ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Peng Zhu,Weizi Zhang,Qinfang Li,Haian Xia
Photocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is an environmental friendly way to convert platform molecules into high-value chemicals. Here, Au/ZnO catalysts with different oxygen vacancies were fabricated by the deposition precipitation method and were used for the photocatalytic oxidation of HMF to FDCA under visible light irradiation. All of the Au/ZnO catalysts showed excellent photocatalytic oxidation selectivity to FDCA greater than 90% under mild conditions. The Au/ZnODP-H catalyst treated by H2 afforded the highest HMF conversion and the selectivities of FDCA up to 96.9%. The localized surface plasmon resonance effect of Au nanoparticles, oxygen vacancy, and the existence of the Schottky barrier enhance the separation and transfer efficiency of photogenerated electron–hole pairs of the catalyst, so as to enhance its photocatalytic activity. The active species trapping experiment and electron spin resonance analysis showed that •O2– and h+ were the active species responsible for the oxidation reaction. The recycle experiment also proved that the catalyst has good stability. This work provides a new strategy for the design of photocatalysts for converting biomass into high-value chemicals.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Ning Shi,Yuju Zhu,Bangzhi Qin,Tianlang Zhu,Hongsheng Huang,Ying Liu
The production of 5-hydroxymethylfurfural (HMF) from cellulose is a crucial step in the production of high-value chemicals and fuels from renewable cellulosic biomass. In this study, the influences of the H2O/organic solvent ratio, the type of organic solvents, the addition of NaCl, and the type and concentration of catalysts on the catalytic conversion of cellulose into HMF in biphasic systems were comprehensively studied, and the highest HMF yield of 45.7% was obtained from cellulose in the H2O–tetrahydrofuran (THF) biphasic system with Al2(SO4)3 as the catalyst. Further investigation reveals that the excellent performance of the H2O–THF–Al2(SO4)3 reaction system was ascribed to the high Vorg/Vaque (60/1), high C[Al2(SO4)3]aque (0.38 g/mL), and low C[Al2(SO4)3]org (10–4 g/mL) of the reaction system. Moreover, the byproduct formed during the conversion of cellulose in the H2O–THF–Al2(SO4)3 reaction system was characterized by liquid chromatography–mass spectrometry (LC–MS) and LC–MS2 to detect considerable initial polymers. One plausible mechanism of glucose conversion in the H2O–THF biphasic system was proposed based on the detected compounds.
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GENE
·
2022
·
IF 3.913
Xiaohong Chen,Yueya Zhang,Haifeng Yan,Meiyun Niu,Yuping Xiong,Xinhua Zhang,Yuan Li,Jaime A. Teixeira da Silva,Guohua Ma
The commercial value of Santalum album L. lies in its aromatic heartwood and essential oil. Sesquiterpenes are the main components of sandal essential oil, and these are synthesized through the plant’s mevalonate (MVA) and methylerythritol phosphate (MEP) pathways. In this study, the first key rate-limiting enzyme, 1-deoxy- d -xylulose-5-phosphate synthase (SaDXS), was investigated to provide a theoretical molecular basis for the sandalwood MEP sesquiterpene biosynthetic pathway. The biofunctions of SaDXS were also analyzed. SaDXS promoters were successfully cloned from a seven-year-old S. album tree. SaDXS1A/1B promoter activity was verified by a β-glucuronidase (GUS) assay and by analyzing cis -acting elements of the promoters, which carried light- and methyl jasmonate (MeJA)-responsive signals. In an experiment involving yellow S. album seedlings, exposure to light upregulated SaDXS1A/1B expression and increased chlorophyll and carotenoid contents when overexpressed in Arabidopsis thaliana . Analysis of the expression of SaDXS1A/1B and SaSSy , key genes of santalol biosynthesis, revealed SaDXS1A expression in all tissues whereas SaDXS1B was expressed in tissues that contained photosynthetic pigments, such as stems, leaves and flowers. Sandal seedlings exogenously treated with two hormones, MeJA and ethylene, revealed similar expression patterns for SaDXS1A/1B and SaSSy . Sandal seedlings were treated with an inhibitor of DXS, clomazone, but showed no significant changes in the contents of α-santalene, β-santalene and α-santalol between treatment and control groups. These results suggest that SaDXS1A/1B play a role in the synthesis of sandalwood sesquiterpenes, providing carbon for downstream secondary metabolites. SaDXS1A/1B also play a role in the biosynthesis of chlorophyll, carotenoids, and primary metabolites.
