ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Dazhen Xiong,Yang Wang,Huihui Ma,Lige Lu,Qian Zhang,Yunlei Shi,Yang Zhao,Jianji Wang
5-Hydroxymethylfurfural (HMF) is a key biobased platform compound for the production of high-value chemicals and fuels. However, separation and purification of HMF is currently the bottleneck for HMF production. In this work, a novel class of temperature-responsive deep eutectic solvent (DES)–water systems have been explored to selectively separate HMF from reaction mixtures. The fructose dehydration reaction was conducted in homogeneous DES–H2O systems, and then, the produced HMF was migrated to the DES-rich phase while the unreacted fructose was retained in the H2O-rich phase upon cooling. Thus, selective separation of HMF was realized. It was found that water–water and DES–DES interactions predominate over DES–water interactions during cooling, thus resulting in upper critical solution temperature phase separation. Under optimal conditions, the partition coefficient and separation factor of HMF could reach up to 78 and 609, respectively, which is about 5 and 13 times those reported in ionic liquid-based aqueous biphasic systems. Furthermore, HMF could be removed from the DES-rich phase, giving a high recovery efficiency of 69%, which is much higher than the best value reported in the literature. At the same time, DES was regenerated and reused in the next process, and no obvious decrease in partition coefficient of HMF was observed after six cycles.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Z.W. Zhu,Q.R. Zheng
Comparisons were made between the samples mechanochemically (MOF-5(M)) and solvothermally (MOF-5(S)) prepared for the development of efficient hydrogen storage medium. Synthesized samples were undergone structural characterization as well as adsorption equilibrium measurements of hydrogen at temperature-pressure range 77 K–87 K and 0.1–10 MPa. Grand Canonical Monte Carlo (GCMC) simulations were further conducted to study the behaviors of hydrogen molecules adsorbed on MOF-5. It shows that, besides the advantage of large scale synthesis and a lower cost, mechanochemical method respectively brings about 207% and 90.5% increments in the specific surface area and the maximum excess adsorption capacity of hydrogen at 77 K within pressure range 0–10 MPa. Results also reveal that the crystal within MOF-5(M) is regular and distributing uniformly with a mean size only one tenth of that of the MOF-5(S); at 77 K within pressure range 0–10 MPa, Toth equation can predict the adsorption equilibrium data of hydrogen on two MOF-5 samples with a mean relative error less than 1.5%. It suggests that MOF-5(M) is more promising for hydrogen storage by adsorption for practical applications.
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Niuniu Zhu,Manyu Zhang,Guo Qiu,Hongyu Tian,Yongguo Liu
The synthesis of platform chemical 5-hydroxymethylfurfural (5-HMF) provides favorable and efficient paths for the utilization of renewable biomass resources. In this work, highly active niobium-modified montmorillonite (Nb-Mont) catalysts were synthesized by a facile and ion-exchange method and were used for the one-pot conversion of cellobiose and sucrose to 5-HMF with optimal results. 5-HMF yield of 68.6% was obtained from cellobiose in a methyl isobutyl ketone (MIBK)/saturated salt water (SSW) biphasic solvent at 170 °C after 3 h. With sucrose as substrate in DMSO at 140 °C after 2 h, 5-HMF yield was 65.4%. The presence of Lewis and Brønsted acid sites on Nb-Mont facilitate the hydrolysis of cellobiose and sucrose and play essential roles in the subsequent isomerization of glucose monomer and the dehydration of fructose monomer. A possible reaction mechanism was proposed for the transformation of cellobiose and sucrose into 5-HMF, and the isomerization process of glucose monomer was the most critical step, confirmed by density functional theory (DFT) calculations. [NbO(OH) 2 ] + species as active sites could effectively reduce the activation energy of the isomerization process, which accelerated the synergetic proton transfer process. Nb-Mont was recycled at least four times without a prominent loss in the catalytic activity. In this study, a promising catalytic strategy was provided for heterogeneous Nb containing catalysts used in the effective synthesis of 5-HMF from carbohydrates.
