FUEL PROCESSING TECHNOLOGY
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2016
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IF 3.847
Haian Xia,Siquan Xu,Xiaopei Yan,Songlin Zuo
It is of great significance to explore and develop a cost-effective and environmentally friendly way to covert cellulosic materials into 5-hydroxymethylfurfural (5-HMF). An inexpensive FePO 4 catalyst, which is insoluble at room temperature but can be partially dissolved and behaves as homogeneous catalyst at elevated temperatures, was used to directly convert cellulose into 5-HMF. The effect of various reaction conditions including reaction temperature, reaction time, cellulose concentration and catalyst amount on the conversion of cellulose and 5-HMF yield was investigated. A 5-HMF yield up to 49.5 mol% was achieved at 160 °C for 60 min with the FePO 4 catalyst, which is comparable to the highest yield of 5-HMF obtained in ionic liquid or homogeneous catalysis reaction systems. Moreover, this unique catalyst is readily separated from the aqueous solution via precipitation after cooling to room temperature since it is insoluble at room temperature. The catalyst can be used over five successive cycles although the amorphous FePO 4 underwent the structural transformation from an amorphous phase into a new crystalline form of FePO 4 , evidenced by XRD, IR, and visible Raman spectroscopic results. The soluble iron species, such as Fe 3 + species, act as Lewis acid sites catalyzing isomerization of glucose to fructose followed by the dehydration of fructose into 5-HMF catalyzed by H + ions.
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AICHE JOURNAL
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2016
·Vol. 62
·期 12
·4403-4417
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IF 2.98
Ye Su,Ganggang Chang,Zhiguo Zhang,Huabin Xing,Baogen Su,Qiwei Yang,Qilong Ren,Yiwen Yang,Zongbi Bao
Glucose conversion to 5-hydroxymethylfurfural (HMF) generally undergoes catalytic isomerization reaction by Lewis acids followed by the catalytical dehydration to HMF with Brönsted acid. In this work, a sulfonic acid functionalized metal-organic framework MIL-101(Cr)-SO 3 H containing both Lewis acid and Brönsted acid sites, was examined as the catalyst for γ-valerolactone-mediated cascade reaction of glucose dehydration into HMF. Under the optimal reaction conditions, the batch heterogeneous reaction gave a HMF yield of 44.9% and selectivity of 45.8%. Reaction kinetics suggested that the glucose isomerization in GVL with 10 wt % water follows the second-order kinetics with an apparent activation energy of 100.9 kJ mol −1 . Continuous reaction in the fixed-bed reactor showed that the catalyst is highly stable and able to provide a steady HMF yield. This work presents a sustainable and green process for catalytic dehydration of biomass-derived carbohydrate to HMF with a bifunctional metal-organic framework. © 2016 American Institute of Chemical Engineers AIChE J , 62: 4403–4417, 2016
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CHINESE CHEMICAL LETTERS
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2016
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IF 1.947
Yu-Tao Zheng,Teng-Teng Zhang,Pei-Yi Wang,Zhi-Bing Wu,Lei Zhou,Yi-Qiang Ye,Xiang Zhou,Ming He,Song Yang
By introducing the pyrazole moiety into the 5-position of 1,3,4-oxadiazole, a series of novel 2-(thioether/sulfone)-5-pyrazolyl-1,3,4-oxadiazole derivatives were synthesized. Preliminary bioassays suggested that target compounds exhibited appreciable activity against pathogenic bacteria Xanthomonas oryzae pv. oryzae ( Xoo ) and five phytopathogenic fungi in vitro . Among them, the half-maximal effective concentration (EC 50 ) values of 6c , 7a , 7b and 7c against Xoo were within 16.6 μg/mL and 65.7 μg/mL, which were better than those of commercial agricultural antibacterial bismerthiazol (92.6 μg/mL) and thiodiazole copper (121.8 μg/mL). While compounds 7a , 7b , and 7c exerted comprehensive antifungal activity toward five plant fungi, which were comparable with that of hymexazol. The results demonstrated that this kind of compounds can be further studied and developed as promising antifungal and antibacterial agents.
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CHEMICAL ENGINEERING JOURNAL
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2017
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IF 6.216
Jundong Xu,Yunfeng Guo,Tingting Huang,Yu Fan
This article proposes a novel decamethonium bromide-assisted method for modulating the size of supported metal nanoparticles in Pd/mesoporous HZSM-5 hydrodesulfurization (HDS) catalysts. The proposed approach significantly promotes the dispersion of supported palladium nanoparticles by bridging and anchoring the palladium precursor onto the surface of mesoporous HZSM-5 as well as restraining the subsequent aggregation of palladium nanoparticles in calcination. The as-prepared catalyst possessed higher 4,6-dimethyldibenzothiophene HDS activity than its counterpart that was prepared via impregnation due to its smaller Pd nanoparticles, higher Pd dispersion and higher content of Pd 0 species. This strategy provides a simple pathway for preparing supported metal nanoparticles with high dispersion.
