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Waste and Biomass Valorization · 2016 ·Vol. 9 ·期 1 ·95-101 · IF 0.915

The Efficient Oxidation of Biomass-Derived 5-Hydroxymethyl Furfural to Produce 2,5-Diformylfuran Over Supported Cobalt Catalysts

Ning Liangmin,Liao Shengyun,Sun Yongfa,Yu Linhao,Tong Xinli

Abstract The catalytic synthesis of 2,5-diformylfuran (DFF) from 5-hydroxymethylfurfural (HMF) attracts extensive attention in the research of biomass conversion. However, it is a challenge to achieve high conversion of HMF under mild conditions with a heterogeneous catalyst, which can be easily separated and recycled. Herein, we report a novel cobalt-based catalyst (Co x O y -N@TiO 2 ) for the oxidation of HMF to DFF with 30 % aqueous tert -butyl hydroperoxide as the oxidant. A series of Co-based catalysts were prepared by a typical impregnation method, and detected by XRD, TEM and FT-IR techniques. Based on the experimental results of catalytic test, it is found that a 91 % conversion of HMF and 40 % selectivity of DFF was obtained with the Co x O y -N@TiO 2 catalyst at 80 °C within 5 h. In addition, the Co x O y -N@TiO 2 can be recycled up to five times without significant loss of activity. Graphical Abstract The efficient oxidation of 5-hydroxymethyl furfural, a biomass-derived platform compound, to produce 2,5-diformylfuran is achieved using Co x O y -N@TiO 2 catalyst under mild conditions.

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RSC Advances · 2017 ·Vol. 7 ·期 23 ·13808-13816 · IF 3.108

Effects of nitroguanidine on the thermal behavior and burning characteristics of 5-amino-1H-tetrazole-based propellants

Cheng-Yang Cao,Song Lu,Dan Zhang,Lun-Lun Gong,He-Ping Zhang

The 5AT/Sr(NO3)2 mixture has recently attracted attention as a gas-generating agent for use in novel fire-suppression applications. However, it cannot provide the desired combustion behavior alone. Thus, nitroguanidine (NQ) was added as a fuel component to 5AT/Sr(NO3)2 in attempt to improve the mixture's combustion behavior. The effects of NQ on the thermal and burning characteristics of 5AT/Sr(NO3)2 were investigated. Thermogravimetry-differential scanning calorimetric (TG-DSC) analysis with four heating rates (5, 10, 15, 20 K min−1) under a nitrogen atmosphere was performed to determine the thermal characteristics and non-isothermal reaction kinetic parameters. The addition of NQ decreases the activation energy of the Stage II and III decomposition reaction, and accelerates the redox reaction and decomposition of Sr(NO3)2. Thermodynamic calculations and measurements of temperature profile and liner burning rates were performed to evaluate the combustion characteristics. Adding NQ decreased the adiabatic combustion temperature, outlet temperature, average flame height, flame oscillation frequency and pressure exponent of Vieille's equation, and increased the gas output and linear burning rate. Notably, mesa burning occurred when NQ was added, the mechanism of which is elaborated using a physical combustion model. The analysis deepens the understanding of when the gas-phase or condensed-phase reactions control the burning characteristics of the composite propellant.

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ACS Sustainable Chemistry & Engineering · 2016 · IF 5.267

Basicity-Tuned Hydrotalcite-Supported Pd Catalysts for Aerobic Oxidation of 5-Hydroxymethyl-2-furfural under Mild Conditions

Yanbing Wang,Kai Yu,Da Lei,Wei Si,Yajun Feng,Lan-Lan Lou,Shuangxi Liu

An environmentally benign and homogeneous base-free route for 5-hydroxymethyl-2-furfural (HMF) aerobic oxidation to 2,5-furandicarboxylic acid (FDCA) in water was reported using Mg–Al–CO3 hydrotalcite-supported Pd nanoparticles (xPd/HT-n) as catalyst. The influences of the Mg/Al molar ratio of hydrotalcite and Pd loading amount on the catalytic performance of these catalysts were originally systematically investigated. These catalysts exhibited excellent catalytic activity and FDCA selectivity in the HMF oxidation, especially for 2%Pd/HT-5 and 2%Pd/HT-6; >99.9% FDCA yields were achieved for 8 h under ambient pressure and homogeneous base-free conditions. The remarkably improved catalytic performance could be attributed to the suitable basicity of the Mg–Al–CO3 hydrotalcite and the abundant OH– groups on the surface of hydrotalcite. The plausible reaction mechanism was proposed based on the results of a series of controlled experiments. Furthermore, these catalysts were quite stable and could be reused at least five times without obvious loss in reaction activity.