✓ 已验证
产品关联
DOI
高影响因子
CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2022
·Vol. 101
·期 6
·3234-3245
·
IF 2.5
Luxin Zhang,Meng Hu,Ruijun Sun,Xu Xing
The production of 5-ethoxymethylfurfural (EMF) from cheap and abundant glucose feedstock has attracted a great deal of attention because of its potential applications. Herein, three porous tetra-component metal oxide solid acid catalysts (SO 4 2− /ZFSA-A, SO 4 2− /ZFSA-F-10, SO 4 2− /ZFSA-F-20) containing both Brønsted and Lewis acid sites have been successfully synthesized and can efficiently catalyze the synthesis of EMF from glucose. Particularly, the SO 4 2− /ZFSA-A, SO 4 2− /ZFSA-F-10, and SO 4 2− /ZFSA-F-20 catalysts were prepared under the template of sodium alginate, 10% F127, and 20% F127, respectively. The prepared catalysts were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), N 2 -adsorption–desorption isotherm, X-ray photoelectron spectroscopy (XPS), thermogravimetry (TG), temperature-programmed desorption of ammonia (NH 3 -TPD), and pyridine infrared spectra (Py-FTIR). The characterization results indicated that all three catalysts have a porous structure. The pore distribution of the SO 4 2− /ZFSA-A catalyst is mainly macroporous and mesoporous, while the SO 4 2− /ZFSA-F-10 and SO 4 2− /ZFSA-F-20 catalysts are mainly mesoporous. The SO 4 2− /ZFSA-F-20 catalyst exhibited the highest catalytic performance due to its large specific surface area, desirable mesoporous structure, high total acidity (especially strong and super strong acidity), and appropriate Lewis/Brønsted acid ratio. By applying SO 4 2− /ZFSA-F-20, the formation of EMF from glucose was successfully catalyzed and EMF was obtained at a yield of 34.56% after 12 h at 160°C. This yield is much higher compared with most other results achieved by solid acids catalysis. In addition, the reaction parameters such as reaction temperature, reaction time, glucose amount, and catalyst dosage were shown to have a significant effect on the catalytic performance. Notably, the SO 4 2− /ZFSA-F-20 catalyst exhibited good reusability, as its activity did not significantly diminish after four rounds of repeated experiments and was successfully reactivated after calcination.
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Cellular and Infection Microbiology
·
2022
·
IF 6.073
Yin Lujun,Shen Wang,Liu Jun-Sheng,Jia Ai-Qun
Siderophore is necessary for the survival of microorganisms and is interregulated with quorum sensing (QS) systems. It is related to growth, proliferation, virulence, and other bacterial social activities as a virulence factor. Thus, we speculated that the QS system could be occluded by inhibiting siderophore production. 2-Hydroxymethyl-1-methyl-5-nitroimidazole (HMMN), one siderophore inhibitor of Pseudomonas aeruginosa PAO1 (P. aeruginosa PAO1), was obtained by using the Chromeazurol S (CAS) method. We found that HMMN inhibited siderophore production and influenced the biological effects of QS regulation, including biofilm formation and pyocyanin production. HMMN (150 μg/ml) inhibited the siderophore production of P. aeruginosa PAO1 by 69.37%. In addition, HMMN could inhibit pyocyanin production and biofilm formation and erase the formed biofilm of P. aeruginosa PAO1. HMMN (150 μg/ml) inhibited the biofilm formation of P. aeruginosa PAO1 by 28.24%. The erasure rate of the formed biofilm reached 17.03%. Furthermore, HMMN (150 μg/ml) inhibited P. aeruginosa PAO1 pyocyanin production by 36.06%. Meanwhile, positive-control hordenine (500.0 μg/ml) reduced the biofilm formation and pyocyanin production of P. aeruginosa PAO1 by 14.42% and 34.35%, respectively. The erasure rate of hordenine to the formed biofilm is 11.05% at 500 μg/ml. Quantitative real-time polymerase chain reaction (qRT-PCR) showed that HMMN downregulates not only siderophore-related genes but also QS-related genes, as well as hordenine. These results suggest that a siderophore inhibitor could be used as a QS inhibitor to occlude the QS system and reduce virulence.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Xusheng Guo,Haoxiang Zhu,Yuxi Si,Heng Ban,Xilei Lv,Youwei Cheng,Lijun Wang,Xi Li
Converting carbohydrates to 5-hydroxymethylfurfural (HMF) is an important goal for biorefinery. Although various deep eutectic solvents (DESs) have been reported for HMF production, the field lacks systematic research on the effect of cations and anions and an effective catalytic system for converting concentrated carbohydrates. Here, 12 kinds of DESs containing four cations and six anions were systematically evaluated and tetraethylammonium bromide (TEAB) was confirmed as the most effective DES, which provided HMF yields of 90 and 76% from fructose and glucose, respectively. The stable bromide-substituted intermediate may explain the positive effect of bromide based on the results of density functional theory calculation. A high concentration substrate has an adverse impact on the selectivity of HMF due to the HMF concentration caused by glucose, CrCl3·6H2O, and concentrated HMF. To inhibit the condensation, a biphasic system of TEAB/THF is developed to convert a highly concentrated glucose of 62.5 wt % (83.3 wt % with respect to TEAB), providing an excellent HMF yield of 72%. This study has revealed the impact of cations and anions of DESs on HMF production, which will serve as a base for designing task-specific DESs. Moreover, an efficient catalytic system to produce HMF from concentrated glucose was also provided.
