CHEMISTRY LETTERS
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2022
·Vol. 51
·期 4
·395-398
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IF 1.715
Zhu Yue,Li Yue,Zhao Shipeng,Jing Ran,Zhang Heqian,Sun Daolai,Sato Satoshi
Hydrogenation of γ-valerolactone (GVL) to form 1,4-pentanediol (1,4-PDO) was performed over Co/ZrO2 catalysts with a Co metal loading of 15 wt. %. The calcination of Co/ZrO2 at high temperatures significantly promoted the catalytic activity irrespective of the decrease in the specific surface area. The 750 °C-calcined Co/ZrO2 with Co2+ species exhibited a high catalytic performance: a GVL conversion of 86.1% with a 1,4-PDO selectivity of 97.2% was achieved at 165 °C under 5 MPa H2 pressure.
研究领域:
化学工程
·
催化科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Shuxing Zhang,Xiaoshu Ding,Yanji Wang
5-Amino-1-pentanol is an important pharmaceutical intermediate used in the synthesis of anti-inflammatory and anticancer drugs. The direct hydrogenolysis of furfurylamine to 5-amino-1-pentanol has the advantages of a simple process route and high atom utilization. In this paper, for Pt/ZrO2 catalysts, the effects of different Pt loading and calcination temperatures on catalyst activity, selectivity, and surface properties such as Pt nanoparticle size, acidity and alkalinity, and the ratio of Pt0/(Pt0+Pt2+) were investigated. Through the study of the relationship between catalyst preparation conditions, furfurylamine hydrogenolysis reaction performance, and surface properties, it was found that moderate Pt nanoparticle size, higher Pt0/(Pt0+Pt2+) ratio, and more acidic sites favored furfurylamine hydrogenolysis. The higher number of basic sites favors the dispersion of Pt metal. The results of in situ FTIR show that the amino group of furfurylamine is adsorbed on the acidic site of Pt/ZrO2, and the furan ring is adsorbed on Pt nanoparticles, which is beneficial to the hydrogenolysis of furfurylamine.
研究领域:
催化化学
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药物合成
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产品关联
DOI
高影响因子
Energy Technology
·
2025
·
IF 3.6
Hui Huang,Qi Xu,Liangyun Yu,Lidong Li,Ying Zhang,Fennv Han,Qi Zhang
Currently, there is a thermodynamic and kinetic mismatch between carbon dioxide methanation. Carbon dioxide is stable in nature and requires a highly active catalyst to facilitate its reduction reaction. In this article, Ru/ZrO 2 catalysts are prepared by a structure-directed derivatization strategy using zirconium-based metal-organic frameworks (MOFs) (UiO-66) as precursors. The porous framework structure of MOFs was utilized to construct Ru nanoparticles with a large size (≈9.7 nm). Photothermal catalysis is employed, and the photoexcitation induced the transfer of electrons from the conduction band of ZrO 2 to Ru, which elevated the electron density of Ru to the enriched state and promoted the activation of CO 2 adsorption, while the photothermal effect facilitated the warming of the catalyst bureau, which provided a favorable condition for CO 2 methanation. The compositional valence, morphology, specific surface area, bandgap and other properties of the catalysts were evaluated by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscpe, Brunner-Emmet-Teller measurements, hydrogen temperature-programmed reduction, CO 2 -TPD, ultraviolet–visible, photoluminescence, and photocurrent response characterization. The experimental results showed that 99% methane selectivity and 120.354 mmol g cat −1 h −1 methane yield were achieved at 1 MPa and photothermal (250 °C) conditions.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
RSC Advances
·
2013
·Vol. 3
·期 26
·10277-10284
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IF 2.562
Xing Tang,Lei Hu,Yong Sun,Geng Zhao,Weiwei Hao,Lu Lin
A green and efficient process was developed for the conversion of biomass-derived ethyl levulinate (EL) into γ-valerolactone (GVL) using supercritical ethanol as the hydrogen donor and the reaction medium over low-cost and eco-friendly ZrO2 catalysts, which were prepared by the precipitation method and characterized by BET, SEM, XRD, FT-IR, TGA-DTA, TPD-NH3 and TPD-CO2. The results indicated that amorphous ZrO2 with a high specific surface area and a large number of acid–base sites exhibited the highest catalytic activity, an excellent GVL yield of 81.5% with 95.5% EL conversion was achieved at 523 K over 3 h. In addition, combined with the results of poisoning experiments, a plausible mechanism of catalytic transfer hydrogenation (CTH) via a six-membered ring transition state was also presented.
