INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2014
·Vol. 16
·期 5
·2490-2499
·
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
BIOSENSORS & BIOELECTRONICS
·
2017
·
IF 7.78
Wenjing Jiang,Linni Wu,Junling Duan,Huanshun Yin,Shiyun Ai
An ultrasensitive sandwiched electrochemiluminescence (ECL) immunosensor was developed for 5-hydroxymethylcytosine (5hmC) detection in genomic DNA by using Fe 3 O 4 @SiO 2 core–shell magnetic nanomaterial as a immobilization matrix for anti-5hmC antibody, PAMAM conjugated avidin and Ru(bpy) 2 (phen-5-NH 2 )(PF 6 ) 2 as signal amplification unit. Importantly, Fe 3 O 4 @SiO 2 nanoparticles were verified to not only possess enormous surface for loading antibody by amido link, but also exhibit excellent bioactivity . With the dual signal amplification strategy, the ECL immunosensor showed wide detection range from 0.1 to 30 nM with low detection limit of 0.047 nM (S/N = 3). Based on the specific immunoreaction, the developed method also illustrated excellent detection selectivity . The fabricated immunosensor was also applied to detect the 5hmC in genomic DNA of cancer tissue, which indicated that the immunosensor possess potential applications in clinical detection.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2015
·
IF 9.312
Liang Wang,Jian Zhang,Xianfeng Yi,Anmin Zheng,Feng Deng,Chunyu Chen,Yanyan Ji,Fujian Liu,Xiangju Meng,Feng-Shou Xiao
Zeolite-based catalysts have been widely used in the conversion of biomass recently, but the catalytic yields of the desired products are strongly limited by the relatively small micropores of zeolite. Here, we reported a hierarchically porous ZSM-5 zeolite with micropore and b-axis-aligned mesopore-supported Ru nanoparticles (Ru/HZSM-5-OM) that are highly efficient for the hydrodeoxygenation of both small and bulky phenolic biomolecules to the corresponding alkanes. Compared with the conventional ZSM-5 zeolite-supported Ru catalyst, the high catalytic activities and alkane selectivities over Ru/HZSM-5-OM are attributed to the abundant exposed acidic sites in HZSM-5-OM with open mesopores. This feature is potentially important for future phenolic bio-oil upgrading.
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2017
·Vol. 10
·期 4
·711-719
·
IF 7.226
Shanshan Li,Fang Chen,Ning Li,Wentao Wang,Xueru Sheng,Aiqin Wang,Yu Cong,Xiaodong Wang,Tao Zhang
Graphical Green triketones : Renewable C 9 –C 12 triketones with repeating [COCH 2 CH 2 ] units are synthesized in high carbon yields (ca. 90 %) over a cost-effective and reusable Au/TiO 2 catalyst. The triketones as obtained can be used as feedstocks in the production of conducting or semi-conducting polymers. Furthermore, they can also be converted to diketones or jet-fuel range branched cycloalkanes with high densities and low freezing points. A series of renewable C 9 –C 12 triketones with repeating [COCH 2 CH 2 ] units were synthesized in high carbon yields (ca. 90 %) by the aqueous-phase hydrogenation of the aldol-condensation products of 5-hydroxylmethylfurfural (HMF) and ketones over an Au/TiO 2 catalyst. Compared with the reported routes, this new route has many advantages such as being environmentally friendly, having fewer steps, using a cheaper and reusable catalyst, etc. The triketones as obtained can be used as feedstocks in the production of conducting or semi-conducting polymers. Through a solvent-free intramolecular aldol condensation over solid-base catalysts, the triketones were selectively converted to diketones, which can be used as intermediates in the synthesis of useful chemicals or polymers. As another application, the tri- and diketones can also be utilized as precursors for the synthesis of jet-fuel range branched cycloalkanes with low freezing points (224–248 K) and high densities (ca. 0.81 g mL −1 ).
✓ 已验证
产品关联
DOI
PubMed
高影响因子
REACTIVE & FUNCTIONAL POLYMERS
·
2024
·
IF 4.5
Linlin Yu,Ruoyu Chen,Qian Jia
Oily wastewater, especially oil-water emulsions, has caused severe environmental damage. It is urgent to develop a simple, efficient superhydrophobic and superoleophilic material to address this issue. In this work, a multifunctional sponge based on MOF was proposed. The hydroxy-assisted method was employed to prepare MOF-5 with metal coordination centers. Subsequently, octadecylphosphonic acid (OPA) was used to hydrophobically modify MOF-5 to prepare stable and hydrophobic OPA-MOF-5. Polydimethylsiloxane (PDMS) with low surface energy was employed as the adhesive, and the hydrophobic OPA-MOF-5 was loaded onto the polyurethane (PU) sponge to obtain the stable superhydrophobic OPA-MOF-5@PDMS@PU with a WCA of 155.9°. The produced modified sponge exhibited high sorption capacity and oil-water separation efficiency, with a sorption capacity of 26.7 (petroleum ether)-85.6 (chloroform) g/g and a separation efficiency of over 99 %. It has also shown satisfactory emulsion purification and flame retardancy capacities.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Sitong Liu,Shengli Niu,Hewei Yu,Kuihua Han,Sunwen Xia,Zihao Yang,Yue Zheng,Yujiao Zhang,Yanan Hao,Abulikemu Abulizi
The current transesterification for biodiesel is normally conducted with heat input and the resource is required to remove the contained water, which is complicated and costly. The novel magnetic catalyst of the bimetallic oxides of CeO 2 and Fe 3 O 4 supported on the hierarchical pore ZSM-5 was prepared and used for the biodiesel production through transesterification of palm oil with methanol under the electrolytic assistance. The prepared catalysts were characterized by SEM-EDS, TEM, FTIR, XRD, CO 2 /NH 3 -TPD, N 2 adsorption–desorption and VSM, etc. The loaded cerium stimulated the particles growth and abundant catalytic active sites were obtained due to the coral-like structure and they were beneficial for transesterification. The presence of both acidic and basic sites guaranteed the strong catalytic capability of the CeO 2 /ZSM-5@Fe 3 O 4 catalyst. Under the optimized transesterification condition of the catalyst dosage of 3 wt%, methanol to oil molar ratio of 18:1, reaction time of 2.5 h, electrolysis voltage of 40 V, presence of 2 % wt/wt of water added and reaction temperature of 25 ℃, the FAME yield of approximately 95 % was achieved. Also, the catalyst showed an acceptable reusability, where the FAME yield of 79 % was obtained after fourth reused cycle. In conclusion, the water in the resource promotes the electrolytic transesterification to occur efficiently at the room temperature.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）