JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
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2021
·
IF 3.995
Ruizhen Zhang,Jie Wang,Lina Han,Jiancheng Wang,Liangfu Zhao
HZSM-5 molecular sieves are efficient catalysts in the aromatization of light hydrocarbons and the fabrication of HZSM-5-based core–shell composites has become an important strategy to improve their catalytic performance due to the simultaneous modification of the acidity and pore structures in the catalyst. In this paper, HZSM-5/SAPO-5 (CSZP and CSZC) were synthesized via a two-stage crystallization process using PDDA and CTAB as modifiers of HZSM-5, respectively. The structure, acidity, and the weight of carbon deposition of the resulting molecular sieves catalysts were characterized using various methods and their catalytic behavior in isobutane aromatization investigated. The results show that CSZP exhibits a perfect core–shell structure with a uniform and thin shell composed of nano-SAPO-5, while CSZC has an irregular coat configuration with HZSM-5 covered by a rough and thick shell consisting of flaky micro-SAPO-5 crystals. The introduction of SAPO-5 via an in-situ synthesis decreases the Brønsted acidity of the catalysts to different extents and provides a large number of intergranular mesopores due to the stacking of SAPO-5 on the surface of HZSM-5, which is favorable toward improving the BTEX selectivity (benzene, toluene, ethylbenzene, and xylene) and catalytic stability over CSZP and CSZC. Meanwhile, CSZP has more competitive advantages than CSZC in promoting the mass transfer efficiency due to its significantly thinner shell than CSZC, which combined with its moderate acidity and appropriate mesopore structure result in its excellent selectivity and stability during the aromatization of isobutane.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yonghou Xiao,Jiahui Fu,Heyang Zhu,Qidong Zhao,Liang Zhou
The diffusion limitation owing to the long and narrow pore structure in traditional ZSM-5 zeolite could restrain the adsorptive desulfurization performance towards thiophene sulfur compounds from fuels. Herein, ZSM-5 zeolite nanocrystals were successfully fabricated using steam-assisted gel crystallization strategy to control the size of zeolite particles within 70 ∼ 160 nm. Compared to traditional micron ZSM-5, ZSM-5 zeolite nanocrystals could effectively reduce the diffusion pathway, enlarge the specific surface area, and increase exposure of adsorption sites, which could enhance the desulfurization performance. ZSM-5 nanocrystals with a mole ratio SiO 2 /Al 2 O 3 of 200 exhibited a satisfactory desulfurization efficiency, and the breakthrough capacity attained 0.0509 mmol S/g adsorbent. After ZSM-5 nanocrystals were ion-exchanged with NH 4 + and Ag + , both mesoporous characteristics and the Lewis acid (L-acid) sites were enhanced, which promoted the adsorption desulfurization performance. Furthermore, nanocrystalline ZSM-5 and Ag/ZSM-5 also exhibited acceptable regeneration performance. This study is expected to provide an effective strategy and a facile method to prepare nanocrystalline ZSM-5 based adsorbents for the development of efficient desulfurization materials.
研究领域:
化学工程
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材料科学
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产品关联
DOI
高影响因子
Nano-Micro Letters
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2025
·Vol. 18
·期 1
·5
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IF 36.3
Huang Rulu,Liu Chao,Zhang Kaili,Jiang Jianchun,Tian Ziqi,Chai Yongming,Wang Kui
A porous carbon-supported Ni-ZnO nanoparticles catalyst (Ni-ZnO/AC) was synthesized by low-temperature coprecipitation, demonstrating exceptional catalytic activity and stability.
Selective hydrogenation of 5-hydroxymethylfurfural (HMF) to 2,5-bis(hydroxymethyl)furan (97.5%) or 2,5-dimethylfuran (99.5%) is achieved over Ni-ZnO/AC catalyst by solvent-tuning.