研究领域:
生物质化学
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催化反应工程
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Yuhao Tian,Yixuan Li,Dong Cao,Qiying Liu,Weijie Cai
Photo-assisted ethanol dry reforming (EDR) for syngas production was deeply studied over nanorod-like Ni/ZrO 2 catalyst synthesized by precipitation and impregnation technique, respectively. The effect of light irradiation as well as catalyst preparation method on EDR reaction was investigated in detail with the stoichiometric feed ratios, over a temperature region of 350 to 550 °C. Photo-enhancement factor of ethanol conversion greatly increased from 10% (dark) to 40% (light) together with less formation of byproducts. Moreover, the experimental results depicted the better performance of P-Ni/ZrO 2 catalyst due to its abundant oxygen vacancies and strong Ni-Zr interaction. Enriched interfacial oxygen defects and more light-excited electrons facilitated the activation/dissociation of ethanol and CO 2 , thereby enhancing the catalytic activity. In addition, the mean particle size of NiO in P-Ni/ZrO 2 was (10.3 nm) which was smaller than that of the I-Ni/ZrO 2 (16.5 nm), suggesting its higher dispersion of active metal. The calculated apparent activation energy of P-Ni/ZrO 2 was 20.6 eV which was much less than the value of I-Ni/ZrO 2 (37.7 eV). This work might provide the valuable insight for the development of highly-efficient photothermal catalyst to enhance the value-added utilization of greenhouse gas CO 2 .
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Fenghao Shu,Guangcai Long,Yanwu Chen,Ying Gao,Menghao Jiang,Jinxing Long
Conversion of renewable lignin to value-added aromatic chemicals presents a broad prospect to achieve the goals of “carbon neutrality”. In this work, an efficient approach is proposed for selective hydrogenolysis of lignin to valuable 4-propyl syringol in the presence of cost-effective catalyst of y Ni/ZrO 2 - x MoO 3 . When the lignin hydrogenolysis is performed with 15Ni/ZrO 2 -10MoO 3 , 15.4% yield of monophenols is achieved, which is approximately twice as that from the 15Ni/ZrO 2 catalytic system (7.8%). Importantly, 33.1% of these monophenols are identified as 4-propyl syringol (4-PS), a versatile fine chemical. An extensive characterization of the modified catalysts by means of XRD, nitrogen adsorption–desorption isotherm, SEM, TEM, XPS, NH 3 -TPD, CO 2 -TPD, and H 2 -TPR, confirms that the introduction of MoO 3 changes the primary phase of ZrO 2 and the acidity/basicity properties of catalyst. As a result, an enhanced cleavage of the C-O linkage between S-lignin and other units is demonstrated, which consequently contributes to the good selectivity of 4-propyl syringol. Therefore, this work provides a new insight for producing bulk aromatic chemicals via a sustainable route.
研究领域:
化学工程
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可再生资源利用
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产品关联
DOI
高影响因子
ENERGY & FUELS
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2020
·
IF 3.421
Yang Qu,Yuan Zhao,Shanshan Xiong,Chenguang Wang,Shurong Wang,Lingjun Zhu,Longlong Ma
5-Hydroxymethylfurfural (HMF) and levulinic acid (LA) are two important platform compounds that can be produced by the dehydration of hexoses from hydrolysis of cellulose. In this study, glucose dehydration was catalyzed by the SO42–/ZrO2 catalyst in the NaCl–THF/H2O biphasic solvent system. Complete conversion of glucose was achieved at 160 °C. The highest HMF yield and LA yield were 61.84% and 29.68%, respectively. The results showed that the conversion and product distribution were influenced by catalyst acidity, solvent composition, temperature, and time. The SO42– load greatly changed the acidity of the catalyst, thus affecting the product distribution. By changing the composition of the catalyst and the biphasic solvent system, different yields of HMF and LA could be obtained, so as to realize directional synthesis of the target products.
