang Luqi,Gao Wei
Main conclusion A novel cytochrome P450 from Tripterygium wilfordii , CYP81AM1, specifically catalyses the C-15 hydroxylation of dehydroabietic acid. This is the first CYP450 to be found in plants with this function. Abstract Cytochrome P450 oxygenases (CYPs) play an important role in the post-modification in biosynthesis of plant bioactive terpenoids. Here, we found that CYP81AM1 can catalyze the formation of 15-hydroxydehydroabietic acid by in vitro enzymatic reactions and in vivo yeast feeding assays. This is the first study to show that CYP81 family enzymes are involved in the hydroxylation of abietane diterpenoids. At the same time, we found that CYP81AM1 could not catalyse abietatriene and dehydroabietinol, suggesting that the occurrence of the reaction may be related to the carboxyl group. Through molecular docking and site mutations, it was found that some amino acid sites (F104, K107) near the carboxyl group had an important effect on enzyme activity, also suggesting that the carboxyl group played an important role in the occurrence of the reaction.
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