KEY ENGINEERING MATERIALS
·
2013
·
IF 0
Yun Xia Jiang,Hu Jin Zuo,Yong Jia Shen,Feng Ping Yi
The Friedel-Crafts acylation reaction between 5-cyanoindole and 4-chlorobutyryl chloride was conducted in ionic liquid 1-buty-3-methylimidazolium chloroaluminate ([bmiCl/AlCl3), the major product was 5-cyano-3-(4-chlorobuty) indole. The structure of the product was characterized by Mass and 1H NMR spectra. When the molar ratio of AlCl3 to [bmiCl in [bmiCl/AlCl3 is at 1:1 or less, no 5-cyano-3-(4-chlorobuty) indole could be obtained. The suitable molar ratios of AlCl3 to [bmiCl in [bmiCl/AlCl3 were from 2:1 to 3:1, the yields of the major product were from 68% to 70%, respectively. When the molar ratio of [bmiCl/AlCl3 to 5-cyanoindole was less than 2:1, the acylation reaction was difficult to carry out, because 5-cyanoindole would be not totally dissolve in [bmiCl/AlCl3 under the situation.
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DOI
FUEL
·
2022
·
IF 8.035
Shijie Wang,Yihang Chen,Yu Jia,Chen Wang,Guizhuan Xu,Youzhou Jiao,Chao He,Chun Chang,Qianhui Guo
An effective catalytic strategy for the conversion of glucose to 5-ethoxymethylfurfural (EMF) catalyzed by ultrastable Y zeolite (USY) in a co-solvent system was developed. Effects of co-solvent and reaction conditions were first investigated. Tetrahydrofuran (THF) with low dipolarity/polarizability (π*) was screened as the appropriate co-solvent, and a higher EMF yield of 41.46% was obtained as the ratio of ethanol to THF was 7:3. The macroscopic reaction kinetic study indicated that THF can protect EMF from easy degradation to EL. Moreover, the reusability and the characterization of USY verified the feasibility of USY as an efficient solid acid catalyst. In this study, density functional theory (DFT) calculations for the catalytic mechanism and solvent effect at the molecular scale were performed for the first time. The extra-framework aluminum species (EFAL), in which Al 3+ played an essential role in the reaction as the preferred EFAL species, and THF can reduce the energy barrier of USY-catalyzed glucose isomerization . Meanwhile, the inhibitory effect of THF on EMF alcoholysis was explored via the frontier molecular orbital theory. The results showed that THF increased the LUMO energy of EMF compared with ethanol and γ-valerolactone, which decreased its susceptibility to nucleophilic attack and reduced the adverse alcoholysis of EMF and humins formation. This study provided an enlightening reference for the efficient synthesis of EMF from carbohydrates catalyzed by solid acid catalyst under solvent effect.
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DOI
高影响因子
NANO
·
2021
·
IF 1.556
Wenlong Li,Weiwei Zhang,Weihao Jin,Longbao Zhu,Wanzhen Li,Ping Song,Yugui Tao,Fei Ge
Design of high-performance drug delivery system is necessary to improve the anticancer ability of 5-fluorouracil (5-FU). In this work, we developed a pH-responsive 5-FU loaded and sodium alginate (SA) modified mesoporous silica nanoparticles (MSNs) drug delivery system (5-FU@MSN-SA). After 5-FU was loaded into the pores, MSNs were successfully functionalized with amino groups and then capped by sodium alginate. Compared to acidic conditions, the drug release rate in the neutral environment was quite low. Moreover, detailed investigations confirmed that 5-FU@MSN-SA can easily be up-taken by cancer cells and proved the high cytotoxicity to 4T1 cells. The calculated IC 5 0 values for 5-FU and 5-FU@MSN-SA were 34.67 μ g/mL and 54.95 μ g/mL, respectively. These results indicated that 5-FU@MSNs-SA can be a promising nanoplatform in cancer therapy.
