RSC Advances
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2016
·Vol. 6
·期 103
·101365-101371
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IF 3.289
Guang Xiong,Jinpeng Yin,Jiaxu Liu,Xiyan Liu,Zhendong Guo,Liping Liu
Nano-sized ZSM-5 aggregates with interparticle mesopores was synthesized by an aerosol-assisted method. The amorphous aluminosilicate powder was used as a precursor, which was obtained by an aerosol process from an aqueous solution of the silicon and aluminium sources. The amorphous powder was crystallized in an autoclave with the structure-directing agent tetrapropylammonium hydroxide. No extra water was added in this step. The synthesis was performed in an extremely dense system, hence the amount of both template and waste water can be significantly reduced. The formation of the nanocrystalline MFI zeolite is mainly based on the liquid phase transformation in a supersaturation system. The nano-sized ZSM-5 aggregates were composed of nanocrystals with a size of 50–100 nm. Compared with the ZSM-5 zeolite synthesized by a conventional hydrothermal method, the nano-sized ZSM-5 aggregates exhibits a higher BET surface area, external surface area, and total pore volume and better Al species distribution. This nanocrystalline ZSM-5 zeolite shows a higher catalytic activity and stability in catalytic cracking of 1,3,5-triisopropylbenzene.
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yunlei Zhang,Yu Cao,Changhao Yan,Wenyun Liu,Yao Chen,Wen Guan,Fang Wang,Yiran Liu,Pengwei Huo
Upgrading bioderived 5-hydroxymethylfurfural (HMF) to high value-added bioplastic monomer 2,5-furandicarboxylic acid (FDCA) is a promising route for biomass conversion. Developing an efficient supported metal catalyst and clarifying the structure–activity relationship between the support and active sites is the key to boost FDCA production. Herein, ZrO 2 coated on natural and abundant halloysite nanotubes (HNTs) was synthesized and employed as a support for Au nanoparticles loading. The Au-ZrO x interface active sites were successfully engineered, and the active site amount can be rationally tailored by adjusting the crystal phases of ZrO 2 via changing calcination temperature. A combination study of catalysts surface physicochemical properties and catalytic activity reveals that oxygen vacancies (O v ) play a vital role in enhancing the adsorption of O 2 . Meanwhile, interface active sites facilitate the chemisorption and activation of O 2 molecules, which makes it easier to produce oxygen active species (superoxide radicals). More importantly, in-situ infrared spectroscopy and adsorption experiments also demonstrate that the catalyst with a higher O v concentration not only contributes to a stronger Lewis acid intensity, but also enhances the adsorption capacity of a key intermediate 5-hydroxymethyl-2-furancarboxylic acid (HMFCA), thus leading to an acceleration of the rate-determining step of hydroxyl group oxidation. The highest 99.4 % of FDCA yield can be obtained in 3.0 h. This newly proposed model of interface active sites may shed a light on the design of novel heterogeneous catalysts for the related biomass oxidation reactions.