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Xiaocui Wei,Yanan Liu,Yang Cao,Jin Li,Xianghao Meng,Zhao Zhang,Zhongyi Jiang
The catalytic pyrolysis of biomass is a sustainable approach for biofuel production, contributing to replacing fossil resources with renewable resources . The ZSM-5 zeolite remains an attractive catalyst in the catalytic pyrolysis of biomass, and how to reduce the product diffusion resistance and regulate the surface acidity of ZSM-5 should be explored more deeply. Herein, a hierarchical gallium-modified ZSM-5@SBA-15 catalyst is fabricated through coating a mesoporous layered SBA-15 shell on a hollow ZSM-5 core with gallium modified on the surface, which is effective for increasing hydrocarbon production during the catalytic pyrolysis of biomass process. The synergistic effect of hollowness, mesoporosity, and activity in the hierarchical gallium-modified ZSM-5@SBA-15 catalysts is found to affect the yield and quality of bio-oil. Accordingly, the hierarchical gallium-modified ZSM-5@SBA-15 catalyst with 11 wt% Ga loading exhibits a superior deoxygenation ability, and the relative content of hydrocarbons in bio-oil reach to 49.76 area% which is much higher than that of ZSM-5 (35.30 area%). Furthermore, a possible catalytic pyrolysis mechanism of biomass was also proposed to clarify the potential application of hierarchical gallium-modified ZSM-5@SBA-15 catalysts.
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2022
·
IF 5.089
Wenpeng Han,Shujuan Wang,Yajie Liu,Chaoqun Li,Ningning Yuan,Ligong Zhou,Mingxing Tang,Hui Ge
The transformation of biomass to liquid fuels and chemicals is of great interests. Herein, a series of reduced NiZn-CT (CT represents calcination temperature) catalysts with flower-like morphology and uniform particle sizes were prepared by co-precipitation method and used for hydrogenolysis of 5-hydroxymethylfural (HMF) to 2,5-dimethyfuran (DMF). The characterizations evidenced the formation of NiZn alloy phase in the catalysts through the strong metal-support interaction (SMSI), which had high C-O hydrogenolysis ability. The synergy of hydrogenation and C-O hydrogenolysis is essential for HMF to DMF, and we surprisingly found that this synergistic effect can be achieved just by controlling calcination temperature to regulated SMSI between Ni and ZnO. By this way, 99% DMF yield was gained at 180 °C for 4 h under 2 MPa H 2 over reduced NiZn-450 catalyst. More importantly, the active centers of this Ni/ZnO catalyst exhibited outstanding stability. There was no significant decrease in activity after reusing 9 times. The current research provided an easy-made catalytic system for HMF hydrogenolysis.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2022
·
IF 2.719
Xiaoli Song,Yuxiu Fu,Yaming Pang,Liguo Gao
La and Zn species were used to modify HZSM-5 zeolite, which was used to treat phenol in wastewater. Through the combination of multiple direct tools, La and Zn species were successfully loaded into the HZSM-5 zeolite. La-Zn/HZSM-5 zeolite has a small band gap and the catalyst can produce highly active electrons and electron holes when energy enters. The HZSM-5 zeolite after modification improves activity and stability of the catalyst. Therefore, it has a significant effect in the phenol removal experiment. Adding 1.2 mL of hydrogen peroxide and 0.11 g of catalyst, the removal rate can reach 99.38 % after being irradiation with a mercury lamp at 60 °C for 180 min. La-Zn/HZSM-5 zeolite has great potential in the application of photocatalytic degradation of phenol.