Solvent-catalyst interaction jointly regulates hydrodeoxygenation behavior in HMF hydrogenation by modulating rate and pathway via a hydrogen shuttle mechanism.
研究领域:
催化化学
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绿色化学
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纳米材料科学
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生物质转化
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有机合成
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产品关联
DOI
PubMed
高影响因子
RSC Advances
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2019
·Vol. 9
·期 56
·32848-32853
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IF 3.049
Yan Huang,Pilan Zhang,Hualei Hu,Danxin Hu,Jie Yang,Yexin Zhang,Chunlin Chen,Yong Yang,Jian Zhang,Lei Wang
A group of CuAPO-5 molecular sieves with trace Cu were successfully synthesized via an ionothermal method and used for fructose dehydration to 5-hydroxymethylfurfural (HMF) in [BMIM]Br ionic liquid. The 0.06-CuAPO-5 sample displayed excellent performance and a HMF yield of 93.8% was obtained, which could be ascribed to the balance between acid strength and mass transfer efficiency. This work demonstrates that the ionothermal synthesized CuAPO-5 molecular sieve was also a good candidate for the efficient production of HMF.
研究领域:
化学工程
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催化反应
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产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Jiang Zhang,Zijian Wang,Mugeng Chen,Yifeng Zhu,Yongmei Liu,Heyong He,Yong Cao,Xinhe Bao
Deoxygenative upgrading of 5-hydromethylfurfural (HMF) into valuable chemicals has attracted intensive research interest in recent years, with product selectivity control remaining an important topic. Herein, TiO 2 supported gold catalysts coated with a thin N-doped porous carbon (NPC) layer were developed via a polydopamine-coating-carbonization strategy and utilized for pathway-specific conversion of HMF into 5-methylfurfural (5-MF) with the use of renewable formic acid (FA) as the deoxygenation reagent. The as-fabricated Au/TiO 2 @NPC exhibited excellent catalytic performance with a high yield of 5-MF (>95%). The catalytic behavior of Au@NPC-based catalysts was shown to be correlated with the suitable combination of highly dispersed Au nanoparticles and favorable interfacial interactions in the Au@NPC core-shell hetero-nanoarchitectures, thereby facilitating the preferential esterification of HMF with FA and suppressing unproductive FA dehydrogenation , which promoted the selective formylation/decarboxylation of hydroxy-methyl group in HMF in a pathway-specific manner. The present NPC/metal interfacial engineering strategy may provide a potential guide for the rational design of advanced catalysts for a wide variety of heterogeneous catalysis processes in terms of the conversion of biomass source.
研究领域:
催化化学
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生物质转化
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材料科学
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产品关联
DOI
高影响因子
FUEL
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2017
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IF 4.601
Dongjing Liu,Weiguo Zhou,Jiang Wu
CuO-based and MnO x -based sorbents modified with Ce and La using sol-gel method, were employed for elemental mercury removal at 120–240 °C. The Hg 0 removal activity of Mn 2 O 3 /ZSM-5 can be significantly enhanced by doping 50 at.% Ce or 10 at.% La, the Hg 0 removal efficiency increased by 94% and 71%, respectively. The Hg 0 removal ability of CuO/ZSM-5 subtly improved by addition of 50 at.% Ce or 10 at.% La, the Hg 0 removal efficiency ascended only by 6% and 18%, respectively. The XPS results revealed that Hg 0 transformed to HgO, and CuO (or Mn 2 O 3 ) was reduced to Cu 2 O (or Mn 3 O 4 ), which is in agreement with Mars-Maessen mechanism.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
