CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
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IF 3.171
Xing Zhang,Jingfeng Wu,Junhao Chen,Liang Lu,Lingjun Zhu,Shurong Wang
The catalytic cracking of bio-oil is important to produce aromatic hydrocarbons , which can partially replace gasoline or diesel to greatly reduce carbon emissions from transportation. To further promote the formation of aromatic hydrocarbons, this work studied the effects of the preparation method and the acid strength of Ga 2 O 3 /HZSM-5 on catalytic cracking of the bio-oil distilled fraction systematically. The preparation method of Ga 2 O 3 /HZSM-5 had an important effect on its catalytic activity: the Ga 2 O 3 /HZSM-5 prepared by physical mixing showed the low dispersion of active phases and poor pore structure, resulting in its insufficient activity and severe coke deposition; the Ga 2 O 3 /HZSM-5 prepared by precipitation exhibited the higher activity, while many polycyclic aromatic hydrocarbons unfavorable for the subsequent utilization were in the oil phase; the Ga 2 O 3 /HZSM-5 prepared by impregnation showed the highest activity and 35.5% (mass) selectivity of the oil phase, including 80.3% monocyclic aromatic hydrocarbons and 12.0% polycyclic aromatic hydrocarbons. The Brønsted acidity of Ga 2 O 3 /HZSM-5 decreased with Si/Al ratio, leading to the decline in reactant conversion, oil phase selectivity and quality. Meanwhile, the polymerization between monocyclic aromatic hydrocarbons and oxygenates was promoted to produce many polycyclic aromatic hydrocarbons and even coke, causing catalyst deactivation .
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2021
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IF 5.541
Jianjun Xiao,Minjiao Yang,Qingfeng Che,Yingquan Chen,Xu Chen,Haiping Yang,Pietro Bartocci,Francesco Fantozzi,Hanping Chen
The effect of potassium in biomass on the catalytic activity of ZSM-5 zeolite in the fast pyrolysis of biomass was investigated using 2-methylfuran (2-MF) as the typical model compound. The mechanism of action of potassium was explored in detail, along with the physicochemical properties of ZSM-5, including crystallinity, pore structure, and surface acidity. The physicochemical properties of ZSM-5 deteriorated to varying degrees after being tainted with different potassium sources (KOH, K 2 CO 3 , KAc, and KCl). Compared with neutral KCl and strong alkali KOH, K 2 CO 3 , and KAc, with weaker alkalinity but larger crystal structure, exerted a larger influence on ZSM-5. Changes in ZSM-5 tainted with K 2 CO 3 were the greatest, and crystallinity, surface area, acidity, and the corresponding yields of valuable aromatic hydrocarbons and gas products, all declined significantly, compared with raw ZSM-5. When the amount of K(CO 3 2− ) on ZSM-5 was less than 0.5 wt%, only minor (<10 %) changes were observed in crystallinity and surface area, but total acidity decreased by over 30 percent. The conversion of 2-MF was increased using ZSM-5 tainted with less than 0.5 wt% K(CO 3 2- ) and less liquid oxygenated compounds and more CO 2 were produced. Appropriate total acidity, adjusted by a tiny amount of K 2 CO 3 , could promote deoxygenation to CO 2. However, the decarbonylation reaction was inhibited, causing a negative effect on monocyclic aromatic hydrocarbons, which was attributed to the large-scale loss of both acidity and physical structure of ZSM-5 caused by more than 1.0 wt% K(CO 3 2- ).
