Co-reporter:Qiguang Dai, Wei Wang, Xingyi Wang, Guanzhong Lu
Applied Catalysis B: Environmental 2017 Volume 203(Volume 203) pp:
Publication Date(Web):1 April 2017
DOI:10.1016/j.apcatb.2016.10.009
•A novel CeO2@HZSM-5hybridcompositeswithsandwichandcore-shellstructurewasdesignedandprepared. (*).•CeO2 nanosheets were completely encapsulated by continuous and dense HZSM-5 membranes.•CeO2@HZSM-5 exhibited a better resistance to the coking and chlorine poisoning for DCE oxidation.•The formation of polychlorinated hydrocarbons (PCHs) by-products over CeO2@HZSM-5 was significantly inhibited.Sandwich-structured CeO2@HZSM-5 core-shell hybrid composites were designed and prepared by an in situ two-step hydrothermal growth method under dynamic condition, and SEM indicated that CeO2 nanosheets were completely encapsulated by HZSM-5 particles which formed continuous and dense zeolite membranes (exposed HZSM-5). The catalytic total oxidation of 1, 2-dichloroethane (DCE) over CeO2@HZSM-5 was investigated, compared with CeO2/HZSM-5 (CeO2 dispersed on HZSM-5) and CeO2 + HZSM-5 (CeO2 mixed with HZSM-5) reference catalysts. Although the latter two showed a better catalytic activity due to the synergies of ceria and HZSM-5 zeolite, the formation of poly-chlorinated hydrocarbons (PCHs) by-products over CeO2@HZSM-5 was significantly inhibited since CeO2 with high activity for Deacon reaction was not directly exposed to DCE or HCl molecules. Moreover, CeO2@HZSM-5 also exhibited a better resistance to the coking and chlorine poisoning, because the formed non-activated coke species or polyaromatic species could be easier to be removed via in situ oxidation by the active oxygen species from CeO2, and the exposed HZSM-5 was tolerant to the chlorination of acid sites and avoided the direct adsorption of HCl on CeO2. Additionally, the presence of water and ethyl acetate (EA) dramatically inhibited the activity of CeO2@HZSM-5 for DCE oxidation, but water also completely suppressed the formation of PCHs by-products. The high Si/Al ratio could improve the water-resistance due to the increase of hydrophobicity, and the induction of trace Pd (0.1 wt%) further increased the CO2 selectivity.Download high-res image (142KB)Download full-size image
Co-reporter:Wei Wang, Qin Zhu, Qiguang Dai, Xingyi Wang
Chemical Engineering Journal 2017 Volume 307(Volume 307) pp:
Publication Date(Web):1 January 2017
DOI:10.1016/j.cej.2016.08.137
•Fe-CeO2 nanosheets were prepared by three different methods.•Fe-CeO2-ST with the most abundant oxygen vacancies exhibited better activity.•15Fe-CeO2-ST showed better stability and lower selectivity of PCHs by-products.•Loading of V or Ru further enhanced stability and inhibited PCHs by-products.Two-dimensional (2D) nano-structured Ce1−xFexO2 mixed oxides (Fe doped CeO2 nanosheets) were synthesized by hydrothermal (HT), cold co-precipitation (CP) and solvothermal (ST) methods, and evaluated in total oxidation of 1,2-dichloroethane (DCE). Fe-doped CeO2 catalysts were characterized by SEM, XRD, EPR, Raman and H2-TPR and the results indicated that 5Fe-CeO2-ST had the largest concentration of oxygen vacancies and surface active oxygen (such as O22− and O2−), meanwhile exhibited a better catalytic activity and lower selectivity of polychlorohydrocarbons (PCHs) by-products. Catalytic activities and stabilities of Fe-CeO2-ST catalysts for DCE oxidation were found to slightly increase with the increase of Fe content, however, the enhancement of more than 15% Fe doping was almost negligible, which was probably related to the disappearing of the sheet-like morphology. Moreover, the stability of 15Fe-CeO2-ST catalyst can be further improved via the loading of VOx or RuO2, more importantly, the formation of PCHs by-products also was significantly inhibited.Fe doped CeO2 mixed oxide catalysts with 2D nanostructures were prepared by hydrothermal method (HT), cold co-precipitation method (CP) and solvothermal method (ST), and investigated in catalytic combustion of 1,2-dichloroethane. And the Fe-CeO2-ST exhibits better catalytic activity. Moreover, the loading of VOx or RuO2 can further improve the stability of Fe-CeO2-ST and inhibit the formation of polychlorinated by-products.Download high-res image (173KB)Download full-size image