研究领域:
催化
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材料科学
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化学工程
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生物质转化
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产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Jiaojiao Liu,Huifang Zhang,Ningyue Lu,Xiaoliang Yan,Binbin Fan,Ruifeng Li
A series of mesoporous ZSM-5-x (x = Si/Al molar ratio) supports, possessing various Si/Al ratios, were prepared without using the secondary templates, and the influences of acidity of ZSM-5-x on catalytic performance of Pt/HZSM-5-x samples prepared by the conventional wetness impregnation in naphthalene hydrogenation were investigated. The results show that decreasing Si/Al ratios of mesoporous ZSM-5 supports promotes the dispersion of the supported Pt species, and the catalytic efficiencies of Pt/HZSM-5-x samples for naphthalene hydrogenation depend on the integrated effects of the Pt dispersion, the acidity, and the mesoporous structure of ZSM-5 supports. This work provides the detailed influences of acidity of mesoporous ZSM-5 on catalytic performance of supported Pt catalysts in naphthalene hydrogenation.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Xiaoxue Li,Xiaopo Niu,Shuaikang Zhu,Shuang Xu,Zheyuan Wang,Xiangwen Zhang,Qingfa Wang
Fabricating zeolite-supported catalysts with excellent catalytic performance for hydroconversion of bio-oils into high-quality fuels is still a great challenge. Herein, hierarchical ZSM-5 zeolites were successfully synthesized with 3-[(trimethoxysilyl) propyl] octadecyldimethylammonium chloride as a mesoporous template. The hierarchical ZSM-5 supported Pt catalysts (Pt/HZ-x) were used to enhance the hydrodeoxygenation of dibenzofuran into bicyclohexane, and the influence of acidity distribution on the reaction pathways was investigated by tailoring the Si/Al molar ratios (50, 75, and 100). For all catalysts, cycloalkanes were produced via the partial hydrogenation of the aromatic rings to generate tetrahydrodibenzofuran, followed by the cleavage of C—O bond. The optimal bicyclohexane selectivity (86.8%) was obtained on Pt/HZ-75 catalyst due to the good synergistic effect between metal dispersion and acid distribution. This catalyst also showed excellent stability because of its strong metal–support interactions. Even after reused five times, the catalytic activity was almost unchanged compared with the fresh one. Furthermore, the possible reaction pathways for conversion of dibenzofuran into bicyclohexane over Pt/HZ-x catalysts were developed.
研究领域:
催化
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化学工程
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材料科学
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DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 27
·16311-16318
·
IF 3.108
Yue Yang,Qiying Liu,Dan Li,Jin Tan,Qi Zhang,Chenguang Wang,Longlong Ma
Selective hydrogenation of 5-hydroxymethylfurfural (HMF) has potential application in high quality biofuels. Herein, the catalytic hydrodeoxygenation (HDO) of HMF to 2,5-dimethylfuran (DMF) was investigated using bi-functional Ru–MoOx/C catalyst prepared by initial wetness impregnation. The high dispersion and electronic transfer between Ru and MoOx were demonstrated by a series of characterization techniques. During this HDO process, the synergy effect between metallic Ru and acidic MoOx species in the Ru–MoOx/C catalyst plays an essential role in obtaining maximized target product DMF (79.4%) via effective aldehyde group hydrogenation by Ru followed by dehydration over MoOx. This work also elucidated that DMF production proceeded through two distinct pathways: the 2,5-hydroxymethyl furan intermediate was preferable by the aldehyde group hydrogenation of HMF over the Ru–MoOx/C catalyst. Over MoOx/C catalyst, comparatively, 5-methyl furfural was the key intermediate by direct hydrogenolysis of the hydroxyl group in HMF. This kind of catalyst is stable for the first two runs by maintaining the target product yield. After the third run, the catalyst showed deactivation gradually but could be almost completely recovered after regeneration by H2 reduction.
研究领域:
催化
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化学工程
·
生物燃料生产
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产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Xia Jing,Gao De,Han Feng,Lv Ruifu,Waterhouse Geoffrey I. N.,Li Yan
The catalytic hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF) is a promising route towards sustainable liquid fuels with a high energy density. Herein, a novel CuCoNiAl-containing mixed metal oxide catalyst (CuCoNiAl-MMO) was prepared by calcination a layered double hydroxide (LDH) precursor in N2 at 500 °C, then applied for the catalytic hydrogenolysis of HMF to DMF. The effects of reaction time, reaction temperature and hydrogen pressure on DMF selectivity were investigated. Under relatively mild reaction conditions (180°C, 1.0 MPa H2, 6.0 h), CuCoNiAl-MMO showed both a high initial activity and selectivity for hydrogenolysis of HMF to DMF, with HMF conversion rate of 99.8% and DMF selectivity of 95.3%. Catalysts characterization studies using scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) revealed the presence of various metal oxides and metallic copper on the surface of the CuCoNiAl-MMO catalyst, with the presence of mixed metal-oxide-supported metallic Cu nanoparticles being responsible good hydrogenolysis activity of the catalyst for selective DMF synthesis.