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ACS Catalysis
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2020
·
IF 12.35
Mo Zhang,Zheng Li,Xing Xin,Junhao Zhang,Yeqin Feng,Hongjin Lv
Selective production of value-added platform chemicals from renewable biomass feedstocks and their derivatives has attracted tremendous attention with high potential in addressing global problems of energy and sustainability. In this work, a lead-halide perovskite (MAPbBr3, MA = methylammonium) is utilized as a photocatalyst for selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) using atmospheric O2 upon visible-light irradiation. Under minimally optimized conditions, the photocatalytic conversion of HMF in acetonitrile solvent reaches 100% with a DFF selectivity of over 90%, achieving an overall furanic carbon yield of over 96%. A detailed catalytic mechanism was proposed based on various spectroscopic and experimental results, revealing that the atmospheric O2, photogenerated electrons (e–), holes (h+), •O2–, and 1O2 species together play crucial roles in the effective and selective photo-oxidation of HMF to DFF. In addition, our present photocatalytic system is also applicable for photo-oxidation of benzyl alcohol with approximately 100% conversion and benzaldehyde selectivity, providing insights for future exploration of the present catalytic system.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Yanying Hao,Anping Tian,Jin Zhu,Jinshi Fan,Yong Yang
5-Hydroxymethyl-2-furancarboxylic acid (HFCA), a promising biomonomer from renewable resources, was used to synthesize two bio-based plasticizers, namely, hexyl 5-((hexanoyloxy)methyl)-2-furancarboxylate (HHMFC) and dihexyl 5,5′-(oxybis(methylene))bis(furan-2-carboxylate) (DHOBFC). The chemical structures of these prepared plasticizers were confirmed using Fourier transform infrared and nuclear magnetic resonance, and then, their plasticization effects on poly(vinyl chloride) (PVC) were also studied. As a result, HFCA-based plasticizers were miscible with PVC and exhibited excellent plasticization performances, compared with commercial dioctyl phthalate. It was noted that HHMFC had a much better plasticizing effect on the PVC film than DHOBFC; however, it displayed a poorer volatility resistance and exudation resistance, which could be attributed to its smaller molecular weight. Besides, because each rigid furan ring of the synthesized plasticizers contained one oxygen atom, the polarity of HFCA-based plasticizers was improved, which inhibited them from migrating from the PVC matrix into nonpolar solvents. Therefore, the HFCA-based plasticizers have good potential as primary plasticizers for PVC.
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MICROCHEMICAL JOURNAL
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2020
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IF 3.594
Yuanyuan Xia,Yuan Wang,Meng Zhang,Faqiong Zhao,Baizhao Zeng
In this work, a novel composite of Au nanoparticles (Au NPs), ionic liquid (i.e. 1-aminopropyl-3-methylimidazolium bromine, [APMIM]Br) and multi-walled carbon nanotubes ( [email protected] ) is prepared through ion-exchange and Au-N coordination between MWCNTs , IL, and Au NPs under mild conditions. The composite is used as support, itaconic acid (IA) and acrylamide (Aam) as functional monomers, 5-hydroxytryptamine (5-HT) as template molecule, ethylene glycol dimethylacrylate (EGDMA) as cross-linking agent and azobisisobutyronitrile (AIBN) as initiator are mixed to synthesize surface imprinted copolymer (DSMIP). The obtained [email protected] has good conductivity and strong adsorption capacity for 5-HT due to hydrogen bonding and electrostatic interaction. When it is immobilized on a glassy carbon electrode for the electrochemical determination of 5-HT, the resulting sensor presents a wide linear response range (i.e. 0.20–10 μmol L −1 and 10–400 μmol L −1 ) and low limit of detection (i.e. 0.080 μmol L −1 ). Furthermore, it shows high selectivity, stability and reproducibility. To evaluate its practicability, the sensor is applied to the determination of 5-HT in human serum and human urine samples, and comparable results are achieved.
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Bioactive Materials
·
2021
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IF 14.593
Beibei Yang,Yating Dong,Yifeng Shen,Ailin Hou,Guilan Quan,Xin Pan,Chuanbin Wu
Hypertrophic scar (HS) is an undesirable skin abnormality following deep burns or operations. Although intralesional multi-injection with the suspension of triamcinolone acetonide (TA) and 5-fluorouracil (5-Fu) has exhibited great promise to HS treatment in clinical, the difference of metabolic behavior between TA and 5-Fu remarkably compromised the treatment efficacy. Besides, the traditional injection with great pain is highly dependent on the skill of the experts, which results in poor compliance. Herein, a bilayer dissolving microneedle (BMN) containing TA and 5-Fu (TA-5-Fu-BMN) with biphasic release profile was designed for HS therapy. Equipped with several micro-scale needle tips, the BMN could be self-pressed into the HS with uniform drug distribution and less pain. Both in vitro permeation and in vivo HS retention tests revealed that TA and 5-Fu could coexist in the scar tissue for a sufficient time period due to the well-designed biphasic release property. Subsequently, the rabbit ear HS model was established to assess therapeutic efficacy. The histological analysis showed that TA-5-Fu-BMN could significantly reduce abnormal fibroblast proliferation and collagen fiber deposition. It was also found that the value of scar elevation index was ameliorated to a basal level, together with the downregulation of mRNA and protein expression of Collagen I (Col I) and transforming growth factor-β1 (TGF-β1) after application of TA-5-Fu-BMN. In conclusion, the BMN with biphasic release profiles could serve as a potential strategy for HS treatment providing both convenient administrations as well as controlled drug release behavior.
