Green Energy & Environment
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2021
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IF 8.207
Weiyao Yang,Mengchen Fu,Chenyu Yang,Yiwen Zhang,Chun Shen
Despite wide applications of noble metal-based catalysts in 5-hydroxymethylfurfural (HMF) oxidation, promoting the catalytic performance at low loading amounts still remains a significant challenge. Herein, a series of metal oxide modified MO x -Au/TiO 2 (M = Fe, Co, Ni) catalysts with low Au loading amount of 0.5 wt% were synthesized. Addition of transition metal oxides promotes electron transfer and generation of the Au δ − –O v –Ti 3+ interface. A combination study reveals that the dual-active site (Au δ − -O v -Ti 3+ ) governs the catalytic performance of the rate-determining step, namely hydroxyl group oxidation. Au δ − site facilitates chemisorption and activation of O 2 molecules. At the same time, O v -Ti 3+ site acts as the role of “killing two birds with one stone”: enhancing adsorption of both reactants, accelerating the activation and dissociation of H 2 O, and facilitating activation of the adsorbed O 2 . Besides, superoxide radicals instead of base is the active oxygen species during the rate-determining step. On this basis, a FDCA yield of 71.2% was achieved under base-free conditions, complying with the “green chemistry” principle. This work provides a new strategy for the transition metal oxides modification of Au-based catalysts, which would be constructive for the rational design of other heterogeneous catalysts.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 22
·7326-7330
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IF 6.119
Wei Wang,Min Wang
Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is a promising and green process, which urgently demands high-performance catalysts. In this work, a nitrogen-modulated NiMoO4 growth on Ni foam (N-NiMoO4/NF) is prepared via the treatment of NiMoO4 in 1% NH3 at 500 °C. Compared with NiMoO4, the nitrogen-modulated NiMoO4 promotes electro-oxidation of HMF to FDCA and exhibits almost 100% HMF conversion, 97% FDCA yield, and 91% faradaic efficiency. N-NiMoO4 has a higher electrochemical surface area and lower charge transfer resistance than NiMoO4, which enhances the activity of the catalyst for electrocatalytic oxidation of HMF to FDCA. This work gives enlightenment on the nitrogen modulation method to tune the activity of electrocatalysts for biomass refineries.
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CHEMOSPHERE
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2021
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IF 7.086
Jian Tian,Kok Bing Tan,Yichen Liao,Daohua Sun,Qingbiao Li
A zeolitic cage was introduced and rationally fabricated by encapsulating Pt nanoparticles (NPs) in hollow ZSM-5, a nanomaterial with a cavity and porous shell, for efficient catalytic oxidation of benzene. The structure and formation of the zeolitic cage were systematically investigated and characterized using transmission electron microscopy , nitrogen sorption investigations, X-ray photoelectron spectroscopy, nuclear magnetic resonance spectroscopy , and X-ray diffraction. The obtained hollow 0.2 Pt@ZSM-5 exhibited a comparable low-temperature catalytic activity with 0.5Pt/ZSM-5 with T 90 value of 178 °C. Various characterization techniques combined with adsorption experiments uncover the tremendous role of the zeolitic cage in the catalytic activity toward benzene oxidation. The porous shell prevented benzene dilution and the acidity originating from the hollow interior of ZSM-5 promoted the storage of benzene, thereby forming a high local concentration of benzene around Pt NPs, resulting in excellent catalytic performance. These findings provide valuable insights into the rational design of efficient catalysts for the catalytic oxidation of volatile organic compounds.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Wei Liu,Taixin Liang,Jiangbo Zhang,Fei Xiao,Houhe Chen
Intermolecular energetic materials (IEMs) have become the focus of attention due to their excellent performance in combustion, ignition, energy release and sensitivity. In this paper, two IEMs were successfully designed and prepared by the self-assembly of 5-aminotetrazole (5-ATZ) and transition metal ions on the surface of ammonium perchlorate (AP) particles. The scanning electron microscope, infrared spectroscopy, powder X-ray diffraction, thermogravimetric analyses, and differential thermal analyses were employed to characterize the prepared samples. The results show that the surface of AP particles is completely covered by a uniform and dense M(5-ATZ) 4 Cl 2 (M = Cu, Co) self-assembled layer. Thermal analyses show that the high-temperature decomposition peak temperatures of AP/Cu(5-ATZ) 4 Cl 2 (10 wt%) and AP/Co(5-ATZ) 4 Cl 2 (10 wt%) are decreased by 93.3 °C and 127.1 °C compared to the case of pure AP, while the heat releases of them are increased by 539 J∙g −1 and 580 J∙g −1 . In addition, the burning rates of AP/Cu(5-ATZ) 4 Cl 2 /Al (10 wt%) and AP/Co(5-ATZ) 4 Cl 2 /Al (10 wt%) are increased by 6.8 mm∙s −1 and 7.8 mm∙s −1 compared with the case of AP/Al. Moreover, the hygroscopicity tests show that the prepared samples do not agglomerate aftter being placed in the atmosphere with a relative humidity of 79% for 66 h. This research shows considerable application prospects in improving the combustion and energy performance of solid propellants, it is also a reference for the design and preparation of other novel IEMs.