PLANT CELL TISSUE AND ORGAN CULTURE
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2018
·Vol. 134
·期 2
·319-330
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IF 2.004
Zheng Jie,An Yuyan,Wang Liangju
Color is a key factor for fruit commercial value. 5-Aminolevulinic acid (5-ALA), as an eco-friendly plant growth regulator, shows an attractively promotive effect on plant secondary metabolism, especially for fruit coloration. Brassinosteroids (BRs) can also improve plant flavonoid biosynthesis. No information is now available on the relationship between 5-ALA and BR. Here, we found that 1.5 mg L −1 24-epibrassinolide (24-EBL) promoted 50 mg L −1 5-ALA-induced anthocyanin accumulation, while, brassinazole (Brz) significantly inhibited the 5-ALA-induced flavonoid accumulation. HPLC analysis further showed that the inductive effects of 5-ALA on the accumulation of cyanidin-3-galactoside, quercetin-3-galactoside, quercetin and kaempferol were elevated by 24-EBL, but impaired by Brz. These results suggest that brassinolide biosynthesis might involve in 5-ALA-induced flavonoid accumulation. Gene expression analysis showed that 5-ALA and 5-ALA + 24-EBL induced the expression of regulatory genes MdMYB10, MdMYB9, MdbHLH3 and MdbHLH33 . These two treatments also up-regulated the structural gene expressions of anthocyanin biosynthesis and transportation, including MdCHS, MdF3′H, MdDFR, MdANS, MdUFGT, MdGST and MdMATE , as well as flavonol biosynthetic gene MdFLS . But Brz decreased 5-ALA-induced up-regulation of these genes. In addition, 5-ALA also induced the expression of MdBRI1, MdBAK1 and MdBZR1 , which are involved in brassinolide signal transduction. These results indicate that 24-EBL enhances 5-ALA-promoted expression of genes related to flavonoid biosynthesis and brassinolide signal transduction, while Brz exhibits the opposite effects. Taken together, we propose that 24-EBL is involved in 5-ALA-induced anthocyanin and flavonol accumulation in calli of apples. Our results provide new insights into 5-ALA-induced fruit coloration.
研究领域:
植物生理学
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分子生物学
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园艺学
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DOI
高影响因子
Catalysis Science & Technology
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2019
·Vol. 9
·期 5
·1238-1244
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IF 5.726
Guohan Sun,Jiahuan An,Hong Hu,Changzhi Li,Songlin Zuo,Haian Xia
A green approach for the conversion of 5-(hydroxymethyl)furfural (HMF) to 5-methylfurfural (MF) by using size-controlled palladium catalysts has been developed. Palladium nanoparticles (Pd NPs) with various sizes supported on activated carbon were prepared with polyvinylpyrrolidone (PVP) as the capping agent. The reaction results showed that all the PVP-assisted Pd catalysts achieved high selectivity whilst the hydrogenation ability of Pd NPs could be rationally tuned by varying the mole ratio of Pd/PVP. 2.5% Pd–PVP/C (1 : 2) presented a satisfactory activity with 80% MF yield and 90% selectivity. The reaction kinetics study showed that the transformation of HMF into MF over bifunctional PVP-assisted Pd NPs underwent an acid-catalyzed esterification followed by a Pd-catalyzed hydrogenolysis procedure. The role of formic acid in the transformation is not only as a hydrogen-donating agent but also as a reactant to form the key intermediate. This work provides a novel and environmentally-friendly method for the selective hydrogenation of bio-based HMF to MF.