研究领域:
生物化学
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催化化学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 23
·15927-15938
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IF 2.993
Xun Suhang,Hou Caozheng,Li Hongping,He Minqiang,Ma Ruliang,Zhang Ming,Zhu Wenshuai,Li Huaming
The catalyst of WO 3 highly dispersed on mesoporous ZrO 2 was prepared by hydrothermal treatment and calcination. Ionic liquid templates with different cations and various calcination temperatures were taken into account to investigate factors that affect the structure of the catalysts. Wide-angle XRD, Raman, low-angle XRD, N 2 adsorption–desorption, SEM, EDS-mapping and TEM analyses were employed to characterize the composition, morphology and the dispersion of WO 3 . It was found that [C 16 H 33 N(CH 3 ) 3 ] 4 SiW 12 O 40 and 700 °C were the optimal ionic liquid template and calcination temperature; the obtained catalyst, expressed as 700-C 16 -WO 3 /ZrO 2 , exhibited the best catalytic activity in oxidation desulfurization. Dibenzothiophene (DBT) in the model oil could be oxidized to DBT sulfone (DBTO 2 ) completely, certified by GC-MS analysis, under optimum conditions. The oxidative desulfurization efficiencies of different substrates catalyze by 700-C 16 -WO 3 /ZrO 2 , and the cycle performance on the oxidation of DBT were studied.
研究领域:
催化化学
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能源化学
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产品关联
DOI
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 14
·8709-8717
·
IF 3.108
Yu Hao Wang,Wen Gui Gao,Hua Wang,Yan E. Zheng,Wei Na,Kong Zhai Li
A series of Cu–ZrO2 (CZ) catalysts with different surface area, copper surface area (SCu), oxygen vacancy concentration, and interaction between Cu and ZrO2 features were synthesized. The factors that could affect catalytic activity of CO2 hydrogenation to methanol were investigated. The interaction between Cu and ZrO2 is crucial for determining the catalytic activity. The catalyst possessing the strongest interaction between Cu and ZrO2, exhibited the optimum catalytic activity. The evolution of carbonaceous species and pyridine adsorption over CZ catalysts were investigated using in situ DRIFT spectroscopy. It is found that the hydrogenation of formate species is a rate-limiting step and H spillover plays an important role. The hydrogenation of formate species and H spillover are strongly dependent on the interaction. These results provide a new way of understanding the activity dependence and reaction mechanism of CO2 hydrogenation to methanol over CZ catalysts.
研究领域:
催化化学
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能源化学
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产品关联
DOI
高影响因子
Green Energy & Environment
·
2020
·
IF 6.395
Yuewen Shao,Tingting Wang,Kai Sun,Zhanming Zhang,Lijun Zhang,Qingyin Li,Shu Zhang,Guangzhi Hu,Xun Hu
Oxides with different crystal phases can have important effects on the configuration of surface atoms, which can further affect the distribution of hydrogenation sites and acidic sites as well as the competitions of these varied types of catalytic sites. This could be potentially used to tailor the distribution of the products. In this study, zirconium oxides with different crystal phases supported copper catalysts were prepared for the hydrogenation of the biomass-derived furfural, vanillin, etc. The results showed that both calcination temperature and Cu species affected the shift of zirconia from tetragonal phase to the monoclinic phase. Monoclinic zirconia supported copper catalyst can effectively catalyze the hydrogenation of furfural to furfuryl alcohol via hydrogenation route due to its low amount of Brønsted acidic sites, although the surface area and the exposed metallic Cu surface area were much lower than the tetragonal zirconia supported copper catalyst. Zirconia with tetragonal or tetragonal/monoclinic phases supported copper catalysts contain abundant acidic sites and especially the Brønsted acidic sites, which catalyzed mainly the conversion of furfural via the acid-catalyzed routes such as the acetalization, rather than the hydrogenation. The acidic sites over the Cu/ZrO 2 catalyst played more predominant roles than the hydrogenation sites in determining the conversion of the organics like furfural and vanillin.