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Energies
·
2021
·Vol. 15
·期 1
·53
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IF 3.004
Kai Miao,Tan Li,Jing Su,Cong Wang,Kaige Wang
Catalytic hydropyrolysis via the introduction of external hydrogen into catalytic pyrolysis process using hydrodeoxygenation catalysts is one of the major approaches of bio-oil upgrading. In this study, hydrodeoxygenation of acetone over Mo/HZSM-5 and HZSM-5 were investigated with focus on the influence of hydrogen pressure and catalyst deactivation. It is found that doped MoO3could prolong the catalyst activity due to the suppression of coke formation. The influence of hydrogen pressure on catalytic HDO of acetone was further studied. Hydrogen pressure of 30 bar effectively prolonged catalyst activity while decreased the coke deposition over catalyst. The coke formation over the HZSM-5 and Mo/HZSM-5 under 30 bar hydrogen pressure decreased 66% and 83%, respectively, compared to that under atmospheric hydrogen pressure. Compared to the test with the HZSM-5, 35% higher yield of aliphatics and 60% lower coke were obtained from the Mo/HZSM-5 under 30 bar hydrogen pressure. Characterization of the spent Mo/HZSM-5 catalyst revealed the deactivation was mainly due to the carbon deposition blocking the micropores and Bronsted acid sites. Mo/HZSM-5 was proved to be potentially enhanced production of hydrocarbons.Keywords:hydrodeoxygenation;biomass;hydropyrolysis;MoO3;bifunctional catalysts
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2021
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IF 3.171
Yao Zhong,Cuiying Huang,Lijie Li,Qiang Deng,Jun Wang,Zheling Zeng,Shuguang Deng
Developing an efficient and selective catalyst for the dehydration of fructose to 5-hydroxymethylfurfural (HMF) is significant for biomass conversion. Herein, a metal-organic framework (MOF) with acidity and strong hydrophobicity is first reported by the condensation of amino-tagged MOFs with mercapto carboxylic acids and subsequent oxidation. The hydrophobic acidic MOFs possess acid densities ranging from 0.2−1.0 mmol·g −1 , H 2 O contact angles of 114°−125°, and specific surface areas above 260 m 2 ·g −1 . Compared to the methyl sulfo-functionalized MOF, the benzene sulfo-functionalized MOF with a strong hydrophobicity shows much higher activity and selectivity for the conversion of fructose to 5-hydroxymethylfurfural. In particular, 2.99% (mass) UiO-PhSO 3 H shows the best catalytic performance with a 90.4% HMF yield due to its suitable hydrophobicity and abundant acidic sites. Moreover, the catalyst shows great stability after recycling for 5 runs. This work provides an interesting design strategy for the preparation of hydrophobic acidic MOFs and shows the powerful synergistic effect of acidity and hydrophobicity.