Co-reporter:Qiguang Dai, Shuxing Bai, Yang Lou, Xingyi Wang, Yun Guo and Guanzhong Lu
Nanoscale 2016 vol. 8(Issue 18) pp:9621-9628
Publication Date(Web):07 Apr 2016
DOI:10.1039/C6NR01800A
PdO/CeO2 nanosheets encapsulated by a monolayer of a continuous and dense HZSM-5 zeolite membrane were prepared by a facile in situ hydrothermal growth process and used as a highly efficient and thermally stable catalyst for methane combustion. Uncoated PdO/CeO2 suffered severe sintering at high temperature or high oxygen concentration. However, the encapsulation of HZSM-5 significantly improved sintering resistance by the suppressing effects of the HZSM-5 coating for the agglomeration of PdOx nanoparticles, resulting in the outstanding thermal stability of PdO/CeO2. Furthermore, the synthesized hybrid materials also exhibited good oxygen- and water-tolerance for methane combustion due to the oxygen or water barrier. In addition, a reactivation behavior was observed due to the self-redispersion of PdOx on CeO2 nanosheets in the reaction atmosphere at high temperature.
Co-reporter:Shuxing Bai, Qiguang Dai, Xinxin Chu and Xingyi Wang
RSC Advances 2016 vol. 6(Issue 58) pp:52564-52574
Publication Date(Web):19 May 2016
DOI:10.1039/C6RA08855D
Bimodal mesoporous alumina (Al2O3) was prepared using polyethyleneglycol (PEG 20000) and cetyl trimethyl ammonium bromide as a template. The incorporation of Ba with various loadings was carried out by incipient wetness. Characterization was performed by XRD, N2 sorption isotherms, and pyridine FTIR. Ba can be highly dispersed on Al2O3 covering the strong acid sites of Al2O3. In the catalytic dehydrochlorination of 1,2-dichloroethane (1,2-DCE), the Ba/Al2O3 catalysts present a high activity, of which Al2O3 is most active with 95% conversion at 325 °C, related to the more Lewis acidic Al3+ sites in a tetrahedral environment. 1,2-DCE adsorbs dissociatively on Lewis acid–base pair sites, forming chlorinated ethoxy species, which are supposed to be intermediate species for vinyl chloride (VC) production. At a temperature higher than 400 °C, the dehydrochlorination of VC occurs on the strong acid sites of Al2O3. Ba can promote greatly the selectivity for VC through a decrease in the strong acid sites. A high stable activity for dehydrochlorination and high selectivity for VC can be obtained over Ba/Al2O3 in the presence of oxygen.
Co-reporter:Qing Zhao;Yanhong Hu
Journal of Applied Polymer Science 2016 Volume 133( Issue 3) pp:
Publication Date(Web):
DOI:10.1002/app.42875
ABSTRACT
Intumescent-flame-retarded polypropylene (PP-IFR) composites were prepared by the incorporation of methyl hydrogen siloxane treated ammonium polyphosphate and dipentaerythritol in a twin-screw extruder. The effects of zeolite (Z), multiwalled carbon nanotubes (CNTs), and maleic anhydride grafted polypropylene on the flame retardancy, mechanical properties, and thermal stability of PP-IFR were investigated. The addition of Z and CNT promoted the flame retardancy of PP-IFR, and the highest limited oxygen index was 35.6%, obtained on PP-M-IFR-2–Z, for which the heat-release rate, total heat release, and smoke production rate based on cone calorimetry analyses decreased by 45.0, 51.0, and 66.3%, respectively, in comparison with those values of the PP-IFR composites. Additionally, scanning electron microscopy analyses showed that there was a good interface interaction between the polypropylene matrix and additives. The flexural, tensile, and impact strengths of the PP-IFR composites were improved significantly with the incorporation of CNT. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016, 133, 42875.
