SCIENCE OF THE TOTAL ENVIRONMENT
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2018
·
IF 4.61
Guanyi Chen,Ruixue Zhang,Wenchao Ma,Bin Liu,Xiangping Li,Beibei Yan,Zhanjun Cheng,Tiejun Wang
The catalytic cracking upgrading reactions over HZSM-5 of different model compounds of bio-oil have been studied with a self-designed fluid catalytic cracking (FCC) equipment. Typical bio-oil model compounds, such as acetic acid, guaiacol, n-heptane, acetol and ethyl acetate, were chosen to study the products distribution, reaction pathway and deactivation of catalysts. The results showed: C 6 –C 8 aromatic hydrocarbons , C 2 –C 4 olefins , C 1 –C 5 alkanes, CO and CO 2 were the main products, and the selectivity of olefins was: ethylene > propylene > butylene . Catalyst characterization methods, such as FI-IR, TG-TPO and Raman, were used to study the deactivation mechanism of catalysts. According to the catalyst characterization results, a catalyst deactivation mechanism was proposed as follows: Firstly, the precursor which consisted of a large number of long chain saturated aliphatic hydrocarbons and a small amount C C of aromatics formed on the catalyst surface. Then the active sites of catalysts had been covered, the coke type changed from thermal coke to catalytic coke and gradually blocked the channels of the molecular sieve, which accelerated the deactivation of catalyst.
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POLYMER DEGRADATION AND STABILITY
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2015
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IF 3.163
Hongli Wu,Binbin Wen,Hua Zhou,Jiadong Zhou,Zuolong Yu,Liyan Cui,Ting Huang,Fei Cao
Polyethylene 2, 5-furandicarboxylate-lactic acid copolyesters (PEFL) were synthesized from bis (hydroxyethyl)-2, 5-furandicarboxylate and oligomer of l -lactic acid, through two-stage condensation . The polyesters were characterized using FTIR, 1 H NMR, GPC , and WXRD. The weight-average molecular weight (M w ) of the polyesters ranged from 68240 to 130433. The glass transition temperature (T g ) of the copolyesters increased gradually with increasing content of 2, 5-furandicarboxylate. In phosphate buffer solution (PBS, pH = 7.4) and in soil, the degradability of the polyesters was evaluated for 55 d. More weight loss was obtained with a higher ratio of lactate polymers in soil than those with a lower ratio in PBS. After 55 d, the weight loss of PEFL20/80 reached 65% and 24% in soil and PBS, respectively. However, the mole fraction of lactyl and furanic units that was calculated by 1 H NMR data did not change. Comparing the scanning electron microscopy images, we found many micro-cracks on the copolyester surfaces. Meanwhile, M w and T g also decreased prominently during degradation.
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RSC Advances
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2013
·Vol. 3
·期 20
·7360-7366
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IF 2.562
Shimin Kang,Jun Ye,Yu Zhang,Jie Chang
Amorphous carbon-based sulfonated catalysts were generated from four kinds of biomass (lignin, cellulose, wood meal and D-xylose) by hydrothermal carbonization at various temperatures (225, 245 and 265 °C) followed by sulfonation, with a yield of 36–56%. All of these catalysts showed aromatic structure, hydroxyl and carboxyl groups, with a density of SO3H groups between 0.56 and 0.87 mmol g−1. 5-Hydroxymethylfurfural (HMF) was produced from inulin in ionic liquids (ILs) in one step with the addition of carbon-based sulfonated catalysts, with a factual yield of 47–65% at 100 °C, 60 min. Moderate extension of reaction time (from 30 to 90 min) and increase of temperature (from 80 to 120 °C) promoted HMF production. Ethyl acetate was used as extractant, and about 39–55% of HMF can be recovered from ILs. One problem with these carbon-based sulfonated catalysts was that they would be partly deactivated in ILs for separate reuse, however, they can be easily regenerated by dilute sulfuric acid treatment. The carbon-based sulfonated catalysts exhibited good catalytic activity compared with traditional solid acid catalysts, and the carbon-based sulfonated catalyst/ILs reaction system showed high reusability. In consideration of the renewable as well as the high catalytic activity abilities, these biomass derived carbon-based sulfonated catalysts would be promising for industrial application.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2014