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DOI
高影响因子
Chemical Engineering Journal Advances
·
2022
·
IF 0
Hengye Li,Xingwei Han,Wenjie Yu,Lin Zhang,Meijie Wei,Zhongxia Wang,Fenying Kong,Wei Wang
Porous organic polymers containing macrocycles are promising adsorbents to remove organic micropollutants from water. However, it is still a big challenge to achieve the balance between economy and performance in real-world application. This study aimed at tackling this challenge by verifying the feasibility of dimethoxypillar[5]arene (P[5]) as a universal knitting crosslinker. Herein, four typical aromatic building blocks were selected and the corresponding P[5] knitted porous polymers with high cost-effectiveness were successfully obtained by a simple Friedel-Crafts reaction with all the yields in excess of 100%. We have demonstrated the significant roles of P[5] content and surface area on the adsorption kinetics and adsorption capacity, respectively. Specially, P[5] knitted 1,3,5-triphenylbenzene (P[5]-TPB) showed the superior adsorption performance among them. The thermodynamic studies certified the spontaneous and exothermic nature, while the mechanism studies revealed that hose-guest and hydrophobic interactions played fundamental roles in the adsorption process. The studies of flow-through adsorption and adsorption at environmentally relevant concentrations further displayed the superior adsorption performance of P[5]-TPB for practical application. The high cost-effectiveness combined with the excellent adsorption properties of P[5]-TPB achieved the balance between economy and performance, demonstrating great potential as promising adsorbent for real-world application. This work paves a way for the synthesis of cost-effective advanced porous polymers with host-guest property for versatile applications.
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DOI
CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Tingting Qi,Linyu Zhou,Yingjiao Li,Guang-Wen Chu,Yong Luo,Jie Shi,Haikui Zou,Bao-Chang Sun
Oxygen vacancy (OV) plays a significant role in the catalytic performance of oxidation catalysts. Herein, ZSM-5@MnO x catalyst with abundant OVs was firstly prepared by in-situ growth method. The prepared catalyst exhibits good catalytic activity for the selective oxidation of benzyl alcohol (BA) to benzaldehyde (BAD) with ~100% BA conversion and ~100% BAD selectivity within 3 h. We have proved that the OV in ZSM-5@MnO x catalyst is the main active site for the BA oxidation. Besides, the OV formation mechanism is proposed based on the influences of modified ZSM-5 supports on OVs. Results show that sodium ions in ZSM-5 are conducive to enhancing the coating of MnO x on supports, and protons in ZSM-5 are beneficial for the formation of OVs by dehydrating with hydroxyls on MnO x . Based on the mechanism, we further enrich OVs by the deep dehydration to improve its catalytic performance. This work provides a novel route for the design of OVs in the ZSM-5@MnO x catalyst.
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DOI
高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 6
·e18054
·
IF 3.7
Feng Xiong,Chen Ji,Shengzhi Gan,Peng Liang,Yi Huang,Jin Shang,Baoyu Liu,Jinxiang Dong
Mesoscopically structured ZSM-5 nanosheets were prepared as highly active catalysts for the alkylation between toluene with methanol. The results showed that the Brønsted acid sites of ZSM-5 nanosheets were mainly distributed on the external surface in aluminum-rich zeolites owing to the charge-balance between positive quaternary ammonium cation (N + ) in C ph-10-6-6 , Na + ions and negative aluminosilicate species. In addition, it revealed that high alkalinity was easier to depolymerize the Si O Si species in Aluminum-rich synthesis gel, and the high alkalinity was required for silica-rich systems to dissolve silica species in order to finish the self-assemble process, leading to ZSM-5 nanosheets with high alkalinity presenting enhanced catalytic performance. Moreover, the optimized ZSM-5-50-2.5 was effective for the alkylation between toluene and methanol with toluene conversion of up to 50%, and it was stably operated for 48 h under the harsh conditions of WHSV = 32.5 h −1 with a desired stability.