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BioEnergy Research
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2013
·Vol. 6
·期 4
·1173-1182
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IF 4.25
Shao Shanshan,Zhang Huiyan,Xiao Rui,Shen Dekui,Zheng Jian
The conversion of three major biomass derivates was conducted in a quartz tubular fixed bed reactor over a ZSM-5 catalyst. As the model compounds of polyols, saturated furans and unsaturated furans, ethylene glycol (EG), tetrahydrofuran (THF) and furan were pyrolyzed to find out the influence of chemical structure on the catalytic characteristics. The effect of pyrolysis temperature (400 ∼ 650 °C), weight hourly space velocity (2.9 ∼ 15.5 h −1 ) and partial pressure (2.12 ∼ 20.49 Torr) on the feed conversion, product yield and selectivity were investigated. The hydrogen to carbon effective ratio (H/C eff ) was referred to, to analyze the capacity of biomass derivates being converted to chemicals (olefins and aromatics). The results showed that the existence of rings and C=C had great effect on the catalytic characteristics. The conversion of furan was much lower (mainly less than 60 %) than that of EG and TH,F which were close to 100 %. It was also found that the chemical yield of THF was slightly more than that of EG, which can be attributed to its relative higher H/C eff of 1.5. Furan produced the highest coke yield, which was more than 15 %, whereas that of EG and THF was only around 5 %. The serious coking of furan led to the lowest chemical yield, which was less than 35 %. This study paves a way for the mechanism study on catalytic characteristics of biomass-derived feedstocks over zeolite catalysts.
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ChemCatChem
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2014
·Vol. 6
·期 3
·728-732
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IF 5.044
Hongliang Wang,Qingqiang Kong,Yingxiong Wang,Tiansheng Deng,Chengmeng Chen,Xianglin Hou,Yulei Zhu
Graphical GO-ing all the way: Graphene oxide is demonstrated to be a green heterogeneous catalyst for the selective dehydration of fructose into 5-hydroxymethylfurfural (HMF) in a cost efficient and environmentally benign isopropanol-mediated solvent system. A small number of sulfonic groups with the synergic effect of oxygen-containing groups (alcohols, epoxides, carboxylates) make graphene oxide an efficient acid catalyst. The design of green heterogeneous catalysts for the efficient conversion of biomass into platform molecules is a key aim of sustainable chemistry. Graphene oxide prepared from Hummers oxidation of graphite was proven to be a green and efficient carbocatalyst for the dehydration of fructose into 5-hydroxymethylfurfural (HMF) in some three-carbon and four-carbon alcohol mediated solvent systems. HMF was obtained in up to 87 % yield in 90 vol % isopropanol-mediated DMSO solvent. Some control experiments and analytical data showed that a small number of sulfonic groups and abundance of oxygen-containing groups (alcohols, epoxides, carboxylates) have an important synergic effect in maintaining the high performance of graphene oxide.
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International Journal of Chemical Engineering
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2014
·
IF 0
Hu Li,Qiuyun Zhang,Song Yang
A series of SO3H-functionalized polymers were prepared and employed as heterogeneous catalysts for one-pot transformation of fructose into 5-ethoxymethylfurfural (EMF) that is considered to be one of potential liquid biofuels. A high EMF yield of 72.8% could be obtained at 110°C for 10 h, and the polymeric acid catalysts could be recycled for five times without significant loss of catalytic performance.
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FUEL
·
2015
·
IF 3.52
Haimei Xu,Zhichao Miao,Huahua Zhao,Jian Yang,Jun Zhao,Huanling Song,Ning Liang,Lingjun Chou
In this paper, a series of ordered mesoporous zirconium oxophosphate with different P/Zr molar ratios (M-ZrPO- x ) were prepared via one-pot evaporation induced self-assembly strategy (EISA). The catalytic performance of M-ZrPO- x for the dehydration reaction of fructose to produce 5-hydroxymethylfurfural (5-HMF) was also studied. With high concentration of Brönsted and Lewis acid sites measured through NH 3 -TPD and pyridine-IR, M-ZrPO-0.75 performed high catalytic activity (up to 97.4%) and selectivity (79.6%) of 5-HMF under relatively mild conditions. Furthermore, M-ZrPO-0.75 performed excellent catalytic stability. Based on detailed analyses of XRD, SEM, TEM, BET and XRF, the structural, surface and textural properties of M-ZrPO-0.75 after reaction were investigated. Obtained results demonstrated that the mesostructure still retained even after twelve cycles, which may be ascribed to the “ordered” mesoporous properties and high thermal stability. In addition, a lower activation energy was obtained in this M-ZrPO catalytic system using dimethyl sulfoxide as solvent.