研究领域:
化学工程
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催化科学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2013
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IF 2.145
Anqiu Liu,Zehui Zhang,Zhongfeng Fang,Bing Liu,Kecheng Huang
In this study, we have developed a new method for the synthesis of EMF from HMF and fructose using mesoporous MCM-41 supported 12-tungstophosphoric acid (MCM-41-HPW) as the catalyst. The structure of 40 wt.% MCM-41-HPW was characterized by various techniques and its surface acidity was determined by potentiometric titration. A high EMF yield of 83.4% was obtained from HMF by the etherification reaction. Synthesis of EMF from fructose was also realized through one-pot reaction with a moderate yield of 42.9%. More importantly, the catalyst could be reused for several times without the loss of its catalytic activity.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
ChemCatChem
·
2021
·Vol. 13
·期 15
·3461-3469
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IF 5.686
Hualei Hu,Tingting Xue,Zhenxin Zhang,Jiang Gan,Liangqi Chen,Jian Zhang,Fengzuo Qu,Weijie Cai,Lei Wang
Graphical Bifunctional catalyst : The highly-efficient conversion of 5-hydroxymethylfurfural (HMF) to 2,5-bis(ethoxymethyl)furan (BEMF) was achieved by using the copper-loaded hierarchically structured ZSM-5 (Cu/HSZ) catalysts in the continuous fixed-bed reactor. The highly-efficient conversion of 5-hydroxymethylfurfural (HMF) to 2,5-bis(ethoxymethyl)furan (BEMF) was achieved over the copper-loaded hierarchically structured ZSM-5 (Cu/HSZ) catalysts in the continuous fixed-bed reactor. The main reaction path for BEMF synthesis on the Cu/HSZ catalysts was confirmed as following: HMF was firstly hydrogenated to BHMF intermediates over metal sites and then the formed BHMF was etherified by acid sites. Benefiting from the ammonia evaporation (AE) method promoted the dispersion of copper and reduced the acidity, the Cu/HSZ-AE catalyst exhibited more excellent BEMF yield and stability than the catalyst prepared by conventional incipient-wetness impregnation (Cu/HSZ-IW). Indeed, the inactivation of Cu/HSZ-IW catalyst was mainly attributed to the deactivation of copper by carbon species deposition.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
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2022
·Vol. 13
·期 18
·16887-16898
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IF 4.05
Wang Fei,Lai Jinhua,Liu Zixuan,Wen Sha,Liu Xianxiang
Spinel copper–manganese oxide catalysts were prepared via the co-precipitation method to be used for the catalytic selective oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA). Morphological characterization revealed that the primary particles of the as-synthesized catalysts were irregular nanoparticles aggregated with each other. The effects of reaction conditions such as time, temperature, and the dosage of oxidant on the catalytic activity were investigated. The experimental results show that the CuMn 2 O 4 showed superior catalytic performance in HMF selective oxidation reaction. In the presence of acetonitrile and tert-butyl hydroperoxide as oxidant, the catalytic reaction can achieve complete conversion of HMF, and the FDCA selectivity reached to 96.4%. The catalyst exhibited good recyclability and recoverability in a three-run recycling test. Mechanism studies reveal that Mn 3+ has a significant influence on the catalytic oxidation and the synergistic interaction between Mn and Cu can facilitate the mobility of oxygen thus improving the catalytic activity. Graphical abstract
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2019
·
IF 4.978
Ting Wang,Junnan Wei,Huai Liu,Yunchao Feng,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Lu Lin
2, 5-Bishydroxymethylfuran (BHMF) has been currently emerged as a promising biomass-derived monomer . It is highly desirable to proceed a chemical process at a high substrate concentration, by which a facile and cost-effective separation of products can be expected. Herein, we report for the first time on the hydrogenation of highly concentrated 5-hydroxymethylfurfural (HMF) in deep eutectic solvents (DESs), giving a near quantitative selectivity towards BHMF in ChCl-glycerol DES at 25 °C in 3 h using NaBH 4 as the H-donor. DES is hailed as a new class of green solvent, in which HMF/BHMF could be stabilized by the strong hydrogen-bond interaction, and allowed the selective hydrogenation of HMF at high concentration up to 40 wt%. Notably, the resulting BHMF could be facilely separated by extraction with ethyl acetate, and then high purity of BHMF with a desirable isolated yield around 80% was obtained after removing of ethyl acetate. Additionally, the reaction efficiency of HMF hydrogenation in DESs was verified to be strongly associated with the viscosity of DESs and the p K a value of hydrogen-bonding donor.
研究领域:
化学工程
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绿色化学
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生物质转化
✓ 已验证
DOI
高影响因子