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DOI
高影响因子
DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 21
·7456-7463
·
IF 4.39
Zhen-Li Yang,Yue-Mei Wu,Piao He,Wen-li Cao,Saira Manzoor,Jian-Guo Zhang
The development of green energetic materials is based on environmental friendliness, safety and performance improvement. It is of great significance to design and synthesize new nitrogen rich salts for a new generation of green energetic materials. In the present work, a series of 3-amino-5-hydrazinopyrazole energetic salts comprising energetic anions were synthesized and were characterized using elemental analysis, IR spectroscopy and differential scanning calorimetry (DSC). Compounds 1–5 were further confirmed by single crystal X-ray diffraction and the sensitivities were measured by the standard BAM methods. Additionally, the structure–property relationship was elucidated from the experimental results and theoretical calculations. Energetic salts of 2 and 5 exhibited high heat of formation (5, 1160.06 kJ mol−1), high decomposition temperature (2, 172 °C; 5, 186 °C), excellent detonation performance (2, Dv, 9076 m s−1, P 34.1 GPa; 5, Dv, 8974 m s−1, P 31.9 GPa), moderate sensitivity towards outer stimuli and high nitrogen contents (2, 41.03%; 5, 63.84%). This work increases future prospects for the design of insensitive and novel high-energy green energetic material.
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DOI
高影响因子
Science China-Chemistry
·
2024
·Vol. 67
·期 4
·1242-1249
·
IF 10.4
Zhang Jingjing,Deng Yongyan,Gai Dongxu,Shi Yang,Feng Xingwen,Li Peilong,An Yongtao,Zou Xiaoqin
Isotopic separation is of paramount importance for producing high-purity heavy hydrogen, yet the process remains hugely challenging. Here, we report on an Fe/ZSM-5 zeolite that was able to efficiently separate deuterium from protium via chemical quantum sieving. Structural data showed that four types of Fe species were present in Fe/ZSM-5 and oligomeric Fe–O clusters in the zeolite pores were correlated directly with gas selectivity. Gas adsorption revealed that Fe–O species served as the main adsorption sites and interacted with D 2 more strongly than with H 2 . D 2 /H 2 separation was exemplified using thermal desorption spectroscopy. D 2 /H 2 selectivity increased with Fe loading in Fe/ZSM-5 and a selectivity of 32.1 was obtained with an optimal loading of 7 wt%. The shift of desorption temperature supports the chemical affinity-based quantum sieving of D 2 over H 2 . This study demonstrates an effective strategy for enhancing D 2 /H 2 separation and the high selectivity means that Fe/ZSM-5 has strong potential in hydrogen isotope separation.
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Junpu An,Hongchen Liu,Fan Yang,Kexin Wei,Chunhui Yu,Siyuan Sun,Yang Sun,Qing Guo,Jianfeng Wang,Chenlin Wang,Jiahui Liu,Kuobo Wang,Yongfeng Li
Nickel-based catalysts show great potential as promising candidates for the electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF). However, the limited adsorption capacity of nickel-based catalysts for OH – and HMF limits their further development. In this study, amorphous Fe/NiOOH-SO x was generated from nanosheets (Fe/NiOOH-Ni 3 S 2 ), which was pre-fabricated on nickel foam via pre-reconstruction and anionic regulation strategy. The optimized catalyst Fe/NiOOH-Ni 3 S 2 demonstrated exceptional activity in the HMF oxidation reaction (HMFOR) with a current density of 10 mA cm −2 at 1.32 V vs RHE, accompanying with the 98.9 % HMF conversion, 97.8 % 2,5-Furandicarboxylic acid (FDCA) selectivity, 96.8 % Faraday efficiency, and stability for ten cycles. The incorporating amorphous FeOOH reduces the electron density around Ni, promoting the formation of high-valent Ni spices. Meanwhile, the SO x combined with amorphous hydroxy nickel oxide provides unsaturated sites, which enhances the adsorption capacity of HMF. Density functional theory (DFT) computations reveal that the designed amorphous Fe/NiOOH and surface-adsorbed SO x collectively modulate the electronic structure of the catalyst, causing an upwards shift of the NiOOH d-band center and enhancing adsorption capacities for both HMF and OH – . This study proposes the adsorption enhancement mechanism of regulating electronic structure and offers a rational strategy for HMFOR electrocatalysts.
