CHINESE JOURNAL OF CATALYSIS
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2016
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IF 2.628
Cheng Wang,Liya Hu,Meiyin Wang,Yuanhang Ren,Bin Yue,Heyong He
A series of graphitic carbon nitride supported vanadium catalysts ( x V/g-C 3 N 4 ) with different vanadium contents ( x /%) were prepared by impregnation. XRD, FT-IR, TEM, TG-DTG, nitrogen adsorption and XPS characterizations were conducted which revealed a strong interaction between the vanadium species and g-C 3 N 4 support. 8V/g-C 3 N 4 exhibited the highest activity and showed stable recyclability in the benzene hydroxylation reaction with a benzene conversion of 24.6% and phenol selectivity of 99.2% under the optimized conditions. The excellent catalytic performance of x V/g-C 3 N 4 was due to the integration of vanadium species with high catalytic activity and the g-C 3 N 4 support in their interaction with the benzene substrate
研究领域:
催化化学
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材料科学
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DOI
高影响因子
Royal Society Open Science
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2018
·Vol. 5
·期 6
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IF 2.504
Cheng Wang,Liya Hu,Meiyin Wang,Bin Yue,Heyong He
A series of Cex-V-g-C3N4 catalysts with different cerium content were synthesized by a facile co-assembly method. Compared with pure V-g-C3N4 catalyst, the addition of cerium facilitated the high dispersion of vanadium species as well as the benzene adsorption ability of the corresponding catalysts. Also, the existence of cerium promoted the partial reduction of vanadium species, which improved the redox property of vanadium species as the active centres. The Cex-V-g-C3N4 catalysts showed considerably improved activity in the benzene hydroxylation reaction compared with V-g-C3N4 catalyst. Among the catalysts studied, Ce0.07-0.07 V-g-C3N4 exhibited the best catalytic activity with a benzene conversion of 33.7% and a phenol yield of 32.3% with good structural and catalytic stability, while only 24.7% of benzene conversion and phenol yield of 24.2% were obtained over 0.07 V-g-C3N4.
研究领域:
化学工程
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催化材料科学
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DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Rui Feng,Zhou Fang,Runxi Zhang,Xiaoyan Hu,Tianbo Li,Wei Zhou,Feifei Yang,Xinlong Yan,Shijian Lu
Direct hydroxylation of benzene to phenol is a more environmentally friendly way to generate phenol compared with the traditional method. This study developed vanadium-modified hollow-structured titanium silicate-1 (TS-1) as a catalyst for the effective hydroxylation of benzene to phenol under moderate conditions using hydrogen peroxide as an oxidant. The synthesis of TS-1 zeolites has been improved using traditional hydrothermal, crystal seed, and dissolution–recrystallization techniques. Compared with conventional TS-1, hollow-structured TS-1 exhibited a higher mesopore volume and surface area. Later, vanadium doping increased the charge density associated with the framework Ti centers and acid site content. In the radical reaction process, the adsorption and activation of benzene on highly reactive Ti–OOH intermediates, as well as the improvement of performances toward benzene hydroxylation to phenol, were facilitated by the increase in the concentration of open active centers and acid and electron characteristics.
研究领域:
催化化学
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环境科学
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材料科学
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DOI
高影响因子
ChemNanoMat
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2024
·Vol. 10
·期 8
·e202400240
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IF 2.6
Xuetong Xu,Xu Jia,Cong Liu,Jiaolong Qiao,Fuying Wang,Liuxue Zhang,Dan Yang,Yuan Zhang,Xiulian Wang
The photocatalytic hydroxylation of benzene to phenol is an important reaction for the synthesis of fine chemicals and pharmaceuticals. However, the development of efficient and selective photocatalysts for this reaction remains a challenge. Here, a highly active and selective Fe-MOF/2D-montmorillonite (Fe-MOF/MMT) photocatalyst was prepared via an in-situ method for the hydroxylation of benzene to phenol under the visible light irradiation. The Fe-MOF/MMT composite exhibited excellent photocatalytic performance, with phenol yield of 30.3 % and benzene selectivity of 96.5 % within 4 hours. The high activity and selectivity of the Fe-MOF/MMT photocatalyst were attributed to the synergistic effect between the Fe-MOF and MMT, as well as the unique 2D structure of MMT, which facilitated charge separation and transfer. The Fe-MOF/MMT composite also showed good stability and re-used without significant decrease of activity. This study demonstrated that the potential of Fe-MOF/MMT as a highly efficient and selective photocatalyst for the hydroxylation of benzene to phenol and provided an insight into the design of advanced photocatalysts for sustainable chemical synthesis.
