Journal of Energy Chemistry
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2014
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IF 0
Hongyan Li,Hong Ma,Xinhong Wang,Jin Gao,Chen Chen,Song Shi,Minjie Qu,Na Feng,Jie Xu
Efficient catalytic oxidation of ethylbenzene to acetophenone was realized using the catalytic system of cobalt zeolitic imidazolate framework ZIF-67/N-hydroxyphthalimide (NHPI) under mild conditions. 95.2% conversion of ethylbenzene with 90.3% selectivity to acetophenone could be obtained at 373 K under 0.3 MPa O 2 for 9 h. The results show that there exists synergetic effect between ZIF-67 and NHPI. 1-Phenylethyl hydroperoxide (PEHP) was generated via a radical process involving the hydrogen abstraction from ethylbenzene by phthalimide N-oxyl, and subsequently effectively decomposed to acetophenone by ZIF-67.
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
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2015
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IF 3.615
Qiming Zhao,Kexian Chen,Wensong Zhang,Jia Yao,Haoran Li
A metal- and initiator-free catalytic system comprising N -hydroxyquinolinimide (NHQI) and 4-carboxyl- N -hydroxyphthalimide (Car-NHPI) was developed for the oxidation of ethylbenzene using molecular oxygen as the terminal oxidant. The catalytic activity of Car-NHPI/NHQI catalytic system was higher than that of Car-NHPI or NHQI alone. The high catalytic performance of Car-NHPI/NHQI catalytic system could be attributed to the dual interactions of radical exchange and acid-base neutralization, which resulted in the increment of the conversion of ethylbenzene up to 70% and the selectivity of acetophenone up to 66% at 120 °C under 1 atm O 2 for 15 h.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
Molecular Catalysis
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2021
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IF 5.062
Dong Ji,Nan Xi,Guixian Li,Peng Dong,Hongwei Li,Hui Li,Chunqiang Li,Ping Wang,Yu Zhao
In this study, a series of Co–Ni–Al–layered double hydroxides (Co x Ni y Al 1 –LDHs) was successfully prepared via a simple co-precipitation method with Na 2 CO 3 and NaOH as the precipitants. After the calcination of the Co x Ni y Al 1 –LDH precursors, the Co–Ni–Al–O mixed oxides were formed and used as highly efficient catalysts in the selective oxidation of ethylbenzene to acetophenone. The Ni addition to CoAlO x can induce the formation of interactions between Co–Ni species and affect the dispersion of metal active centers, thereby greatly influencing the catalytic performance. The typical Co 2 Ni 1 Al 1 O x sample with a Co:Ni molar ratio of 2:1 exhibited the highest surface area (165 m 2 /g) and the best catalytic performance (80.0% ethylbenzene conversion and 88.9% acetophenone selectivity). The high catalytic efficiency was mainly attributed to the high-efficiency synergistic effect between the highly dispersed active center Co and the promoter Ni species. More importantly, the good recyclability and stability of the Co 2 Ni 1 Al 1 O x catalyst made it more competitive.
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
Molecular Catalysis
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2019
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IF 2.938
Zhijie Wang,Anxiang Guan,Mayfair C. Kung,Anyang Peng,Harold H. Kung,Ximeng Lv,Gengfeng Zheng,Linping Qian
Aerobic oxidation of α-C H bond of organic compounds to valuable chemicals is widely investigated in both fundamental research and industry. Due to the good stability of molecular oxygen, severe reaction conditions are generally required. Herein, by in situ synthesis we used molecular oxygen to induce cobalt nanoclusters with the sensitive catalysis in mild selective oxidation. The cobalt containing clusters with an average diameter around 0.9 nm are in situ prepared in the presence of cis -cyclooctene epoxidation and cyclooctene dimer oxide is formed at the interface to stabilize Co clusters with electron donation as an oil-soluble surfactant. The soluble clusters exhibit high activity in selective oxidation of α-C H bond of ethylbenzene into acetophenone and turnover number (TON) reaches about 7 × 10 4 during 50 h’ reaction at 373 K, which is around 960 times more active than the one using CoCl 2 salt as the catalyst, resulting from efficient mass transportation, π bond interaction and oxygen gas activation. Extended work based on this understanding demonstrates that cobalt nanoclusters also effectively catalyze aerobic oxidation of cyclohexene.