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INTERNATIONAL BIODETERIORATION & BIODEGRADATION · 2016 · IF 2.429

Enhanced biodegradation of di-n-butyl phthalate by Acinetobacter species strain LMB-5 coated with magnetic nanoparticles

Jing Wang,Li-Hua Jiang,Ying Zhou,Bang-Ce Ye

Phthalate acid esters (PAEs) are widely present in a variety of consumer products and they pose a public health concern due to the high mobility and hazards. In this study, we designed an immobilized method to eliminate phthalates by using Fe 3 O 4 @NH 2 nanoparticles (NPs). The surface-modified NPs showed a good dispersion property, and the particle size was approximately 230 nm. The results showed that Acinetobacter sp. strain LMB-5 could be coated by the prepared magnetic particles allowing easy separation from solution by applying an external magnetic field. The coated cells possessed adaptability to a wide range of pH and high tolerance towards toxic substances. More importantly, when the temperature was elevated to 60 °C, the coated cells also exhibited remarkable degradability . There was no change in the main metabolites during the biodegradation between the free cells and immobilized ones through GC/MS analysis to detect the degradation intermediates. These results show that immobilization method using magnetic nanoparticles is a promising way for degradation of phthalates in application.

CAS / MDL: 1317-61-9
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2024 · IF 3.7

Cost-effective bifunctional lignin-derived carbon supported tin oxide with efficient production of 5-hydroxymethylfurfural from glucose

Sien Yan,Linhuo Gan,Kui Wang,Kang Sun

5-Hydroxymethylfurfural (5-HMF) is one of the important bio-based platform compounds, and the catalytic conversion of glucose to 5-HMF is a highly desirable approach that is receiving increasing attention. Herein, we reported the synthesis of lignin-derived carbon supported tin oxides (SnO x /LC) catalyst via a two-step hydrothermal-pyrolytic method using wheat straw alkali lignin as a cost-effective carbon source with high carbon content. The key preparation conditions of catalyst and its catalytic conditions for the conversion of glucose to 5-HMF were investigated, respectively. Results show that under the preparation conditions of tin tetrachloride dosage of 3.0 mmol and pyrolysis temperature of 500°C, the optimized catalyst (3.0-SnO x /LC-500) with a high yield of 63.4% exhibits good catalytic performance of 5-HMF yield of 50.1% and reaction selectivity of 86.0% under the optimum conditions of reaction temperature and time of 190°C and 3 h, initial glucose concentration of 10 wt%, 3.0-SnO x /LC-500 dosage of 100 mg in a biphasic solvent system of volume ratio of water to tetrahydrofuran of 1:4. In addition, 3.0-SnO x /LC-500 exerts an excellent reusability in five-cycle experiment. Furthermore, SnO x /LC was characterized in detail using X-ray diffraction patterns (XRD), X-ray Photoelectron Spectroscopy (XPS) Brunauer-Emmett-Teller (BET), ammonia temperature-programmed-desorption (NH 3 -TPD), pyridine adsorption infrared spectroscopy (Py-FTIR), scanning electron microscope (SEM) and thermal gravimetric analysis (TGA). Results indicate that Brønsted acid sites and Lewis acid sites coexist on 3.0-SnO x /LC-500, and more Sn 4+ as well as proper ratio of weak acidity to medium acidity are conductive to its catalytic performance in glucose-to-5-HMF reaction.

CAS / MDL: 50-99-7 67-47-0
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CHINESE JOURNAL OF CATALYSIS · 2024 · IF 15.7

Dual-metal synergy unlocking ROS-free catalysis for rapid aerobic oxidation of 5-hydroxymethylfurfural at room temperature

Meiyun Zhang,Penghua Che,Hong Ma,Xin Liu,Shujing Zhang,Yang Luo,Jie Xu

Clean catalytic oxidation has a broad prospect in the modern chemical engineering and energy chemistry fields. However, unexpected over-oxidation and disruptive degradation are frequently induced by excessive reactive oxygen species (ROS). Herein, we reported a new ROS-free approach to effectively drive O 2 to be activated into highly reactive surface peroxo species through enzyme-mimicking mechanism. Benefiting from the dual-metal synergy effect between Cu and Co active sites, ROS (H 2 O 2 and OH • ) is generated in situ while further scavenged completely into surface peroxo species, which gives rise to very high selectivity and extremely high carbon balance. For example, the CuCo/N-C catalyst affords >99.8% conversion and 94.5% selectivity to 2,5-furanedicarboxylic acid at 25 °C for 6 h in the aerobic oxidation of biomass platform 5-hydroxymethylfurfural. Moreover, it achieved exceptional performance in the oxidation of a variety of hydroxyl compounds to organic acids with high yields (89.9%–99.5%) at a mild temperature (25–40 °C). This exploration introduces an innovative clue for emulating enzyme catalysts, thereby enriching our comprehension and advancement of biologically inspired catalytic oxidations.