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PubMed
高影响因子
FUEL
·
2022
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IF 8.035
Xiaopo Niu,Rong Zhao,Yunxi Han,Xiangwen Zhang,Qingfa Wang
Deep hydrogenation of polycyclic aromatic hydrocarbons is a feasible strategy to acquire high-performance aviation fuels, in which the key is to design highly active hydrogenation catalysts. Herein, hollow ZSM-5 (HZ) and silicalite-1 (HS) zeolites with hierarchical porous architectures were manufactured through a post-alkali treatment strategy, and further supported Pt to fabricate Pt/HZ-WI, Pt/HZ-SEA and Pt/HS-SEA catalysts employing wet impregnation (WI) and strong electrostatic adsorption (SEA) methods. The SEA catalysts presented higher metal dispersion, more election-deficient Pt δ+ species and stronger spillover hydrogen ability, thus resulting in better intrinsic hydrogenation properties in the deep hydrogenation reaction of phenanthrene than the WI ones. Moreover, Pt/HZ-SEA catalyst showed the supreme catalytic activity and the lowest activation energy of 52.11 kJ·mol −1 due to more hydrogenation active sites generated by the highly dispersed Pt clusters and the accelerated diffusion of reactants via the hierarchical porous architectures. Almost 100% selectivity to the deep hydrogenation products was achieved at rather low temperature of 220 °C. The Pt/HZ-SEA also displayed outstanding activity for hydrogenation of naphthalene, acenaphthylene and fluorene and excellent sulfur resistance. Furthermore, the acidic sites in HZ zeolite were favorable to boost the formation of electron-deficient Pt δ+ species having stronger deep hydrogenation ability and intensify the additional hydrogenation route through the spillover hydrogen. Finally, the DFT calculation results further verified that the Pt δ+ substances could heighten the adsorption of polyaromatics, thereby improving the deep hydrogenation activity.
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Frontiers in Chemistry
·
2022
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IF 5.545
Jia Hongyan,Lv Qing,Xia Qineng,Hu Wanpeng,Wang Yanqin
Efficient conversion of biomass-derived 5-hydroxymethylfurfural (HMF) to renewable fuels such as 2,5-dimethylfuran (DMF) and 2,5-dimethyltetrahydrofuran (DMTHF) is of significance for sustainable energy supply. For efficient catalyst design, it is important to understand the catalytic behavior and clarify the influence of physico-chemical properties of catalyst on reaction performance. Herein, to study the structure-activity relationships of monometallic Cu catalysts for HMF hydrogenolysis, a series of Cu/SiO2 catalysts with different physico-chemical properties were prepared and compared for their catalytic performance in HMF hydrogenolysis. It was found that Cu/SiO2-HT-8.5 catalyst prepared by hydrothermal method showed excellent activity in HMF hydrohydrolysis reaction. Under the optimal reaction condition, the total yield of liquid fuels reaches 91.6% with 57.1% yield of DMF and 34.5% yield of DMTHF in THF solvent. Characterizations such as XRD, H2-TPR, N2-adsorption/desorption, TEM and XPS revealed that the Cu particles in the Cu/SiO2-HT-8.5 catalyst have uniform size and high dispersion. The Cu species and the SiO2 support have relatively weak interaction and are easy to be reduced to Cu0, which makes it show excellent activity in the hydrogenolysis of HMF.
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高影响因子
FUEL
·
2022
·
IF 8.035
Chenyao Bi,Zhuangzhuang Zhang,Daizong Han,Chengan Wang,Jianbo Zhang,Ming Sun,Qingqing Hao,Huiyong Chen,Xiaoxun Ma
Quality improvement of pyrolysis tar with yield increasing of high value-added components is highly desired for coal utilization. Herein, Ga-impregnated mesoporous ZSM-5 (Ga/MZ5) directed by organosilane surfactant of [3-(trimethoxysilyl) propyl] octadecyldimethylammonium chloride (TPOAC) is used as a catalyst for the catalytic upgrading of coal pyrolysis volatiles. Effective regulation by reduction and reduction/reoxidation promotes a secondary dispersion of gallium species from external surface deposition to micropore permeation. The comprehensive evaluation of catalytic upgrading performance indicates that the designedly regulated gallium species (mainly Ga + , GaH 2 + and GaO + ), feasible balance of Brønsted and Lewis active sites and mesopore diffusion superiority effectively contribute the yield increasing of both light-fraction ( M LF / M Tar ) and target products of BTEXN (benzene, toluene, ethylbenzene, xylene and naphthalene). The optimal catalyst of Ga/MZ5_R/O exhibited the highest value of M LF / M Tar (88 %) and highest yield of BTEXN (31.84 mg.g −1 ), which are 173 and 589 % higher than non-catalytic single pyrolysis and 133 and 280 % higher than those over the conventional Ga-impregnated ZSM-5 (Ga/Z5). Moreover, the possible reaction networks towards high value-added products of BTEXN based on the positive conversion of polycyclic aromatic hydrocarbons (PAHs), phenols, and other oxygen-containing compounds (abbreviated as PPO) is further proposed.