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2024
·
IF 5.7
Jing Wang,Xin Xu,Wanqing Wei,Wei Song,Jian Wen,Guipeng Hu,Xiaomin Li,Cong Gao,Xiulai Chen,Liming Liu,Jing Wu
Pyridoxal 5′-phosphate (PLP) is highly valuable in food and medicine. However, achieving the efficient biosynthesis of PLP remains challenging. Here, a salvage pathway using acid phosphatase from Salmonella typhi (StAPase) and pyridoxine oxidase from Escherichia coli (EcPNPO) as pathway enzymes was established for the first time to synthesize PLP from pyridoxine (PN) and pyrophosphate (PPi). StAPase was identified as a rate-limiting enzyme. Two protein modification strategies were developed based on the PN phosphorylation mechanism: (1) improving the binding of PN into StAPase and (2) enhancing the hydrophobicity of StAPase’s substrate binding pocket. The kcat/Km of optimal mutant M7 was 4.9 times higher than that of the wild type. The detailed mechanism of performance improvement was analyzed. Under the catalysis of M7 and EcPNPO, a PLP high-yielding strain of 14.5 ± 0.55 g/L was engineered with a productivity of 1.0 ± 0.02 g/(L h) (the highest to date). The study suggests a promising method for industrial-scale PLP production.
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DOI
PubMed
高影响因子
CHEMBIOCHEM
·
2018
·Vol. 19
·期 7
·654-659
·
IF 2.774
Ke-Feng Wang,Chun-lei Liu,Kun-yan Sui,Chen Guo,Chun-Zhao Liu
Graphical Cleaning up catalysis : There is a great need for the eco-efficient and sustainable oxidation of bio-based chemicals by using clean catalysts. In this study, magnetic laccase catalyst with TEMPO as the mediator showed high activity in the oxidation of 5-hydroxymethylfurfural (HMF). Interesting and promising results were obtained, with 90.2 % yield of 2,5-furandicarboxylic acid (FDCA) and complete HMF conversion. 2,5-Furandicarboxylic acid (FDCA) is a bio-based platform chemical for the production of polyethylene furanoate (PEF) and other valuable furanic chemicals. A magnetic laccase catalyst with (2,2,6,6-tetramethyl-piperidin-1-yl)oxyl (TEMPO) as the mediator has the remarkable capability of oxidizing 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA). Under optimal reaction conditions, a quantitative yield (90.2 %) of FDCA with complete HMF conversion was obtained after 96 h of reaction. More importantly, the magnetic laccase catalyst exhibited good recyclability and stability, maintaining 84.8 % of its original activity following six reuse cycles. This is the first report on the efficient catalytic oxidation of HMF to FDCA by using an immobilized enzyme catalyst.
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产品关联
DOI
PubMed
高影响因子
ChemCatChem
·
2025
·
IF 3.9
Xinyu Xiao,WEIWEI ZHAO,Mingyue Li,Guangmeng Chen,Wenjie Yu,Weihua Zhou,Xiaoqing Liu
The electrooxidation of 5-hydroxymethylfurfural (HMF) has emerged as a promising way to generate high-value-added bio-based products. However, improving catalyst selectivity for HMF and inhibiting competitive oxygen evolution reaction (OER) in a limited potential range remain long-term targets. In this work, the self-supported LIG-NiCuP electrode, utilizing porous laser-induced graphene (LIG) skeleton as the substrate and loaded with NiCuP compound, is designed for the efficient and highly selective electrooxidation of HMF to 2,5-furandicarboxylic acid (FDCA). The surface reconstruction of electrode forms a LIG-NiCuP/NiCu(OH)x heterostructure, demonstrating high activity (HMF conversion 99.7%, FDCA yield 92.6%) for HMF oxidation reaction (HMFOR). Studies indicate that the low activity of Cu for OER allows it to function as a co-catalyst, enhancing the selectivity of Ni-based primary catalyst for HMF. In addition, the pine needle-like structure of Cu can optimize the morphology of catalyst deposited on LIG skeleton, increasing the contact area with HMF. On the other hand, in terms of the substrate to support metal catalysts, LIG fabrication combines the characteristics of rapidity, simplicity, scalability, and low cost, therefore, holding high promise in practical applications. Overall, the material system and processing method in this work present a significant step toward developing efficient catalyst electrodes for biomass conversion.
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产品关联
DOI
高影响因子
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