研究领域:
催化化学
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可再生能源
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材料科学
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产品关联
DOI
PubMed
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2017
·
IF 3.181
Miao Zuo,Kai Le,Yunchao Feng,Caixia Xiong,Zheng Li,Xianhai Zeng,Xing Tang,Yong Sun,Lu Lin
In this study, we put forward an effective two-step method of producing biofuel 5-ethoxymethylfurfural (5-EMF) from carbohydrates with DES mixture. With the catalysis of Amberlyst-15, 77.3% and 65.2% yield of 5-EMF were obtained respectively from the fructose and inulin in mild conditions. In addition, CrCl 3 modified Amberlyst-15 showed excellent catalytic performance in the aldoses dehydration, 46.7% and 50.2% of 5-EMF yield could be obtained from glucose and sucrose in the two-step reactions. Moreover, all catalysts used in this study could be effectively reused for several times.
研究领域:
生物化学
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可再生资源与环境科学
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产品关联
DOI
高影响因子
ENERGY & FUELS
·
2016
·
IF 2.835
Zhenzhen Yang,Wei Qi,Rongxin Su,Zhimin He
Selective synthesis of various versatile compounds from biomass is of great importance to replace traditional fossil fuel resources. A novel magnetic catalyst, ZnFe1.65Ru0.35O4, was prepared via a simple alkali-coprecipitation method. The structure of the as-prepared catalyst was characterized, and its catalytic performance was investigated for aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-diformylfuran (DFF) and 2,5-furandicarboxylic acid (FDCA) under different reaction conditions. A high DFF yield of 93.5% was obtained for the reaction at 110 °C for 4 h in dry DMSO, whereas the maximum FDCA yield of 91.2% was achieved for the reaction at 130 °C for 16 h in H2O/DMSO (1:2, v/v). More importantly, a plausible reaction pathway was proposed for the aerobic oxidation of HMF into FDCA, with the rate-determining step determined through kinetic study. In addition, DFF or FDCA could be produced from fructose by sequentially using a magnetic solid acid (Fe3O4–RGO–SO3H) and ZnFe1.65Ru0.35O4. The dehydration of fructose in the presence of Fe3O4–RGO–SO3H resulted in HMF. After the removal of Fe3O4–RGO–SO3H from the reaction solution with a magnet, HMF was further oxidized in the catalysis of ZnFe1.65Ru0.35O4. These two consecutive steps gave DFF in 73.3% yield and FDCA in 70.5% yield, under the respective optimum reaction conditions. The direct synthesis of DFF or FDCA from fructose avoids tedious separation of intermediate HMF, leading to savings, with regard to both time and cost.
研究领域:
化学工程
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催化科学
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绿色化学
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DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Zhijiao Huang,Yong Liu,Lungang Chen,Xinghua Zhang,Jianguo Liu,Chenguang Wang,Qi Zhang,Longlong Ma
2,5-dimethylfuran (DMF), a promising biomass-derived fuel, is synthesized via the hydrodeoxygenation of 5-hydroxymethylfurfural (HMF). This study focuses on the inherent activity of a 5Pt5Fe/C catalyst for HMF hydrodeoxygenation to DMF. The catalyst exhibited exceptional performance, achieving a remarkable DMF yield of 99.6 %. It displayed specific selectivity for C = O bond hydrogenation and C O bond cleavage in diverse substrates, producing high yield of 2-methylfuran from furfural and furfury alcohol, and high yield of toluene from benzaldehyde, benzyl alcohol. In-depth characterizations unveiled valuable insights into the 5Pt5Fe/C catalyst's properties, emphasizing a harmonious balance between metal and acid sites due to the interactive synergy between Pt and Fe species, enhancing hydrodeoxygenation activity. Additionally, the catalyst demonstrated satisfactory stability, maintaining a commendable DMF yield over five reaction cycles despite observed changes.