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Frontiers in Chemistry
·
2022
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IF 5.545
Zhao Kangyu,Xiang Yanping,Sun Xiaoao,Chen Linjiao,Xiao Jiafu,Liu Xianxiang
In this study, a novel sulfonic acid-modified catalyst for MOFs (UIO-66-SO3H) was synthesized using chlorosulfonic acid as a sulfonating reagent and first used as efficient heterogeneous catalysts for the one-pot conversion of fructose into biofuel 5-ethoxymethylfurfural (EMF) in a cosolvent free system. The physicochemical properties of this catalyst were characterized by Fourier transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), and powder X-ray diffraction (XRD). The characterization demonstrated that the sulfonic acid group was successfully grafted onto the MOF material and did not cause significant changes to its morphology and structure. Furthermore, the effects of catalyst acid amount, reaction temperature, reaction time, and catalyst dosage on reaction results were investigated. The results showed that the conversion of fructose was 99.7% within 1 h at 140°C, while the EMF yield reached 80.4%. This work provides a viable strategy by application of sulfonic acid-based MOFs for the efficient synthesis of potential liquid fuel EMF from renewable biomass.
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高影响因子
JOURNAL OF FOOD PROCESSING AND PRESERVATION
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2022
·Vol. 46
·期 5
·e16582
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IF 2.609
Hua Yang,Xuexue Chen,Xiaomin Li,Dianhui Wu,Guolin Cai,Jian Lu
The effects of ascorbic acid (VC), reduced glutathione (GSH), sulfur dioxide (SO 2 ), chitosan, and ethylenediaminetetraacetic acid disodium (EDTA-2Na) on the color parameters of Dangshan pear wine during storage were investigated. The different addition amounts of VC and EDTA-2Na increased the browning degree of pear wine, and chitosan had a weak inhibitory effect on the browning of pear wine. The addition of 0.01%, 0.05%, and 0.10% GSH reduced the browning degree of pear wine by 8.80%, 13.82%, and 5.02%, respectively; 0.05% GSH decreased the color saturation and increased the brightness during the storage of pear wine. Adding 0.05% and 0.10% SO 2 reduced the browning degree of pear wine by 14.73% and 21.05%, respectively, the inhibitory effect for browning was significant, 0.10% SO 2 reduced the brightness of pear wine during storage. This result showed that GSH and SO 2 were the most effective candidate inhibitors for Dangshan pear wine browning. Novelty impact statement The addition of 0.05% GSH reduced the browning degree of pear wine by 13.82%. Adding 0.10% SO2 reduced the browning degree of pear wine by 21.05%. GSH and SO2 were the most effective inhibitors for Dangshan pear wine browning.
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ACS Omega
·
2022
·
IF 4.132
Huan Zhou,Wenwen Lin,Chao Chen,Chuang Liu,Jianghua Wu,Jianghao Wang,Jie Fu
As an essential chemical feedstock, aromatics can be obtained from biomass by catalytic fast pyrolysis (CFP) technology, in which diffusion limitation is still a problem. In this study, several ZSM-5 zeolites with intercrystal stacking macropores were synthesized by adding organosilanes (OSAs) with different alkyl chain groups. Due to the structure-directing effect of the OSA, the prepared ZSM-5 zeolites possess a larger external surface area and pore volume than Blank-Z5. Moreover, the pore size is related to the extent of anchoring of the OSA and silicon–aluminum species in the zeolite precursor. Pyridine Fourier transform infrared (Py-FTIR) and NH3-temperature-programmed desorption (TPD) analyses show that the obtained ZSM-5 zeolites have a higher Brønsted acidity and total number of acid sites. In addition, excessive addition of OSA is not conducive to the growth of ZSM-5 zeolites. The catalytic performance of the synthesized ZSM-5 zeolites was evaluated by Py-GC/MS. The larger external surface area and pore volume improve the accessibility of the acid sites and thus promote the conversion of biomass into aromatics.