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
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2019
·
IF 3.372
Piao Liu,Jianxin Cao,Zheng Xu,Chunliang Yang,Xiaodan Wang,Fei Liu
Core-shell structured ZSM-5@t-ZrO 2 catalysts were prepared by a hydrothermal coating method, and their physicochemical properties, catalytic performance, and deactivation behavior in thiolation reactions were studied using a ZSM-5/t-ZrO 2 physically-blended catalyst as a comparison. Reactions using the core-shell ZSM-5@t-ZrO 2 catalyst were carried out at a pressure of 0.7 MPa, 370 °C, a H 2 S:CH 3 OH molar ratio of 2:1, and a N 2 flow rate of 90 ml·min −1 . The conversion of CH 3 OH, and the selectivity and yield of CH 3 SH under these conditions were 92.07%, 90.89%, and 83.68%, respectively, and the catalytic lifetime was longer than 30 h. Compared with the ZSM-5/t-ZrO 2 physically-blended catalyst, the CH 3 SH yield and the catalytic lifetime of the core-shell structured ZSM-5@t-ZrO 2 catalyst were higher by 5.37% and 150%, respectively. The unique reaction pathway of the shell (t-ZrO 2 , Lewis (L) base active site)-core (ZSM-5, Brǿnsted (B) acid active site) and the Lewis-Brønsted acid active center based on a composite solid-solution interface were mainly responsible for the high activity of the thiolation reaction. Meanwhile, the formation of a micro-mesoporous system increased the diffusion of molecules and reduced the deactivation rate of carbon- and sulfur-containing deposits. Generally, carbon- and sulfur-containing substances deposited on catalysts were mainly composed of polymethylbenzene, polymethyl naphthalene, cyclic elemental sulfur, and other compounds containing C S and S S bonds. Finally, the core-shell structured catalysts showed excellent resistance to deactivation by carbon- and sulfur-containing deposits.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Zhuping Li,Yong Men,Shuang Liu,Jinguo Wang,Keye Qin,Dandan Tian,Tianle Shi,Li Zhang,Wei An
The crystalline phases of support have great influence on their surface and structure properties. Therefore, adjusting the crystalline structure of heterogeneous catalysts imposes a significant impact on the catalytic performance. Herein, a suite of Pd/In 2 O 3 /ZrO 2 catalysts with different crystalline phases of ZrO 2 were prepared and evaluated for CO 2 hydrogenation to CH 3 OH using the same amount of metal loading. The activity data showed the distinct superior reactivity of Pd/In 2 O 3 /ZrO 2 catalyst used mixed monoclinic and tetragonal phases ZrO 2 (Mix-ZrO 2 ) as support as compared to respective single phase of monoclinic ZrO 2 (m-ZrO 2 ) and tetragonal ZrO 2 (t-ZrO 2 ). The catalysts are extensively characterized through BET, XRD, HRTEM, UV–vis, H 2 -TPR, CO 2 /H 2 -TPD and XPS. Combining the characterization results and activity data, the superior activity of Pd/In 2 O 3 /Mix-ZrO 2 catalyst can be correlated with large particle size of Pd nanoparticles, the concentration of oxygen vacancies, and the abundant medium basic sites, which were essential for activation of H 2 and inert CO 2 and enhancement of catalytic performance. The best-performing Pd/In 2 O 3 /Mix-ZrO 2 catalyst exhibited a remarkable reactivity with space time yield (STY) of 0.54 g methanol ·h −1 ·g cat −1 at 573 K and 5 MPa, and stability without noticeable deactivation after 100 h of time on stream, demonstrating its potential as catalyst used in CH 3 OH synthesis from CO 2 hydrogenation.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子