研究领域:
材料科学
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环境化学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2013
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IF 3.41
Hua Yang,Qing Wu,Jun Li,Wen Dai,Hengyun Zhang,Dan Lu,Shuang Gao,Wansheng You
A novel catalyst, [Mo 2 V 2 O 9 (bpy) 6 ][PMo 11 VO 40 ], was synthesized by the self-assembling of [PMo 11 VO 40 ] 4− and [Mo 2 V 2 O 9 (bpy) 6 ] 4+ unit and characterized by elemental analyses, TG, IR, X-ray powder diffraction and X-ray single crystal diffraction. [Mo 2 V 2 O 9 (bpy) 6 ][PMo 11 VO 40 ] with multi-isolated active sites showed good catalytic activities for hydroxylation of benzene to phenol . A high yield of phenol (25.5%) with selectivity to phenol of 90.7% was obtained using H 2 O 2 as oxidant. The catalyst can be recycled for 5 times while its structure was unchanged and its catalytic activity was maintained.
研究领域:
化学
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催化材料科学
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DOI
高影响因子
NANO
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2018
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IF 1.1
Qiang Sun,Long Liu,Yi-Ding Li,Zeng-Rong Wang,Xue Zhang
We report engineered iron-based nanoparticles supported on cagelike mesoporous carbon that leaves its most mesopores empty to retain an open pore network and are expected to be efficient catalyst with fast molecular diffusion/transportation. The nano-scale iron-based particle inlayed in mesoporous carbon catalyst was obtained via the introduction of N atoms as an anchor. Results of X-ray diffraction, N 2 sorption and transmission electron microscopy showed that the cagelike mesoporous structure of the carbon matrix was retained during catalyst preparation and iron-based nanoparticles were spatially dispersed on the mesoporous carbon. Importantly, it was found that the obtained iron-based nanoparticles inlayed into mesoporous carbon with a low Fe loading of 1.26 wt.% was an appropriate catalyst for the benzene hydroxylation to phenol using H 2 O 2 as the oxidant. At a low temperature of 30 ∘ C, 19.4% conversion to benzene and 14.6% phenol yield were obtained; in addition, the catalyst could be recycled at least four times.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Jie Wu,Xiaoyu Bai,Jianbo Yang,Siman Li,Hua Mei,Yan Xu
Phenol, as an important industrial raw material, the traditional three-step method for preparing phenol has drawbacks such as numerous by-products and difficulties in oxidation. In this regard, we use nitrogen-containing cations that can make conjugated π electrons more active to assemble with Keggin-type polyoxometalates with excellent redox properties, which can not only enable Keggin-type polyoxometalates to obtain the catalytic performance of activated benzene rings, but also increase their stability in organic solvents. Therefore, we synthesized three zero-dimensional compounds ((C 10 H 10 N 2 ) 2 [HPMo VI 9 V V 3 O 40 (FeH 2 O) 0.5 ].1.5H 2 O ( 1 ), (C 7 H 10 N 4 ) 2 [H 3 PMo VI 8 V V 4 O 40 ] ( 2 ), (C 9 H 8 N) 3 [PMo VI 8 Mo V 4 V IV 2 O 42 ] ( 3 )) through simple hydrothermal and solvothermal methods using different nitrogen-containing cations and molybdovanadate. Structural analysis indicates that these three compounds are structurally similar, each consisting of its own molybdovanadate anion and protonated organic counter cations. The experiment demonstrated that compound 3 had a yield of 11.2 % and a selectivity of 93 % for phenol at 60°C. To further explore the oxidation performance of the compound, we selected different sulfides for oxidation experiments and found that it could completely oxidize sulfur-containing substances (such as BT) at 90°C. This indicates that the idea of combining molybdovanadate and nitrogen-containing organic cations has a promising application prospect in the benzene hydroxylation and Sulfur oxidation.
研究领域:
无机化学
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催化化学
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有机反应
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材料化学
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环境化学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Yuzhou Wu,Xubin Zhang,Fumin Wang,Yi Zhai,Xianbao Cui,Guojun Lv,Tao Jiang,Jiaqi Hu
Direct hydroxylation of benzene to phenol is an effective and environment-friendly route to obtain phenol. Herein, Fe-doped and cupric acetylacetonate [Cu(acac)2]-grafted mesoporous silica (Cu/Fe-SBA-15) with highly dispersed metallic sites has been synthesized and used as a heterogeneous catalyst in the hydroxylation of benzene. The physiochemical properties of the synthesized materials as well as the reciprocity between iron and copper sites were analyzed by several characterization techniques including nitrogen adsorption–desorption, X-ray diffraction, transmission electron microscopy, UV–vis diffuse reflectance spectroscopy, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. In direct hydroxylation of benzene with H2O2 as the oxidant, the prepared Cu/Fe-SBA-15 material showed great catalytic activity. Moreover, the synergistic effect between doped Fe sites and grafted Cu sites was also investigated. In this catalyst, Fe and Cu species both played the role of active sites. Excessive activity of iron would lead to benzene peroxidation, while the presence of copper sites could effectively hinder benzene peroxidation.
