Molecular Catalysis
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2021
·
IF 5.062
Yue Zhang,Zhiyong Pan,Nan Wang,Li Wang
Silica SBA-15 without removal of template P123 was calcined in an inert atmosphere and the carbon-modified SBA-15 thus obtained was used as the support of Pd catalyst for the hydrogenation of 2-ethylanthraquinone (EAQ). The effects of extraction times of P123 in SBA-15 with water prior to inert calcination and calcination temperature on the structure and catalytic performance of Pd catalyst were studied. The results of elemental analysis, X-ray diffraction, X-ray photoelectron spectroscopy, inductively coupled plasma, Fourier transform infrared spectroscopy, Raman spectra, water contact angle measurement, N 2 adsorption-desorption, transmission electron microscopy and energy dispersive X-ray mapping showed that carbon content of catalysts varied in the range of 3.4 % and 1.1 % with increasing extraction times from 0 to 6 due to the decrease in the residual amount of P123 in uncalcined SBA-15. With rising calcination temperature, the occurrence state of carbon in catalysts was converted from amorphism into graphite. The Pd catalyst supported on SBA-15 extracted for 3 times and calcined at 650 °C had 2.0 % carbon, and exhibited the highest activity (0.37 molH 2 ·gPd −1 ·min −1 ) and selectivity (98.9 %). This is due to the presence of appropriate amount of carbon, which provided a relatively high hydrophobicity without significantly reducing the specific surface area and pore size of SBA-15 support. The high hydrophobicity benefits the adsorption of EAQ from the working solution to the surface of catalyst.
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
JOURNAL OF MOLECULAR LIQUIDS
·
2019
·
IF 4.561
Hongxin Bai,Xiangchen Fang,Chong Peng,Quanjie Liu,Weibin Xie,Liming Jia,Zhaoyang Song
Alkylated anthraquinone is widely used as promising redox-active materials for both redox flow batteries technology and hydrogen peroxide production via anthraquinone oxidation (AO) process, yet its inadequate solubility in solvents has been the one of the main limitations resulting to insufficient energy density of working solution. In present study, solubility of 2-ethylanthraquinone was specifically investigated by the synthetic method at the temperature range from 304.15 to 344.15 K under the pressure of 101.325 kPa. In support for decent working solution exploit, various types of solvents were specifically selected as the working solution constituent in this work. Solubility data and activity coefficient of 2-ethylanthraquinone were correlated by modified Apelblat and λ-h models. Furthermore, thermodynamic analysis was subsequently performed based on the thermodynamic fitting results. As a result, dissolution process of 2-ethylanthraquinone is endothermic and entropy-driven in these neat solvents, higher dissolution temperature leads to smaller value of partial molar excess Gibbs free energy and therefore results to a greater solubility.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 152
·期 5
·1495-1505
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IF 3.186
Zhang Yue,Wang Li,Ma Qingqing,Wang Nan,Pan Zhiyong
SBA-15 was modified via post-treatment with (NH 4 ) 2 SiF 6 and (NH 4 ) 3 AlF 6 solution (NSF-T and NAF-T) and applied as support of Pd catalysts for the hydrogenation of 2-ethyl-anthraquinone (EAQ). The characterization results revealed that F could be incorporated into the framework of SBA-15 by forming Si–F bond and the amount of F increased as the molar ratio of F in treating solution to Si species in SBA-15 (F/Si) increased from 0.1 to 0.4 for NSF-T and 0.3 to 0.6 for NAF-T. At the same F/Si, the incorporated amount of F was larger with NSF-T than with NAF-T, and the latter could simultaneously create acid sites in catalysts. The hydrophobicity of catalysts could be effectively improved by incorporating F into SBA-15 supports, which favored the catalytic performance. The catalyst on SBA-15 treated by NSF with F/Si of 0.3 exhibited the high initial activity (0.24 molH 2 ·gPd −1 ·min −1 ) and selectivity (95.5%). Graphic Abstract
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
CATALYSIS LETTERS
·
2017
·Vol. 147
·期 7
·1802-1810
·
IF 2.799
Hong Runrun,He Yufei,Miao Chenglin,Feng Junting,Li Dianqing
Abstract Pd–Ir mesocrystals with rough surface and highly branched structure were synthesized through a facile co-reduction method. The morphology evolution shows the mesocrystals were formed by oriented attachment of nanoparticles, and abundant defects sites as well as synergetic effect between building units were formed during mesocrystals oriented attachment process. Therefore, the supported Pd–Ir mesocrystals show a significant enhancement in catalytic performance in hydrogenation of 2-ethylanthraquinone compared with conventional Pd–Ir nanoparticles. The high activity can be ascribed to high densities of defect sites in Pd–Ir MCs catalyst, which facilitated H 2 activation. In addition, the geometric effect of Pd–Ir MCs catalyst was responsible for inhibiting further hydrogenation of eAQH 2 to undesired consecutive byproducts. Graphical Abstract
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
MICROPOROUS AND MESOPOROUS MATERIALS
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2018
·
IF 3.649
Qingqing Ma,Nan Wang,Guozhu Liu,Li Wang
Pd catalysts on mesoporous silica SBA-15 functionalized with alkyltriethoxysilane (alkyl = methyl, ethyl, propyl and isobutyl) were prepared. The effects of grafting sequence on the grafting amount were studied. The catalysts were characterized by XRD , FT-IR, elemental analysis , thermogravimetric analysis , nitrogen adsorption-desorption, TEM and XPS , and evaluated using catalytic hydrogenation of 2-ethyl-anthraquinone. The grafting amount increases with increasing the alkyl chain length of alkyltriethoxysilane. The highest grafting amount with the carbon content of 1.56% is obtained using an ante-grafting procedure where the grafting is performed prior to the removal of template, and this catalyst shows the highest activity and selectivity (98.3%). The accordant relationship between the activity of Pd/SBA-15 catalysts and their grafting amount indicates a positive effect of hydrophobicity of SBA-15 created by grafting on the catalytic hydrogenation of 2-ethyl-anthraquinone.