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PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 9
·4236-4245
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IF 3.591
Jia Zhang,Jian Yang,Junying Tian,Hailong Liu,Xuemei Li,Weiguo Fang,Xun Hu,Chungu Xia,Jing Chen,Zhiwei Huang
The synthesis of useful amines from bio-based carbonyl compounds is highly desired owing to their mild reaction conditions and green sustainability. The reductive amination of bio-furfural-derived 2-hydroxytetrahydropyran (2-HTHP) to high-value-added 5-Amino-1-pentanol (5-AP) was carried out over efficient Ni–Al2O3 catalysts prepared by a co-precipitation method. Among the Ni–Al2O3 catalysts with different Ni loadings (0–100 wt%) tested, the 50Ni–Al2O3 catalyst exhibited the highest 5-AP yield of 91.3% under mild conditions of 60 °C and 2 MPa H2. This catalyst also presented good stability during a 150 h time-on-stream without appreciable deactivation. Characterization results showed that the 50Ni–Al2O3 catalyst exhibited small Ni0 nanoparticles (5.5 nm), a high reduction degree (up to 95%), and a large amount of strong Lewis acid sites. The cooperative catalysis of the strong Lewis acid sites and highly dispersed metallic Ni sites is suggested to play an important role in achieving high efficiency in 2-HTHP reductive amination.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Gang Li,Shanhong Ma,Feng Ye,Liang Zhou,Yanhong Wang,Xuemei Lang,Shuanshi Fan
Effective water removal from bio-oil is very important for upgrading bio-oil quality via esterification because water strongly inhibits the conversion and simultaneously lowers the heating value. In the present study, ZSM-5 zeolite membranes are applied to make bio-oil pervaporation dehydration more efficient. An investigation of the permeation performance demonstrated that water mainly permeated through ZSM-5 membranes via intercrystalline pores, whereas intracrystalline pores in the membrane were almost completely blocked because of intensive membrane fouling. The above result showed that tuning water transport paths was significantly important when designing high-performance ZSM-5 membranes for bio-oil pervaporation. A decrease in membrane fabrication time successfully created loose membrane structures with abundant intercrystalline pores and resulted in highly selective and stable ZSM-5 membranes with significantly improved permeation flux in bio-oil dehydration. These robust ZSM-5 membranes show great potential for bio-oil refining in industrial applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Changqu Lin,Hongli Wu,Junyi Wang,Jinsha Huang,Fei Cao,Wei Zhuang,Yanyu Lu,Jiao Chen,Honghua Jia,Pingkai Ouyang
The acidic catalysts play pivotal roles in the dehydration of hexose into 5-hydroxymethylfurfural (HMF). However, these acidic catalysts were usually exogenously added or self-made, which increase the cost of preparation of HMF. Herein, a novel route to prepare HMF from high fructose corn syrup (HFCS-55) using gluconic acid in situ produced by bio-oxidation as a catalyst has been investigated. In the process of bio-oxidation of HFCS-55, the introducing of ε-polylysine (EPL) can effectively improve the acid tolerance of the coimmobilized glucose oxidase and catalase. The immobilized enzymes can keep activity in the existence of a large amount of gluconic acid. Through the chelation of gluconic acid and calcium ions, the degree of gluconic acid ionization was raised and enough protons were released to convert fructose to HMF without the addition of acid. Using 2-methyltetrahydrofuran (2-MeTHF) as an extractor and adding 2 wt % CaCl2, the HMF’s yield reached 85% from fructose–gluconic acid mixture solution at 150 °C for 10 min with 200 W microwave irritations. Furthermore, we also used nuclear magnetic titration to investigate the complexation mechanism of the calcium ion and gluconic acid.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2020
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IF 4.939
Liying Zeng,Yizhou Wang,Jun Mou,Fei Liu,Chunliang Yang,Tianxiang Zhao,Xiaodan Wang,Jianxin Cao
γ-Al 2 O 3 was composited with ZSM-5 molecular sieve to improve its catalytic performance and hydrothermal stability during the conversion of crude methanol into dimethyl ether (DME). When prepared by a liquid-phase coating chemical compounding, the ZSM-5/γ-Al 2 O 3 composite catalyst reached an excellent methanol conversion of 91.9% and DME selectivity of 100%. The DME yield was increased by about 13% compared to only using γ-Al 2 O 3 . Partial desiliconization and dealumination of the ZSM-5 molecular sieve effectively reduced the surface acid center strength and increased the mesoporous ratio. The special composite phase interface effectively decreased surface charge density of γ-Al 2 O 3 and formed the B (Brønsted) - L (Lewis) synergistic active centers. All these factors contribute to improving the catalytic performance, hydrothermal stability and resistance to deactivation of ZSM-5/γ-Al 2 O 3 during the conversion of crude methanol to DME.