研究领域:
化学催化
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有机合成
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Arabian Journal of Chemistry
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2020
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IF 4.762
Kechen Song,Shuo Wang,Qiang Sun,Deping Xu
Nano-sheets Al 2 O 3 supported CeO 2 -Fe 2 O 3 binary oxides were prepared by the vacuum impregnation method. The structural and textural properties were characterized by pertinent techniques, and the materials were evaluated as catalysts for the oxidative dehydrogenation of ethylbenzene with carbon dioxide (CO 2 -ODEB). The characterization results show that all samples maintain the hierarchical structure, and CeO 2 -like and Fe 2 O 3 -like solid solutions were formed when changing the Ce-to-Fe molar ratio. The catalytic performances indicate that CeO 2 -Fe 2 O 3 binary oxides were effective for CO 2 -ODEB, and the activity is determined by mobile oxygen, which can facilitate the dehydrogenation process. The DFT studies further identified the reaction pathway and rate-determining step. The inter-transmission of oxygen species and the presence of CO 2 refill the oxygen vacancies and restore the redox cycle of CeO 2 -Fe 2 O 3 binary oxides.
研究领域:
催化化学
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材料科学
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理论计算化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
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IF 3.9
Ziyi Wang,Changyan Guo,Kefu Wang,Jiang Li,Jide Wang
Upgrading waste PET to prepare metal–organic frameworks (MOF) through chemical recycling provides new ideas and methods for PET recycling treatment and high value-added conversion. In this paper, Cobalt-based metal–organic frameworks (Co-MOF) were prepared from PET by one-pot solvothermal method without adding acids or bases. The prepared Co-MOF was used as a heterogeneous catalyst to catalyze the selective oxidation of ethylbenzene (EB) for the preparation of acetophenone (AP). When only tert-butyl hydroperoxide (TBHP) was used as the oxidizing agent without any additional solvents, 89% EB conversion and 94% AP selectivity were achieved, respectively. Moreover, the catalyst showed excellent stability with no significant deactivation under 5 cycles. In addition, the synthesized Co-MOF-10 also exhibits impressive conversion rates of 96% and 93% in benzyl alcohol and styrene oxidation, respectively. Compared with the Co-MOF prepared by commercial terephthalic acid (BDC), the Co-MOF-10 synthesized via the one-pot method using PET exhibits enhanced cost-effectiveness, environmental sustainability, and superior catalytic performance. The present study establishes a foundation for the conversion of plastic PET into valuable MOF and its subsequent application in C–H bond oxidation.
研究领域:
化学工程
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环境科学
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材料科学
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产品关联
DOI
高影响因子
CHINESE JOURNAL OF CHEMISTRY
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2021
·Vol. 39
·期 9
·2563-2569
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IF 6
Yue-Ran Wang,Jian Sheng,Wen-Duo Lu,Bing Yan,An-Hui Lu
Main observation and conclusion Oxidative dehydrogenation of ethylbenzene is considered as an alternative route to styrene because of its exothermic and irreversible reaction nature, but encounters low styrene selectivity due to the deep-oxidation over metal oxide-based catalysts. Herein, we reported that a metal-free boron-based catalyst consisting of boron phosphate and boron nitride (BPO 4 /BN) exhibited high activity and selectivity in oxidative dehydrogenation of ethylbenzene to styrene. High selectivity of styrene (95.1%) was achieved at 27.7% ethylbenzene conversion level over the optimized BPO 4 /BN catalyst. The tetra-coordinated boron (BO 4 ) species of BPO 4 was speculated to be responsible for the ODH of ethylbenzene, and a synergistic effect between BPO 4 and BN can remarkably improve the catalytic performance of the BPO 4 /BN catalyst. The optimized BPO 4 /BN catalyst showed a higher styrene formation rate of 4.0 mmol g cat −1 ·h −1 , compared individually to BPO 4 (2.8 mmol·g cat –1 ·h –1 ) and BN (0.5 mmol·g cat –1 ·h –1 ).
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
Journal of Physical Chemistry C
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2022
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IF 4.177
Yuemiao Lai,Zhengtian Pu,Peng Liu,Fangliang Li,Jie Zeng,Xueming Yang,Qing Guo
The low-temperature C–H bond activation of alkanes remains a big challenge in alkane dehydrogenation. In this work, ethylbenzene (EB) oxidative dehydrogenation has been investigated on rutile(R)-TiO2(110) under both ultrahigh vacuum (UHV) and ambient conditions. Under UHV conditions, styrene is produced with nearly 100% selectivity in a stepwise manner, in which the first C–H bond dissociation of EB occurs at <285 K with the help of surface O22– species, followed by the second C–H bond dissociation at about 400 K. However, styrene, acetophenone, and 2,3-diphenylbutane products are produced from EB oxidative dehydrogenation under ambient conditions, suggesting that α-H dissociation is the initial step of EB oxidative dehydrogenation. This may be also possible for EB oxidative dehydrogenation on R-TiO2(110) under UHV conditions. The different pathways of EB oxidative dehydrogenation under UHV and ambient conditions may originate from different intermediates and O2 concentrations. This work provides new insight into the fundamental understandings of the low-temperature C–H bond activation of alkyl chains of aromatic hydrocarbons, which may promote the development of new catalysts for efficient styrene production from EB oxidative dehydrogenation under mild conditions.