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
CHINESE JOURNAL OF CATALYSIS
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2018
·
IF 3.525
Yanyan Guo,Chengna Dai,Zhigang Lei
We studied the hydrogenation of 2-ethylanthraquinone (eAQ) over Pd/SiO 2 /COR (COR = cordierite) monometallic and Pd-M/SiO 2 /COR (M = Ni, Fe, Mn, and Cu) bimetallic monolithic catalysts, which were prepared by the co-impregnation method. Detailed investigations showed that the particle sizes and structures of the Pd-M (M = Ni, Fe, Mn, and Cu) bimetallic monolithic catalysts were greatly affected by the second metal M and the mass ratio of Pd to the second metal M. By virtue of the small particle size and the strong interaction between Pd and Ni of Pd-Ni alloy, Pd-Ni bimetallic monolithic catalysts with the mass ratio of Pd/Ni = 2 achieved the highest H 2 O 2 yield (7.5 g/L) and selectivity (95.3%). Moreover, density functional theory calculations were performed for eAQ adsorption to gain a better mechanistic understanding of the molecule-surface interactions between eAQ and the Pd(1 1 1) or PdM(1 1 1) (M = Ni, Fe, Mn, and Cu) surfaces. It was found that the high activity of the bimetallic Pd-Ni catalyst was a result of strong chemisorption between Pd 3 Ni 1 (1 1 1) and the carbonyl group of eAQ.
研究领域:
催化化学
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理论计算化学
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2022
·
IF 4.889
Congcong Ji,Hongyu Wang,Shiqin Sun,Qi Li,Ji-Jun Zou,Shitao Yu,Huibing Shi,Genkuo Nie,Shiwei Liu
2-Ethylanthraquinone is frequently used for producing bulk consuming chemicals. However, the synthesis of 2-ethylanthraquinone is still restricted by expensive raw materials, complex preparation process and poor-cycling catalyst. Herein, a one-pot method is developed to synthesize 2-ethylanthraquinone using phthalic anhydride and ethylbenzene as feedstock by combination of acylation and dehydration over a Sc-modified Hβ catalyst. Sc-modified Hβ was prepared via impregnation and catalyzed conversion of phthalic anhydride about 58.8% and 2-ethylanthraquinone selectivity up to 78.5% which is better than the results by other metals-modified Hβ zeolites. By adjusting Sc loading amount in Hβ, more acids are created especially strong Lewis acid and an appropriate synergistic effect of Lewis/Bronsted acids is obtained for cascade reactions of acylation and dehydration. Then, the reaction conditions were investigated and the catalyst can be reused in 4 runs. This work provides a green and simple way for 2-ethylanthraquinone synthesis.
研究领域:
化学工程
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催化材料科学
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DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Yanyan Guo,Yichun Dong,Zhigang Lei,Zhixue Liu,Jiqin Zhu
The catalytic performance of Pd-N/Silicon Dioxide/Cordierite (Pd-N/SD/C) ( N = Ga and Ag) bimetallic monolithic catalysts for 2-ethylanthraquinone (eAQ) hydrogenation was investigated. Catalyst characterization by HRTEM, XPS, and TPR reveal that Pd-Ga/SD/C can form an alloy structure to produce significant synergetic effects. Moreover, the use of different Pd/Ga mass ratio in catalysts reveals that when the mass ratio of Pd and Ga/Ag = 2:1, Pd-Ga/SD/C obtains the highest yield of H 2 O 2 and selectivity toward active quinones, which can reach 7.4 g L −1 and 90%. Moreover, to have a deep understanding of the eAQ-PdN(1 1 1) or eAQ-Pd(1 1 1) interaction mechanism, the calculation of eAQ adsorption on Pd-N/SD/C catalysts surface was performed by density functional theory (DFT). It is shown that the higher catalytic activity over Pd-Ga/SD/C is due to the stronger carbonyl group of eAQ adsorption on Pd 3 Ga 1 (1 1 1).