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Asia-Pacific Journal of Chemical Engineering
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2017
·Vol. 12
·期 4
·527-535
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IF 0.836
Guizhuan Xu,Binglin Chen,Zhangbin Zheng,Kai Li,Hongge Tao
5-Ethoxymethylfurfural (EMF) and ethyl levulinate (EL) have been considered as the new promising biofuels. A comparative study was conducted for the direct conversion of carbohydrates into EMF and EL in different medium containing ethanol. The distribution and formation kinetics of EL, EMF, 5-hydroxymethylfurfural (HMF) and levulinic acid (LA) in pure ethanol and ethanol/organic solvent medium were compared, and the results showed that the addition of n-hexane can improve the accumulation of EMF. When the volume ratio of ethanol to n-hexane was 6:4, 66.29% of EMF yield can be obtained from fructose at 120°C and 180 min. The total yield of the EMF and EL can reach to 83.71%, increased by 5.73% compared with that in pure ethanol medium. Moreover, water addition can suppress the etherification of HMF to EMF and promote the rehydration of HMF to LA in the process. On the basis, a putative reaction pathway for the conversion of carbohydrates in ethanol/n-hexane medium was proposed. © 2017 Curtin University of Technology and John Wiley & Sons, Ltd.
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SCIENTIA HORTICULTURAE
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2017
·
IF 1.624
Jie Zheng,Yu-yan An,Xin-xin Feng,Liang-ju Wang
5-Aminolevulinic acid (5-ALA), an eco-friendly plant growth regulator, has been increasingly applied to crop and fruit production. In the actual production, many fruits are often covered by plastic bags which will not be removed until the fruits are harvested. Therefore, although 5-ALA shows promotive effect on fruit quality, fruit spray cannot be implemented in the orchards using plastic bags. In this study, rhizospheric application of 5-ALA increased the endogenous 5-ALA content in the leaves and fruits, suggesting that 5-ALA is transported from roots to aboveground. Using a multiple plant efficiency analyzer (M-PEA), we also found that rhizospheric application of 5-ALA significantly improved PS II and PS I photosynthetic activities of apple leaves. It means that 5-ALA-treated apple trees might accumulate more assimilates for fruits to improve their quality. Meanwhile, rhizospheric application of 5-ALA obviously increased fruit weight, the content of flavonoids, total soluble solids and ascorbic acid, as well as activities of antioxidant enzymes. Most importantly, rhizospheric irrigation of 5-ALA also significantly improved fruit coloration. Using calli induced from the flesh of ‘Fuji’ fruits, we found that 5-ALA up-regulated the expressions of many genes involved in flavonoid anabolism. These results suggest that rhizospheric application of 5-ALA solution is effective to improve external and interior qualities of apple fruits although 5-ALA was not directly applied to fruit surface. Taken together, we conclude that rhizospheric application of 5-ALA can be transported to the leaves and fruits of apple trees, where it enhances leaf photosynthetic capacity and improves fruit coloration and interior qualities simultaneously. This finding provides an effective and handy method to improve apple quality in modern orchards.
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RSC Advances
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2015
·Vol. 5
·期 128
·106053-106060
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IF 3.84
Jie Wang,Ting Qu,Minsi Liang,Zhenbo Zhao
In this work, we investigated the dehydration of fructose into 5-hydroxymethylfurfural using solid catalysts with microwave assistance in dimethyl sulfoxide. Five kinds of solid catalyst ZrO2, WOx/ZrO2, MoOx/ZrO2, SO42−/WOx–ZrO2 and SO42−/MoOx–ZrO2 were prepared and characterized by XRD, UV-DRS, FTIR, XPS, TEM, TPD, BET, and Raman and the surface acid amount was obtained by combining pyridine adsorption and UV spectrometry. The SO42−/WOx–ZrO2 catalyst was found be the most active catalyst, and a fructose conversion of 95.80% with 83.90% 5-HMF yield was obtained at 150 °C in a relatively short reaction time of 5 min. The value of the activation energy was comparable with previous values reported in the literature, implying that SO42−/WOx–ZrO2 was efficient for the dehydration of fructose to 5-HMF and that microwave radiation heating had a remarkable accelerating effect on the fructose conversion.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Tianli Hui,Haowei Liu,Tonghui Li,Jinbo Pan,Tao Zheng,Rui Zhang,Xianghai Meng,Haiyan Liu,Zhichang Liu,Chunming Xu
The electrooxidation of 5-hydroxymethylfurfural (HMF) has emerged as a promising way to generate high-value-added products. However, evoking high-valence state NiOOH species as active sites to realize high current density remains a challenge. Herein, we report an efficient electrocatalyst for HMF electrooxidation based on phosphate anion intercalated layered double hydroxides (NiCo-Pi-LDHs). Onset potential at 1.16 V vs. RHE and current density of 200 mA/cm 2 at 1.41 V vs. RHE were realized. The intercalated phosphates act as proton transfer intermediates, facilitating the dehydrogenation of hydroxides to form oxyhydroxides while the protonated phosphate generated. The obtained oxyhydroxide oxidized HMF to 2,5-furandicarboxylic (FDCA) while cycling backward to hydroxide, accompanied by the cycle of protonated phosphate to phosphate. This novel strategy with dual-cycle of phosphate and nickel species can effectively evoke NiOOH species, thereby speeding up the reaction rate and having a great potential for biomass upgrading.
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