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RSC Advances
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2021
·Vol. 11
·期 54
·33969-33979
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IF 3.361
Luxin Zhang,Yuting Liu,Ruijun Sun,Simin Yi
5-Ethoxymethylfurfural (EMF) has been identified as a potential biofuel and fuel additive, for which the production from glucose (the most abundant and inexpensive monosaccharide) in a one-step process would be highly desirable. Here, the synthesis of sulfonic acid-functionalized porous coordination polymers (PCPs) and their application as catalysts for EMF synthesis are reported. PCP(Cr)-BA (PCP material with Cr3+ ions and H2BDC-SO3H linkers) and PCP(Cr)-NA (PCP material with Cr3+ ions and H2NDC(SO3H)2 linkers) materials containing both Cr3+ sites and Brønsted-acidic –SO3H sites were prepared. The morphology, pore structure, acidity, chemical composition, and thermal stability of the two functionalized PCP(Cr) catalysts were analyzed by systematic characterization. The catalysts featured a porous morphology and dual Cr3+ and –SO3H sites, which enabled the cascade conversion of glucose to EMF. PCP(Cr)-BA exhibited higher performance than PCP(Cr)-NA with an EMF yield of 23.1% in the conversion of glucose at 140 °C after 22 h in an ethanol/water system. In addition, the as-prepared catalyst exhibited a high stability in the current catalytic system for EMF production from glucose with a constant catalytic activity in a four-run recycling test without an intermediate regeneration step.
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高影响因子
CHEMOSPHERE
·
2021
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IF 7.086
Jinyu Hou,Daoxu Zhong,Wuxing Liu
Hazardous oil sludge (OS) poses a great challenge to the environment, whereas conventional treatment methods (i.e., incineration or pyrolysis-incineration) are relatively less value-added and will bring about air pollution problems. To realize the high-value utilization of OS, catalytic co-pyrolysis with waste biomass to produce platform chemicals was studied using TG-FTIR and Py (pyrolyzer)-GC/MS methods. Results showed that for the non-catalytic co-pyrolysis of RH (rice husk) and OS, the main synergy on weight loss was the greatly lowered initial pyrolysis temperature of RH (for ∼55 °C) at the lower temperatures and the reduced weight loss ratio of OS (∼10–18 wt%) within the higher temperature range. ZSM-5 catalyst promoted the degradation of OS and RH mixtures at < 150 °C, yet showed minor effects on their weight loss at higher temperatures. The oxygenated and aliphatic compounds from non-catalytic co-pyrolysis were efficiently converted, resulting in an increased relative yield of aromatics to the highest of 46% and an elevated selectivity to BTX (as high as 60%). Despite the relatively short carbon chain length of OS components, ZSM-5 was proved effective to activate the OS pyrolysis products, thus enhancing the further aromatization reactions with biomass pyrolysis intermediates. This study provides a novel method for value-added co-utilization of hazardous OS waste and abundant biomass waste, and thus is beneficial to producing renewable chemicals while reducing the environment pollutant.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Junzong Chen,Miaojuan Qiu,Shiqiang Zhang,Binbin Li,Dong Li,Xiuyu Huang,Zhirong Qian,Jing Zhao,Zhiyong Wang,Di Tang
Calcium based biomaterials were widely used for drug delivery application due to their biodegradability, biocompatibility, and high drug loading capacity. Herein, amino-capped polyamidoamine (PAMAM) dendrimer was applied as a macromolecular template to form amino-modified calcium phosphate hollow sphere (CaPO-NH 2 ). After loading with 5-fluorouracil (5Fu), this system performed synergistic cancer chemotherapy. In this study, the 5Fu/CaPO-NH 2 particles could be efficiently uptaken by cancer cells, and then decompose into Ca 2+ and release 5Fu drug in the cytoplasm; therefore calcium overload and reactive oxygen species (ROS) accumulation were found in PSN1 cells that could induce cell membrane damage and elicit cell apoptosis through a series of biochemical reactions including endoplasmic reticulum stress, lipid peroxidation and mitochondrial apoptosis. In the PSN1 pancreatic cancer xenograft model, the 5Fu/CaPO-NH 2 system performed high tumor inhibition via chemotherapy and calcium overload induced apoptosis. Comparingly, the normal cells and organs were insensitive to this synergistic therapy, which indicated the well biocompatibility of delivery system. Thus, this study provided a promising CaPO-NH 2 drug delivery platform for enhanced 5Fu chemotherapeutic effect.