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
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DOI
高影响因子
Chemical Engineering and Processing-Process Intensification
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2018
·
IF 2.826
Yanyan Guo,Chengna Dai,Zhigang Lei
A series of Pd-La/SiO 2 /cordierite (cordierite = COR) and Pd-Zn/SiO 2 /COR bimetallic monolithic catalysts were prepared, characterized, and tested for the hydrogenation of 2-ethylanthraquinone (eAQ) as the key step of anthraquinone method for production of H 2 O 2 . It was found that the metal particle size is remarkably dependent on the Pd/M (M = La, and Zn) mass ratio of bimetallic monolithic catalysts. By virtue of its small metal particle size and the strong interaction, the 0.8% Pd-0.4% La/SiO 2 /COR monolithic catalyst presents the highest H 2 O 2 yield (7.7 g L −1 ) and selectivity toward active quinones (95%), which is attributed to the addition of La leading to the synergistic effect between Pd and La. Moreover, the density functional theory (DFT) calculations for the adsorption of eAQ over the surface of Pd-La/SiO 2 /COR and Pd-Zn/SiO 2 /COR bimetallic monolithic catalysts have been conducted to further understand the mechanism of molecule–surface interactions between eAQ and the PdM(1 1 1) or Pd(1 1 1) surfaces. Detailed studies showed that the high catalytic activity of Pd-La/SiO 2 /COR bimetallic monolithic catalyst is attributed to the stronger adsorption between Pd 3 La 1 (1 1 1) and the carbonyl group of eAQ.
研究领域:
催化化学
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材料科学
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理论化学
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DOI
高影响因子
RSC Advances
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2017
·Vol. 7
·期 11
·6447-6456
·
IF 3.108
Jinli Zhang,Kaige Gao,Suli Wang,Wei Li,You Han
A series of bimetallic PdRu catalysts supported on γ-Al2O3 were prepared by incipient wetness impregnation method and were assessed in the 2-ethylanthraquinone hydrogenation process. It is found that the addition of Ru to Pd can improve the catalyst's activity and maintain high selectivity at the same time for 2-ethylanthraquinone hydrogenation. Several analysis techniques including N2 adsorption–desorption, ICP-AES, XRD, TEM, H2-TPR, H2-TPD and XPS were adopted for characterizing the structural and electronic properties of the samples. It is revealed that PdRu bimetallic system shows stronger hydrogen desorption behavior in contrast to the monometallic catalysts. In addition, the higher fraction of Pd2+ and the presence of Ru4+ in the PdRu system may act as the electrophilic sites for the adsorption and activation of the CO of the 2-ethylanthraquinone molecule through the lone electron pair of the oxygen atom. These factors may be attributed to the superior performance of PdRu bimetallic samples for 2-ethylanthraquinone hydrogenation.
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
RESEARCH IN MICROBIOLOGY
·
2022
·
IF 3.946
Yuanyuan Song,Ziqi Wang,Yijing Long,Yang Mao,Feng Jiang,Yuanyuan Lu
Candida albicans can form biofilm on biotic and abiotic surfaces of medical implants to cause superficial and systemic infections under specific condition. The formation of hyphae and matrix of C. albicans are considered as probable virulence factors . We assessed the inhibitory activities of 26 anthraquinones against C. albicans biofilm formation, which were substituted by different functional groups including hydroxyl groups, amino groups, carboxyl groups, alkyl groups, and glycoside groups at C1- or C2-position. Among them, anthraquinones without substituents at other positions but only an alkyl group attached to C2-position, namely 2-alkyl-anthraquinones were determined to have significant anti-biofilm activities. Furthermore, 2-ethylanthraquinone can significantly affect genes related to extracellular matrix ( PMT6 and IFD6 ), and hyphal formation ( HWP1 , ECE1 and EFG1 ), leading to the disrupted formation of biofilm, by detail transcriptomics analysis. We believed that 2-ethylanthraquinone could inspire more discoveries of anti-biofilm agents against C. albicans .
研究领域:
微生物学
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药理学
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分子生物学
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DOI
PubMed
高影响因子
AICHE JOURNAL
·
2025
·Vol. 71
·期 8
·e18862
·
IF 4
Yue Zhang,Rongrong Zhang,Shuzhen Lyu,Xiangwei Ren,Guozhu Liu,Li Wang
Supported Pd-based nanoparticles are widely regarded as the most effective catalysts for 2-ethylthraquinone hydrogenation. Herein, the heteroenergetic dual-supports were prepared by coating resorcinol-formaldehyde (RF) resin on mesoporous SBA-15 to regulate the growth and surface microenvironment of Pd. After calcination and reduction, phenolic hydroxyl groups in the residual carbon layer effectively reduced the Pd particle size, induced the formation of adjacent Pd 0 –Pd δ+ , and created hydrophobicity. Density functional theory calculations revealed that Pd atoms preferentially interact with OH on C, rather than with OH on SBA-15, providing an intrinsic driving force for smaller Pd particle size. The mass ratio of RF to SBA-15 was shown to be a crucial parameter affecting the catalytic performance. At the ratio of 4 (carbon content of 2.02%) the catalyst possesses the smallest Pd particles, 30% Pd δ+ proportion, and higher hydrophobicity, achieving the best catalytic performance, with an activity of 0.57 molH 2 ·gPd −1 ·min −1 and a selectivity of 95.3%.
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高影响因子
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