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ANTIVIRAL RESEARCH · 2024 · IF 4.5

Drug delivery system based on metal-organic framework improved 5-Fluorouracil against spring viremia of carp virus

Liang Zhao,Wei-Ze Wang,Tian-Tian Jiang,Tian-Zi Sun,Bo Liu,Bin Zhu

Spring viremia of carp virus (SVCV), as a high pathogenicity pathogen, has seriously restricts the healthy and sustainable development of cyprinid farming industry. In this study, we selected 5-Fluorouracil (5-Fu) as the drug model based on zeolitic imidazolate framework-8 (ZIF-8) to construct a drug delivery system (5-Fu@ZIF-8), and the anti-SVCV activity was detected in vitro and in vivo . The results showed 5-Fu@ZIF-8 was uniform cubic particle with truncated angle and smooth surface, and the particle size was 90 nm. The anti-SVCV activity in vitro results showed that the highest inhibition rate of 5-Fu was 77.93% at 40 mg/L and the inhibitory concentration at half-maximal activity (IC 50 ) was 20.86 mg/L. For 5-Fu@ZIF-8, the highest inhibition rate was 91.36% at 16 mg/L, and the IC 50 value was 5.85 mg/L. In addition, the cell viability was increased by 18.1% after 5-Fu treatment. Similarly, after 5-Fu@ZIF-8 treatment, the cell viability increased by 27.3%. Correspondingly, in vivo experimental results showed the viral loads reduced by 18.1% on the days 7 and the survival rate increased to 19.4% at 80 mg/L after 5-Fu treatment. For 5-Fu@ZIF-8, the viral loads reduced by 41.2% and the survival rate increased to 54.8%. Mechanistically, 5-Fu inhibits viral replication by regulating p53 expression and promoting early apoptosis in infected cells. All results indicated that 5-Fu@ZIF-8 improved the anti-SVCV activity; it may be a potential strategy to construct a drug-loaded system with ZIF-8 as a carrier for the prevention and treatment of aquatic diseases.

CAS / MDL: 67-68-5 67-56-1
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JOURNAL OF CATALYSIS · 2017 · IF 6.844

Role of Brønsted acid site during catalytic combustion of methane over PdO/ZSM-5: Dominant or negligible?

Qiguang Dai,Qin Zhu,Yang Lou,Xingyi Wang

ZSM-5 zeolites (NaZSM-5, HZSM-5 and Silicalite-1) with different acid nature were synthesized and used as supports of Pd catalysts for catalytic combustion of methane. Moreover, the acid property of the as-synthesized Pd/NaZSM-5 catalyst was adjusted by a NH 4 + ion-exchange process to post-generate Brønsted acid sites and different preparation methods were investigated. The potential roles of Brønsted acid sites (anchoring Pd species or activating methane molecules) were discussed, and the experimental results indicated that the anchoring effect of Brønsted acid sites on Pd species was not directly observed. However, the acid properties of supports (the presence of Al 3+ as Lewis acid sites, especially coordinatively unsaturated Al 3+ ) were crucial for the preparation of Pd/ZSM-5 catalysts with high Pd dispersion. Additionally, although Brønsted acid sites of ZSM-5 was contributed to the activation or even cracking of long-chain alkanes (such as n -decane), the direct adsorption/dissociation of methane on Brønsted acid sites was difficult and depended more on the dispersion and particle size of PdO x . Pd/NaZSM-5 catalyst presented an outstanding durability at low-temperature (350 °C) and high-temperature (800 °C), and the high Si/Al ratio could improve the water-resistance due to its good hydrophobicity, but the reversible deactivation owing to the formation of PdO into Pd(OH) 2 under high concentration of water vapor was still unavoidable.

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RSC Advances · 2017 ·Vol. 7 ·期 44 ·27682-27688 · IF 3.108

p-Hydroxybenzenesulfonic acid–formaldehyde solid acid resin for the conversion of fructose and glucose to 5-hydroxymethylfurfural

Wenzhi Li,Tingwei Zhang,Haosheng Xin,Mingxue Su,Longlong Ma,Hason Jameel,Hou-min Chang,Gang Pei

A novel solid p-hydroxybenzenesulfonic acid–formaldehyde resin (SPFR) was prepared via a straightforward hydrothermal method. The catalytic properties of SPFR solid acids were evaluated in the dehydration reaction of fructose and glucose to 5-hydroxymethylfurfural (HMF). SEM, TEM, N2 adsorption–desorption, elemental analysis (EA), thermogravimetric analysis (TGA), and FT-IR were used to explore the effects of catalyst structure and composition on the HMF preparation from fructose. The effects of reaction time and temperature on the dehydration of fructose and glucose were also investigated. An HMF yield as high as 82.6% was achieved from fructose at 140 °C after 30 min, and 33.0% was achieved from glucose at 190 °C in 30 min. Furthermore, the recyclability of SPFR for the HMF production from fructose in 5 cycles was good.