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高影响因子
Materials Today Communications
·
2021
·
IF 3.383
Yanqing Xue,Bo Li,Xinliang Wang,Xinlei Li,Han Zhang,Qitang Hao
Agglomeration behavior of TiB 2 particles in 5%TiB 2 /Al-4.5%Cu composites (all compositions are in wt.% unless otherwise specified) is studied by adding different content of Mg to improve its strength and ductility, a widely used in-situ molten salt reaction process is used to produce the composites. The results show that addition of Mg could not only significantly segregate TiB 2 particles but also further refine the α-Al grains and then improve the mechanical properties of the composites on the basis of TiB 2 particles. Here, 0.5% Mg is considered the optimum mass fraction for dispersion, refinement, and modification of particles based on the results of investigation. The yield strength (YS), ultimate tensile strength (UTS), elastic Young’s modulus (EM), and Vicker’s hardness (VHN) of the composites in T6 heat treatment are increased to 375 MPa, 486 MPa, 88 GPa, and 167 HV - an improvement of 21.8%, 16.5%, 20.9%, and 9.4%, respectively, versus the original TiB 2 /Al-4.5%Cu composite (308 MPa, 417 MPa, 63 GPa, and 153 HV). The elongation of the composite is improved by 20.9%. These merits are mainly attributed to addition of Mg, which increases the surface-spread coefficient of TiB 2 particles by reducing the surface tension of the Al melt, thereby improving the wettability .
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CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Zenan Ni,Yuming Li,Yaoyuan Zhang,Yajun Wang,Guoqing Cui,Guiyuan Jiang,Zhen Zhao,Chunming Xu
Ga species with high dehydrogenation capability were prepared by H 2 -O 2 atmosphere treatment, and efficient balance of bifunctionality (dehydrogenation/cracking) was realized between Ga species and ZSM-5 over Ga/ZSM-5 based catalysts. Compared with parent Ga/ZSM-5, the conversion rate of n -butane was increased from 0.53 to 2.59 mmol·g −1 ·min −1 on Ga/ZSM-5 with H 2 -O 2 treatment. Kinetic analysis revealed that the apparent activation energy of n -butane catalytic cracking decreased largely from 141 to 47 kJ·mol −1 , which is attributed to the formation of new interaction between Ga species and ZSM-5 upon such an atmosphere treatment. It was also found Butane-O 2 treatment acted as a similar role with H 2 -O 2 treatment in enhancing the catalytic performance. On this basis, different Ga species were correlated with activity and kinetic data, and the effect of practical reaction atmosphere on Ga species was also investigated.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2021
·
IF 5.541
Yang Li,Bin Hu,Salman Raza Naqvi,Zhen-xi Zhang,Kai Li,Qiang Lu
5-Hydroxymethylfurfural (5-HMF) is a value-added platform chemical, which can be obtained from pyrolysis of biomass materials, whereas related investigation on its selective production via catalytic fast pyrolysis (CFP) process is still insufficient. In this work, a zirconium-tin mixed metal oxide (ZrO 2 -SnO 2 ) catalyst was developed for the selective production of 5-HMF from the in-situ CFP of cellulose. According to pyrolysis-chromatography/mass spectrometry (Py-GC/MS) tests, the ZrO 2 -SnO 2 catalyst has better performance on the selective preparation of 5-HMF than single nano oxide ZrO 2 , SnO 2 , or their physical mixture. 5-HMF was sensitive to the reaction conditions, and its yield and selectivity always exhibited the tide of first increasing followed by decreasing along with the increase of Zr loading and catalyst-to-cellulose (CA-to-CL) ratio. At the optimum conditions with ZrO 2 -SnO 2 of 15 wt% Zr loading (ZrO 2 -SnO 2 -15), pyrolysis temperature of 350 °C and CA-to-CL ratio of 2:1, the 5-HMF yield was 6.49 wt%, which was 4 times more than that of the non-catalytic process (1.35 wt%). Correspondingly, the selectivity of 5-HMF was up to 23.50 %. The catalyst characterization combined with the pyrolysis texts of several typical saccharides, including cellobiose, maltose, glucose, and mannose indicated that the ZrO 2 -SnO 2 -15 could promote the breakage of glycosidic bonds with the formation of reducing ends and the selective conversion of the reducing end to 5-HMF due to its mild acidity. Overall, the ZrO 2 -SnO 2 is expected a promising catalyst for the CFP of cellulose to prepare 5-HMF.
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