·
IF 2.235
Lei Hu,Xing Tang,Jiaxing Xu,Zhen Wu,Lu Lin,Shijie Liu
A simple and efficient process was presented for the selective hydrogenation of 5-hydroxymethylfurfural (HMF) into the high-quality liquid fuel 2,5-dimethylfuran (DMF) in the presence of tetrahydrofuran (THF). Among the employed metal catalysts, the relatively inexpensive carbon-supported ruthenium (Ru/C) displayed the highest catalytic performance, which led to 94.7% DMF yield with 100% HMF conversion at a relatively mild reaction temperature of 200 °C for only 2 h. Although Ru/C had a little loss in the catalytic activity when it was used for five successive reaction runs, the partially deactivated Ru/C could be easily regenerated by heating at a mixed flow of H2 and N2. Moreover, the plausible mechanism involving an aldehyde group, a hydroxyl group, and a furan ring for the selective hydrogenation of HMF into DMF was also proposed. Subsequently, DMF was separated from the crude hydrogenation mixture according to their various boiling points by the combination of atmospheric distillation and vacuum distillation, and then, the chemical structures and physical properties of the separated DMF were confirmed to be consistent with the authentic DMF. More gratifyingly, Ru/C and THF were also found to be a good combination for the direct hydrogenation of carbohydrate-derived HMF into DMF, which is very important for the practical production of DMF from a variety of biomass-derived carbohydrates such as fructose, glucose, sucrose, maltose, cellobiose, starch, and cellulose.
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BIOMATERIALS
·
2014
·
IF 8.312
Pengfei Chen,Shouan Zhu,Yanyan Wang,Qin Mu,Yan Wu,Qingqing Xia,Xiaolei Zhang,Heng Sun,Jiadong Tao,Hu Hu,Ping Lu,Hongwei Ouyang
Degradation of proteoglycan is the key early event in the development of osteoarthritis (OA). The aggrecanase ADAMTS-5 has been identified as the major enzyme responsible for the degradation and thus is an attractive therapeutic target for OA. However, currently there is no report on using an ADAMTS-5 inhibition strategy for OA treatment. The present study aimed to investigate the synergic effect of combining an ADAMTS-5 inhibitor (114810) with a hyaluronic acid hydrogel (HAX) for OA therapeutics. Two OA models were induced by surgically creating an osteochondral defect or removing the anterior cruciate ligament (ACL) in Sprague–Dawley rats. Human OA cartilage was obtained from total joint replacement patients. Both human and rat OA cartilage showed marked proteoglycan loss with significantly increased ADAMTS-5 expression. The effectiveness of ADAMTS-5 inhibition by 114810 was confirmed by a cartilage explants assay in vitro , which showed that the 114810 halted the aggrecanase-mediated 374 ARGS neoepitope released from aggrecan induced by IL-1β stimulation. The in vivo effect of ADAMTS-5 inhibition was assessed by the articular injection of HAX with 114810 into OA knee joints. Evaluated eight weeks after injection, 114810 with HAX significantly promoted the in vivo cartilage healing in the osteochondral defect model, and prevented the progression of degenerative changes in the ACL model. Our results confirmed that ADAMTS-5 is an effective target for OA treatment, and the intra-articular injection of an ADAMTS-5 inhibitor within HAX gel could be a promising strategy for OA treatment.