研究领域:
催化化学
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表面科学
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产品关联
DOI
高影响因子
MATERIALS RESEARCH BULLETIN
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2014
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IF 1.968
Shi Li,Shang-Ru Zhai,Qing-Da An,Ming-Hui Li,Yu Song,Xiao-Wei Song
The preparation of Co(II) supported magnetic heterogeneous catalyst, i.e. Fe 3 O 4 @SiO 2 –NH 2 @CS–Co, and its efficient and selective catalytic properties toward the oxidation of ethylbenzene to acetophenone are presented. The materials were characterized by various physicochemical techniques such as scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, vibrating sample magnetometer, elemental analysis, inductively coupled plasma-atomic emission spectrometer and X-ray photoelectron spectroscopy, etc. The reaction conditions were thoroughly investigated and highly improved catalytic performance (82.5% conversion of ethylbenzene and 80.1% selectivity to acetophenone) was gained under more mild reaction conditions of lower temperature (70 °C), shorter reaction period (60 min) and cheaper and greener oxygen source (H 2 O 2 ). More importantly, it could be reused successively at least 10 times when more than 80% of its catalytic activity maintained.
研究领域:
材料科学
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催化化学
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环境化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Kaiyi Su,Chaofeng Zhang,Yehong Wang,Jian Zhang,Qiang Guo,Zhuyan Gao,Feng Wang
ABSTRACT Although different NbO x units are present in Nb 2 O 5 -based catalysts, the correlations between these structures and activity remain unclear, which considerably hinders the further development of Nb 2 O 5 photocatalysis . Herein, we utilized N- hydroxyphthalimide (NHPI) as the probe molecule to distinguish the role of different NbO x units in the activation of C–H bond under visible light irradiation. With the addition of NHPI, Nb 2 O 5 catalysts with highly disordered NbO 6 units exhibited higher activities than that with slightly disordered NbO 6 units (419–495 vs . 82 μmol·g −1 ·h −1 ) in photocatalytic selective oxidation of ethylbenzene . Revealed by Raman spectra, electron paramagnetic resonance spectra, and transmission-electron-microscopy images, highly disordered NbO 6 units were confirmed to act as the active sites for the transfer of photogenerated electrons from NHPI, promoting the generation of phthalimide- N -oxyl (PINO) radicals for the enhanced conversion of ethylbenzene under visible light irradiation. This study provides guidance on the role of local NbO x units in Nb 2 O 5 photocatalysis.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Zhihui Liu,Siyuan Sun,Fan Yang,Hongchen Liu,Yang Sun,Na Ta,Ge Zhang,Sai Che,Yongfeng Li
Transition metal-based (Fe, Co, Cu, etc.) single-atom catalysts (SAC) have been widely used in the direct oxidation of ethylbenzene and benzene. However, their catalytic performance is limited by the low metal loading. Compared with traditional SAC, dual site single-atom catalysts (DSAC) show the advantages of abundant active sites, high metal loading, and excellent catalytic performance. Herein, a novel Fe/Cu N C DSAC was prepared by facile one-pot pyrolysis of formaldehyde, dicyandiamide, and metal salts. Dicyandiamide acted as the carbon source with advantage of high nitrogen content, which promoted the formation of metal centers and increased the metal loading. Meanwhile, the synergistic effect between Fe and Cu active centers was revealed to adjust the coordination environment, thus improving the catalytic activity of oxygen activation. The synthesized Fe/Cu N C DSAC demonstrated superior catalytic performance in ethylbenzene oxidation reaction with O 2 as a green oxidant under mild reaction conditions, with a 99 % conversion of acetophenone and no significant degradation of activity after 10 circles. In addition, NaCl was added into the synthesis as a template to adjust the pore structure, and the modified Fe/Cu N C DSAC showed excellent performance in benzene oxidation reaction with high product conversion. In conclusion, this work paves the way for the construction of efficient, green, and cost-effective catalysts for the direct oxidation of ethylbenzene and benzene.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）