研究领域:
化学工程
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催化
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可再生能源
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产品关联
DOI
高影响因子
Materials
·
2022
·Vol. 15
·期 22
·8097
·
IF 3.748
Hongyun Wang,Haijun Cheng,Fang Lai,Deyuan Xiong
Copper(II)-containing aluminum phosphate material (CuAPO-5) was synthesized hydrothermally and used as a multiphase catalyst for the oxidation of α-pinene to verbenone. The catalysts were analyzed using X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET) surface area techniques, X-ray photoelectron spectroscopy (XPS), and ammonia temperature programmed reduction (NH3-TPD). Scanning electron microscopy (SEM), X-ray energy spectrometry (EDS), inductively coupled plasma emission spectroscopy (ICP-OES), Fourier infrared spectroscopy (FT-IR), and ultraviolet-visible spectroscopy (UV-vis) were performed to characterize the material. The effects of reaction temperature, reaction time, n(α-pinene)/n(TBHP), and solvent on the catalytic performance of CuAPO-5 were investigated. The results show that all the prepared catalysts have AFI topology and a large specific surface area. Copper is evenly distributed in the skeleton in a bivalent form. The introduction of copper increases the acid content of the catalyst. Under the optimized reaction conditions, 96.8% conversion of α-pinene and 46.4% selectivity to verbenone were achieved by CuAPO-5(0.06) molecular sieve within a reaction time of 12 h. CuAPO-5(0.06) can be recycled for five cycles without losing the conversion of α-pinene and the selectivity to verbenone.Keywords:CuAPO-5;α-pinene;selective oxidation;verbenone
研究领域:
催化化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Xu Xian,Lan Ling,Xu Jiangong,Liang Zheng,Tan Jin,Wang Haiyong,Qiu Songbai
The development of biodegradable materials from biomass is a crucial strategy for leveraging biomass resources. A key component in this process is 2,5-bis(hydroxymethyl)furan (BHMF), a significant biomass-derived platform chemical. However, producing BHMF with high selectivity through the selective hydrogenation of 5-hydroxymethylfurfural, while avoiding the creation of unwanted byproducts, is a complex challenge. In our research, we have developed a novel catalyst featuring a magnetic core. This catalyst, which consists of platinum loaded onto a graphene-like shell, has been applied to the catalytic hydrogenation of HMF in an aqueous environment. Under the optimized conditions of 373 K, 3 MPa H 2 , and 1 h reaction time, a BHMF yield exceeding 99% was achieved. This method presents a promising and effective approach for the high-value conversion of biomass waste into polymer materials and pharmaceutical chemicals. Graphical Abstract
研究领域:
化学工程
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催化科学
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可再生资源转化
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产品关联
DOI
高影响因子
FUEL
·
2016
·
IF 3.611
Panpan Yang,Qineng Xia,Xiaohui Liu,Yanqin Wang
Catalytic transfer hydrogenation/hydrogenolysis of 5-hydroxymethylfurfural (HMF) to valuable chemicals, 2,5-dimethylfuran (DMF), is realized over a carbon supported nickel-cobalt catalyst with formic acid as hydrogen donor. The highest DMF yield, 90.0%, is achieved at 210 °C under self-generated pressure. A reaction route involving 5-methylfurfural (5-MF) instead of 2,5-bis(hydromethyl)furan (BHMF) as an intermediate has been investigated, which is different from that when H 2 is used as hydrogen source in previous reports. The influence of the amount of formic acid is investigated on the conversion of HMF and the yield of DMF. The effectiveness of this strategy has also been used for the conversion of furfural to 2-methylfuran, another valuable chemicals.
研究领域:
催化
·
化学工程
·
可再生能源
✓ 已验证
产品关联
DOI
高影响因子