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高影响因子
GREEN CHEMISTRY
·
2014
·Vol. 16
·期 5
·2490-2499
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IF 6.852
Jinzhu Chen,Kegui Li,Limin Chen,Ruliang Liu,Xing Huang,Daiqi Ye
A series of sulfonic acid-functionalized metal–organic frameworks (MOF-SO3H) were prepared by postsynthetic modification (PSM) of the organic linkers within the MOF with chlorosulfonic acid. The obtained MOF-SO3H, including sulfonic acid-functionalized MIL-101(Cr) [MIL-101(Cr)-SO3H], UIO-66(Zr) [UIO-66(Zr)-SO3H], and MIL-53(Al) [MIL-53(Al)-SO3H], have been systematically studied as solid acids in fructose transformation to 5-hydroxymethylfurfural (HMF). With MIL-101(Cr)-SO3H as catalyst, a HMF yield of 90% with a full fructose conversion was obtained at 120 °C for 60 min in DMSO. The concentration of –SO3H in MOF-SO3H as well as the contribution of Brønsted acidity of MOF-SO3H parallels its –SO3H grafting rate. Under a lower –SO3H grafting level, a good linear correlation between catalytic activity, in terms of turnover frequency, and sulfonic acid-site density of MOF-SO3H was found. Moreover, the sulfonic acid groups, which function as the catalytic sites, are equivalent in all MOF-SO3H for fructose-to-HMF transformation, regardless of precursor MOFs. Both conversions of fructose and selectivities towards HMF increase with the sulfonic acid-site density of MOF-SO3H at an initial stage of fructose-to-HMF transformation. Kinetics studies reveal that the MIL-101(Cr)-SO3H promoted fructose-to-HMF transformation may follow pseudo-first-order kinetics with observed activation energy of 55 kJ mol−1 under the investigated conditions. Moreover, MIL-101(Cr)-SO3H behaves as a heterogeneous catalyst and can be easily recovered and reused. The research highlights a good prospect for catalytic application of MOF-derived solid acid catalysts for biomass carbohydrate valorization.
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BIORESOURCE TECHNOLOGY
·
2013
·
IF 4.75
Huiyan Zhang,Mengmeng Luo,Rui Xiao,Shanshan Shao,Baosheng Jin,Guomin Xiao,Ming Zhao,Junyu Liang
Chemical liquid deposition (CLD) with KH550, TEOS and methyl silicone oil as the modifiers was used to modify ZSM-5 and deposit its external acid sites. The characteristics of modified catalysts were tested by catalytic conversion of biomass pyrolysis-derived compounds. The effects of different modifying conditions (deposited amount, temperature, and time) on the product yields and selectivities were investigated. The results show KH550 modified ZSM-5 (deposited amount of 4%, temperature of 20 °C and time of 6 h) produced the maximum yields of aromatics (24.5%) and olefins (16.5%), which are much higher than that obtained with original ZSM-5 catalyst (18.8% aromatics and 9.8% olefins). The coke yield decreased from 44.1% with original ZSM-5 to 26.7% with KH550 modified ZSM-5. The selectivities of low-molecule-weight hydrocarbons (ethylene and benzene) decreased, while that of higher molecule-weight hydrocarbons (propylene, butylene, toluene, and naphthalene) increased comparing with original ZSM-5.
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INORGANICA CHIMICA ACTA
·
2015
·
IF 2.046
Hui Liu,Chun Hua,Changhua Song,Shifeng Dai,Hongwei Wang,Wenshuai Zhu,Huaming Li
Some sulfur oxyacid salts with weak acidity or alkalinity, including Na 2 SO 4 , (NH 4 ) 2 SO 4 , (NH 4 ) 2 S 2 O 3 and Na 2 S 2 O 3 , were applied to the conversion of fructose to 5-hydroxymethylfurfural. The results indicated that (NH 4 ) 2 S 2 O 3 had excellent catalytic performance for the conversion of fructose. A desired HMF yield of 81.6% was obtained with only 5 mg (NH 4 ) 2 S 2 O 3 as the catalyst in [Bmim]Cl at 120 °C for 50 min. Furthermore, the HMF yield remained at 76.6% with 60 wt% water in the IL–water mixture solvent. In addition, the system of (NH 4 ) 2 S 2 O 3 and [Bmim]Cl exhibited a constant stability and activity, and a good HMF yield was maintained after nine recycles.
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CATALYSIS TODAY
·
2015
·
IF 3.893
Chunyu Chen,Xiong Wang,Jian Zhang,Chaoqun Bian,Shuxiang Pan,Fang Chen,Xiangju Meng,Xiaoming Zheng,Xionghou Gao,Feng-Shou Xiao
Catalytic combustion over zeolite supported platinum catalysts is regarded as one of the efficient methods for removal of volatile organic compounds (VOCs). In this work, we show a preparation of Pt loaded mesoporous ZSM-5 zeolite (Pt/Meso-ZSM-5) with various cations. The sample N 2 sorption isotherms and TEM image show abundant mesoporosity existing in the zeolite crystals. The catalytic toluene combustion tests show that the Pt/Meso-ZSM-5 catalysts have higher activities than conventional ZSM-5 supported Pt catalysts (Pt/ZSM-5), which is related to their difference in the concentration of active sites Pt 0 and the rate of mass transfer. Particularly, after reduction with hydrogen at 300 °C, the Pt nanoparticles supported on Meso-ZSM-5 with K + and Cs + cations (Pt-R/Meso-KZSM-5 and Pt-R/Meso-CsZSM-5) exhibit much higher activities than those on Meso-ZSM-5 with Na + and H + cations, which is well consistent with their order of the Pt 0 concentration. For example, Pt-R/Meso-KZSM-5 gives the temperature for conversion of 98% toluene ( T 98 ) at only 175 °C, while Pt-R/Meso-HZSM-5 shows the T 98 at 190 °C. More importantly, Pt-R/Meso-KZSM-5 has a long life, and its activity cannot be influenced by the water and CO 2 . These features are critically important for practical applications of these catalysts in the future.