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2022
·Vol. 2022
·期 24
·e202200260
·
IF 2.551
Guang Xiong,Shengyang Zhou,Liping Liu,Ji Qian,Jiaxu Liu,Leping Zhao
Graphical Y/ZSM-5 composite zeolite was synthesized by an aerosol-assisted hydrothermal method including a two-step crystallization. The structure and acidity of the composite zeolite can be modulated by monitoring the synthesis conditions. Y/ZSM-5 composite zeolite was synthesized by an aerosol assisted hydrothermal method including a two-step crystallization. The aerosol technique was used to prepare the precursor of Y/ZSM-5 composite zeolite. This helped to fully utilize the amorphous silica-alumina species left in the primary crystallization solution of NaY zeolite, and to bring the two zeolites close to each other during the second crystallization step. The optimal adding sequence and synthesis conditions were investigated to reduce the amount of template and accelerate the crystallization rate. The composite zeolites were analyzed using XRD, SEM, nitrogen physical adsorption, NH 3 -TPD techniques. It was found that the acid properties can be adjusted by modulating the SiO 2 /Al 2 O 3 molar ratio of the secondary crystallization feed. The BET specific surface area of the optimal Y/ZSM-5(20) composite zeolite is 502 m 2 /g, the pyrolysis conversion rate of 1,3,5-triisopropylbenzene reaches 95.1 %, and the selectivity to benzene reaches 53.4 %.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Zixuan Ma,Fenghai Cao,Yuhao Yang,Liyan Wang,Tao Zhang,Minghui Tan,Guohui Yang,Yisheng Tan
Bifunctional catalysts composed of ZnCrO x oxide and ZSM-5 were widely used in syngas-to-aromatics (STA). The CO conversion on bifunctional catalysts was generally higher than that on oxide catalysts attributed to the pulling effect of zeolite, but the key factor for the improvement of CO conversion was still short of systematical explanation. In this work, the degree of nonstoichiometric spinel of ZnCrO x (ZxC) oxides was finely tuned through modulating the ratio of Zn/Cr, which could significantly influence the catalytic behaviors of ZnCrO x /ZSM-5 catalysts for the CO hydrogenation to aromatics. The increase of nonstoichiometric spinel corresponded to the increase of oxygen vacancies and the enhancement of Zn-Cr synergistic effect, which promoted the activation of H 2 and CO, leading to a dramatic increase of CO conversion. The work revealed that the action of ZnO and oxygen vacancies was the key factor for CO pulling in ZnCrO x oxide and ZSM-5 catalyzed STA reaction.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2022
·Vol. 105
·期 11
·6816-6825
·
IF 4.186
De-Bao Liu,Bao-Lu Shi,Yi-Guang Wang,Bao-Sheng Xu
In this work, we have prepared a novel yttria-stabilized zirconia fiber (YSZ f )-reinforced (La 1/5 Nd 1/5 Sm 1/5 Gd 1/5 Yb 1/5 ) 2 Zr 2 O 7 porous ceramics (YSZ f /(5RE 1/5 ) 2 Zr 2 O 7 PCs) through a foam-gelcasting-freeze drying process. The microstructure, phase composition, density, porosity, thermal conductivity, and compressive strength of the as-prepared YSZ f /(5RE 1/5 ) 2 Zr 2 O 7 PCs were systematically investigated. In addition, the high-temperature thermal cycle stability and thermally insulating property of the samples were also tested. The results indicated that the as-synthesized YSZ f /(5RE 1/5 ) 2 Zr 2 O 7 PCs (with 25 wt% YSZ fibers) exhibited high porosity, high compressive strength, low thermal conductivity as well as low thermal cycling shrinkage. This work demonstrated that the added YSZ fiber can remarkably improve the strength of (5RE 1/5 ) 2 Zr 2 O 7 PCs with the high porosity, and as-developed YSZ f /(5RE 1/5 ) 2 Zr 2 O 7 PCs would be an excellent candidate for high-temperature thermal insulator materials.
✓ 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）