研究领域:
催化化学
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材料科学
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环境化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Tao Chen,Fangpei Ma,Zhe Chen,Menglin Xie,Ting Li,Yu Zhou,Jun Wang
Solar-driven benzene oxidation with dioxygen (O 2 ) provides a green and sustainable alternative for phenol production, but the construction of heterogeneous photocatalysts remains a huge challenge for efficient conversion under visible light irradiation and ambient conditions. Herein, we reported a facile microwave assisted strategy for the defect engineering of two-dimensional (2D) tungsten oxide while well maintaining the original crystalline architecture. Abundant oxygen vacancies were constructed on the 2D tungsten oxide, which remarkably promoted photochemical (light harvesting, charge separation and transfer) and O 2 activation behaviors, this promotion effect was further strengthened by the hybridization with Pt species with the formation of Schottky junction. The champion catalyst enabled a high phenol yield of 11.3% with a selectivity of 91% in the visible-light-driven benzene hydroxylation with atmospheric O 2 at room temperature. The catalyst can be facilely recovered and reused with stable activity. The oxygen vacancies and Pt co-catalyst were demonstrated to play vital roles in the photocatalytic formation of the reactive oxygen species (hydroxyl radials, ·OH) for effective oxidation.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
JOURNAL OF POROUS MATERIALS
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2024
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IF 2.5
Xue Changhao,Hou Xiaohui,Sun Weijie,Yuan Xia
The acidic molecular sieve carrier Hβ supported non-noble metal catalyst Ni/Hβ was prepared by equal volume impregnation method and applied to the hydroalkylation of benzene to cyclohexylbenzene. The effects of calcination procedures on the particle size of Ni and the dispersion degree of metal on the carrier were investigated. Compared with the samples reduced by hydrogen after calcination, the active site Ni of Ni/Hβ obtained by direct thermal reduction in hydrogen is mainly dispersed on the surface of the carrier, with better metal dispersion and smaller particle size of Ni. Under the optimized reaction conditions, the initial pressure of H 2 is 2.5 MPa, the amount of catalyst is 4% of the total reaction liquid, and at the reaction temperature 190 °C for 3 h, the conversion of benzene is 38.4%, the selectivity of cyclohexylbenzene is 72.8%, the selectivity of cyclohexane is 5.2%, the selectivity of dicyclohexylbenzene is 16.5%, and the selectivity of other by-products decreased to 5.5%. After the catalyst was reused for 5 times, the conversion of benzene and selectivity of cyclohexylbenzene were both have a slight decrease. Characterization results showed that the structure of the recovered catalyst was stable, but the specific surface area and pore volume decreased significantly, the resulted problem of catalyst pore blockage can be restored through calcination treatment.
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
Molecular Catalysis
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2021
·
IF 5.062
Mengzhe Li,Xiaohua Shen,Miaoqing Liu,Jianjun Lu
L-lysine is used as a crystallization regulator, and a two-step synthesis method is adopted in a concentrated gel system, which provides a new route to synthesize of nano-sized TS-1 zeolite. The new synthesis strategy was used to successfully synthesize TS-1 zeolite with a particle size less than 100 nm. The rate of crystal nucleation is faster than the crystal growth at the low temperature in the first step. Introduction of L-lysine can prevent crystal growth to form nano-sized TS-1 zeolite at the high temperature in the second step. Meanwhile, L-lysine decrease the pH value of the gel system, which is favorable for Ti atoms to incorporate the TS-1 framework. TS-1 nanozeolite can effectively reduce the diffusion resistance, and nanozeolite has a large specific surface area and high stability. Therefore, TS-1 nanozeolite exhibits the excellent catalytic performance during the hydroxylation of benzene. The conversion of benzene has been greatly improved and the types of by-products are effectively reduced. The conversion of benzene reached 50.2%, and the yield of phenol was 30.8% without by-product benzoquinone. TS-1 nano-zeolite as a catalyst for benzene hydroxylation shows great potential in industrial application.
研究领域:
化学工程
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材料科学
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催化化学
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产品关联
DOI
高影响因子
ACS Catalysis
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2015
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IF 9.312
Dengke Wang,Mengtao Wang,Zhaohui Li
Phenol is one of the most important chemicals in industry. One-step selective benzene hydroxylation is an attractive yet challenging method for phenol production, especially when such a reaction can be driven by solar energy. Herein, we reported that a highly selective benzene hydroxylation to phenol can be achieved over two Fe-based metal–organic frameworks [MIL-100(Fe) and MIL-68(Fe)] under visible light irradiations using hydrogen peroxide (H2O2) as an oxidant. An optimal benzene conversion of 30.6% was achieved with a H2O2:benzene ratio of 3:4 over MIL-100(Fe) after 24 h irradiations. ESR results and the kinetic studies suggested that a successful coupling of the photocatalysis of Fe–O clusters in Fe-based metal–organic frameworks (MOFs) with a Fenton-like route is involved in this benzene hydroxylation process. The comparison of the reaction over MIL-100(Fe) and MIL-68(Fe) reveals that the structure of MOFs significantly influences the photocatalytic efficiency. Because the composition and the structure of MOFs are highly tunable, this study highlights the great potential of using Fe-based MOFs for photocatalytic benzene hydroxylation to form phenol, which may result in an economical, sustainable, and thus green process for phenol production.
研究领域:
化学工程
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材料科学
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环境化学
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光化学
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DOI
高影响因子
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