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ACS Applied Materials & Interfaces
·
2015
·
IF 6.723
Yonghuan Ren,Daobin Mu,Feng Wu,Borong Wu
We report a novel slurry electrolyte with ultrahigh concentration of insoluble inorganic lithium metasilicate (Li2SiO3) that is exploited for lithium ion batteries to combine the merits of solid and liquid electrolytes. The safety, conductivity, and anodic and storage stabilities of the eletrolyte are examined, which are all enhanced compared to a base carbonate electrolyte. The compatibility of the elecrolyte with a LiNi0.5Mn1.5O4 cathode is evaluated under high voltage. A discharge capacity of 173.8 mAh g–1 is still maintained after 120 cycles, whereas it is only 74.9 mAh g–1 in the base electrolyte. Additionally, the rate capability of the LiNi0.5Mn1.5O4 cathode is also improved with reduced electrode polarization. TEM measurements indicate that the electrode interface is modified by Li2SiO3 with a thinner solid electrolyte interphase film. Density functional theory computations demonstrate that LiPF6 is stabilized against its decomposition by Li2SiO3. A possible path for the reaction between PF5 and Li2SiO3 is also proposed by deducing the transition states involved in the process using the DFT method.
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POLYMER DEGRADATION AND STABILITY
·
2015
·
IF 3.163
Mingguang Li,Hongjun Zang,Jiaxuan Feng,Qing Yan,Nianqin Yu,Xiaolong Shi,Bowen Cheng
A new process for the efficient conversion of chitosan into 5-hydroxymethylfurfural (5-HMF) has been developed. Chitosan was hydrolyzed in the presence of acidic ionic liquids (ILs), with N-methyl imidazolium hydrogen sulfate ([MIM]HSO 4 ) giving the best results. The effects of reaction time, temperature and quantity of water and IL were investigated in detail. The optimal reaction conditions were found to be 4wt % IL ([MIM]HSO 4 ) aqueous solution under hydrothermal condition, 180 °C and a reaction time of 5 h. A yield of 29.5 mol% 5-HMF was obtained from 100 mg chitosan. Furthermore, chitosan with different molecular weight could be directly converted into 5-HMF in good yields under these conditions. More importantly, [MIM]HSO 4 could be recovered by simple post-processing and exhibited constant activity over 5 cycles.
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Journal of the Taiwan Institute of Chemical Engineers
·
2015
·
IF 3
Shuguo Wang,Bing Liu,Ziliang Yuan,Zehui Zhang
In this study, magnetic γ-Fe 2 O 3 @ HAP-Mo catalyst was successfully prepared and characterized. The activity of the as prepared γ-Fe 2 O 3 @ HAP-Mo catalyst was evaluated by the oxidation of 5-hydroxymethylfurfural (HMF) with molecular oxygen. Some important reaction parameters were investigated and it was found that both the solvent and the reaction temperature showed great effect on HMF conversion and products selectivity. The highest HMF conversion of 95.8% was obtained in 4-chlorotoluene at the reaction temperature of 120 °C for 12 h, and the corresponding 2,5-diformylfuran, 2,5-furandicarboxylic acid and 5-hydroxymethyl-2-furancarboxylic acid yields were 67.5, 19.6 and 8.7%, respectively. The γ-Fe 2 O 3 @ HAP-Mo catalyst could be easily separated from the reaction mixture and reused several times without the loss of its catalytic activity.
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危险品化学品经营许可证（带存储）