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FOOD CHEMISTRY · 2024 · IF 8.5

High-performance ratiometric fluorescence detection and removal of tetracycline in milk based on CDs@ZSM-5:Eu3+

Yuchi Zhang,Le Han,Bohan Li,Yan Xu

Exploring materials with the dual functionality of detecting and removing tetracycline (TC) residues is crucial because of the environmental and health risks posed by antibiotic overuse. This study introduces a dual-emissive luminescent probe, CDs@ZSM-5:Eu 3+ , created through a solvent-free method combined with subsequent Eu 3+ ion exchange. The nanocomposite's blue emission, originating from carbon dots (CDs), is quenched by TC via an internal filtering effect, while an antenna effect triggers a strong red fluorescence of a TC-Eu 3+ chelate. The ratiometric fluorescence changes in CDs@ZSM-5:Eu 3+ endow a self-calibrated sensing mechanism for TC, offering a low detection limit of 5.04 nM and a broad detection range of 0.01–50 μM. Demonstrated in real milk samples, the probe exhibits high selectivity and accuracy in detecting TC. The nanocomposite also displayed an impressive TC removal capacity of 238.1 mg g −1 in water, ascribing to the enrichment and electrostatic attraction effects of ZSM-5 toward TC molecules. This research offers a facile strategy for constructing multifunctional zeolite-based hybrids for simultaneous TC detection and removal from aqueous solutions.

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Molecular Catalysis · 2024 · IF 3.9

Fabrication of tannic acid promoted lignin-MOF hybrids derived catalysts for catalytic transfer hydrogenation of 5-hydroxymethylfurfural

Yin Wang,Haihong Xia,Fei Ge,Yanrong Wang,Xiaohui Yang,Jianchun Jiang,Minghao Zhou

The catalytic conversion of 5-hydroxymethylfurfural (5-HMF) to value-added chemicals was quite vital for the conversion and utilization of biomass resources. The development of novel and efficient catalysts was of great significance. In this work, a series of tannic acid doped catalysts (Ni-Co/TA@C) were prepared by hydrothermal self-assembly method using lignosulfonate as a building block and coordinating with metal ions Ni 2+ and Co 2+ . The effects of different preparation conditions and reaction conditions on the performance of the catalysts were investigated, and the optimal conditions for catalytic transfer hydrogenation were also explored. The results showed that the conversion of 5-HMF was 99.97% and the yield of 2,5-dimethyl furan (DMF) was as high as 87.10% with Ni 2 Co/TA@C as catalyst under mild reaction conditions (240 °C, 2 MPa N 2 , 4h). The surface morphology, surface area and composition of the catalysts were characterized in detail. The Ni 2 Co/TA@C catalyst had higher total acidity and larger amount of strong acid sites, which was conducive to highly selective catalytic transfer hydrogenation (CTH) of DMF, and the larger specific surface area also promoted the dispersion and loading of Ni and Co. This study provided some novel findings for the construction of catalysts for biomass conversion.

CAS / MDL: 67-47-0 8061-51-6
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RENEWABLE ENERGY · 2024 · IF 9

Hierarchical HZSM-5 catalysts enhancing monocyclic aromatics selectivity in co-pyrolysis of wheat straw and polyethylene mixture

Hong Tian,Rui Zhu,Guangming Zhu,Jiawei Wang,Yi Cheng

The limitation in bio-oil quality hampers its further utilization in the fuel or chemical industry. This study employed a combination of tetra propylammonium hydroxide (TPAOH) and NaOH solutions for HZSM-5 desilication to enhance the yield of monocyclic aromatic hydrocarbons in the catalytic co-pyrolysis of wheat straw with polyethylene. Results revealed hierarchical HZSM-5, prepared with equal mole concentrations of NaOH and TPAOH, exhibited optimal catalytic performance. The bio-oil from this process had an aromatic content of 72 %, with monocyclic aromatic hydrocarbons (MAHs) constituting 56.26 %. Further optimization was achieved through iron modification of hierarchical HZSM-5. The addition of 0.5 % iron-modified hierarchical HZSM-5 increased the aromatic hydrocarbons to 80.57 %, with BTX compounds (benzene, toluene, and xylene) reaching a selectivity of 61.9 %. This approach reduced polycyclic aromatic hydrocarbons (PAHs), contributing to less coke formation, presenting a promising method for high-quality bio-oil.

CAS / MDL: 12125-02-9
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