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高影响因子
PROGRESS IN ORGANIC COATINGS
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2022
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IF 6.206
Mengqin Li,Mei-jin Lin,Yuezhong Meng,Dongyang Chen
To expand the properties of epoxy coatings for emerging technologies, herein, a pillar[5]arene-based epoxy compound (PAEP) containing unique pillar-shaped three dimensional macrocyclic structure was prepared and cured with conventional 4,4′-diaminodiphenylmethane (DDM). Interestingly, the PAEP exhibited a strong host-guest complexation with 1,4-dibromobutane (DBrBu), a potential organic antibacterial agent, with a complex constant of 215.7 ± 11.02 M −1 . Furthermore, the PAEP/DDM resin possessed enhanced mechanical and thermal properties, probably due to the increase of chain-entanglement brought about by the cyclic structure. Also, the PAEP/DDM resin exhibited excellent intrinsic flame retardant properties, including significantly reduced peak heat release rate (153.5 W·g −1 ) and high limit oxygen index (LOI) (34.7%), and a V-0 rating in the UL-94 test. Moreover, the PAEP/DDM resin exhibited a remarkably low dielectric constant of 2.25 at 10 6 Hz for telecommunication applications, which is much lower than the current epoxy resins with nanoporous inorganic modifiers. Therefore, the incorporation of pillar[5]arene is a fruitful pathway to expand the properties of epoxy resins and provides a new platform for decoration for various applications.
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CATALYSIS LETTERS
·
2022
·Vol. 152
·期 11
·3400-3413
·
IF 2.936
Xia Jing,Gao De,Han Feng,Li Yan,Waterhouse Geoffrey I. N.
Currently, there is tremendous interest in the discovery of efficient and low-cost catalysts for the selective hydrogenation of biomass-derived 5-hydroxymethylfurfural (HMF) to the biofuel 2,5-dimethylfuran (DMF). In this study, a CoNC x /NiFeO catalyst was synthesized by the adsorption of cobalt (II) phthalocyanine (CoPc) on ultrathin NiFe-layered double hydroxide nanosheets (NiFe-LDH), followed by mild pyrolysis of the resulting CoPc/NiFe-LDH composite at 550 °C under N 2 for 5 h. XRD, TEM and XPS showed CoNC x /NiFeO to contain CoO x /Co 0 and Ni 0 nanoparticles on a NiFe-mixed metal oxide support. CoNC x /NiFeO showed very high initial activity and selectivity for the hydrogenation of HMF to DMF in tetrahydrofuran (THF) under mild reaction conditions (180 °C, 1.0 MPa H 2 , 6.0 h), evidenced by a 99.8% HMF conversion and 94.3% DMF selectivity. Reaction pathways for the conversion of HMF to DMF over CoNC x /NiFeO were revealed by monitoring the intermediates formed at different stages of the reaction. Graphical Abstract In this study, a CoNC x /NiFeO catalyst was synthesized by the adsorption of cobalt (II) phthalocyanine (CoPc) on ultrathin NiFe-layered double hydroxide nanosheets (NiFe-LDH), which showed very high initial activity and selectivity for the hydrogenation of HMF to DMF.
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CELLULOSE
·
2022
·Vol. 29
·期 3
·1419-1433
·
IF 6.123
Huang Ting,Zhou Yaohong,Zhang Xiaohua,Peng Dayong,Nie Xuliang,Chen Jing,Xiong WanMing
A furfuryl alcohol resin-based solid acid (SC-FAR-800) was prepared and applied in the conversion of carbohydrates into furan platform compounds in microwave. The results showed that SC-FAR-800 was an irregular mesoporous material containing sulfonic acid groups with an acid density of 3.43 mmol/g, which was quite stable below 200 °C. SC-FAR-800 showed good catalytic activity, and the yield of furfural from xylose could reach 60.46%; the yield of 5-HMF from fructose, glucose, cellobiose and cellulose macromolecules could reach 89.35%, 38.17%, 42.6%, 14.73%, respectively. However, the effect of reaction temperature, reaction time, catalyst dosage and water content on various carbohydrate’s conversion was different. SC-FAR-800 could be reused more than 6 times in fructose conversion, and could be regenerated after a re-sulfonation process. Moreover, the catalytic activity of SC-FAR-800 was super to some biomass-based solid acid. Therefore, this catalyst may be an attractive alternative in the conversion of biomass to prepare furan compounds. Graphical abstract Furfuryl alcohol resin-based solid acid (SC-FAR-800), which has a high acidity of 3.43 mmol/g, was applied in the conversion of carbohydrates in a microwave oven. The peak yield of furfural from d -xylose could reach 60.46%; the yield of 5-HMF from d -fructose, glucose, cellobiose and cellulose macromolecules could reach 89.35%, 38.17%, 42.6%, 14.73%, respectively.
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危险品化学品经营许可证（带存储）