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高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 8
·2468-2473
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IF 9.48
Taimei Cai,Qiang Deng,Hailong Peng,Jin Zhong,Rui Gao,Jun Wang,Zheling Zeng,Ji-Jun Zou,Shuguang Deng
The major challenge in the synthesis of high-density biofuels is to identify the bio-based source for C–C cyclic compounds and C–C coupling reactions with a suitable selectivity. Herein, we selectively synthesize 1,2,4-benzenetriol (BTO) with a yield of 51.4% from cellulose-derived 5-hydromethylfurfural via a ring-rearrangement reaction. The cellulose-derived route is a more meaningful route for the C–C cyclic compounds compared to the traditional hemicellulose- and lignin-derived routes. Furthermore, BTO is very easily dimerized via a C–C oxidative coupling reaction, showing a yield of 94.4% and selectivity of nearly 100% under environmentally friendly reaction conditions. After hydrodeoxygenation, bicyclohexane is obtained with a yield of 87.4%. This work not only provides a promising route to produce C–C cyclic fine compounds based on a cellulose-derived route, but also shows a highly efficient synthesis route for high-density biofuels via the C–C oxidative coupling reaction.
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JOURNAL OF SOLID STATE CHEMISTRY
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2020
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IF 2.726
Yang Yunxia,Xia Shiying,Zhang Haixia,Niu Huihui,Dong Wenjing,Wu Xiangxiang
Two kinds of new complexes based on 3, 5-bis (triazol-1-yl) benzoic acid (HL) and 1, 3, 5-benzenetricarboxylic acid (H 3 bta), {[Zn 2 (μ 4 -L)(μ 3 -bta(3H 2 O)]∙H 2 O}n( 1 ) and {[Cd 2 (μ 4 -L)(μ 3 -bta(3H 2 O)]∙4H 2 O}n( 2 ), were prepared by solvothermal reactions and the structures were characterized by single-crystal X-ray diffraction. The experimental results showed that complexes 1 and 2 were isomorphic, in which metal ions were separately chelated with the ligands to form one mononuclear Cd 1 and another binuclear Cd 2 O 4 structure. Each metal center (M) can be considered as a three-connection, each M 2 O 4 as a six-connection, and the ligands of HL and H 3 bta can be used as three-junctions. Finally, complex 1 and 2 showed a (3, 6)-connection of {6 3 } 6 {6 6 ;8 6 ;10 2 ;12} topology. Solid-state fluorescence experiments showed that only complex 1 could selectively identify Fe 3+ (detection limit: 0.11 mM) and Cr 6+ (detection limit: 0.1 mM) in aqueous solution by a fluorescence quenching mechanism and the fluorescence quenching constant of Fe 3+ reached 10 4 . Dye adsorption experiments showed that the complexes could absorb different organic dyes and the adsorption capacity was 1 > 2 . Furthermore, the adsorption efficiency of 1 for methylene blue was as high as 97.64%.
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危险品化学品经营许可证（带存储）