Co-reporter:Shuxing Bai, Bingbing Shi, Wei Deng, Qiguang Dai and Xingyi Wang
RSC Advances 2015 vol. 5(Issue 60) pp:48916-48927
Publication Date(Web):27 May 2015
DOI:10.1039/C5RA07405C
The lower temperature catalytic combustion of 1,2-dichloroethane (DCE) over Al2O3, CeO2 and Al2O3–CeO2 catalysts were studied. An apparent deactivation for pure Al2O3 and CeO2 catalyst was observed at 300 °C, which was ascribed to the formation of coke for pure Al2O3 while the strong adsorption of Cl species at active sites for pure CeO2. However, Al2O3–CeO2 mixed oxides exhibited a high stable activity compared with the pure Al2O3 and CeO2, which indicated that suitable acidity and excellent redox performance was equally important for total oxidation of DCE. TPSR experiments indicated that ClCH2CHO was the intermediate product and vinyl chloride (VC) was the main by-product for DCE catalytic oxidation over Al2O3–CeO2 catalyst, ClCH2CHO and VC were the competitive products of the C–H-scission ethoxides, which generated by α- and β-CH-scission respectively. Based on in situ DRIFTS study, a simple reaction pathway was proposed: Firstly, DCE adsorbed on surface hydroxyl groups or Lewis acid sites via the C–Cl bond and was attacked by the basic site (O2−), and then the intermediates such as aldehyde species and by-product VC formed. Sequentially, the aldehyde species were converted into H2O, COx and HCl via further Cl abstraction and oxidation process, by contrast, VC was not easy to be further decomposed because of its stable structure, the weak adsorption and difficult dissociation on acid sites.
Co-reporter:Qing Zhao;Xing-yi Wang 王幸宜;Yan-hong Hu 扈艳红
Chinese Journal of Polymer Science 2015 Volume 33( Issue 10) pp:1359-1372
Publication Date(Web):2015 October
DOI:10.1007/s10118-015-1685-0
Polyimides (PIs) with various molecular weights synthesized via the reaction of aromatic diamine monomer containing tert-butyl groups with aromatic dianhydride were highly soluble in common organic solvents and some epoxy resins at room temperature. These PIs can be incorporated in the absence of organic solvent into epoxy resin E51 with the loading below 2 wt% forming EP-PI composites. No phase separation is observed by SEM on cryogenically fractured surfaces of EP-PI composites. The PI can improve mechanical properties, especially impact strength. Adding 2 wt% PI-1.5W, the impact strength reaches to 55 kJ/m2 with the increase in tensile and flexural strengths by 14% and 3%, respectively. SEM analyses for the fracture surface suggest that PI reduces the crosslink density, improves the plasticity of epoxy resin and changes the mode of fracture from fragile to ductile. Moreover, the glass transition temperature of EP-PI composites was found to increase to a significant extent.
Co-reporter:Qiguang Dai, Shuxing Bai, Hua Li, Wei Liu, Xingyi Wang and Guanzhong Lu
CrystEngComm 2014 vol. 16(Issue 42) pp:9817-9827
Publication Date(Web):27 Aug 2014
DOI:10.1039/C4CE01436G
Two types of CeO2 nanosheet, petal-like and belt-like, were synthesized using a facile aqueous phase precipitation method with NH4HCO3 as the precipitant at 0 °C and 25 °C, without hydrothermal or solvothermal treatment, without template or surfactant and without organic solvent. The reaction temperature and the supersaturation played key roles in the formation of the ceria nanosheets, namely, a lower temperature and higher supersaturation were favorable for the synthesis of sheet-like CeO2 by the oriented aggregation of the as-synthesized nanocrystalline precursors, whereas elevated temperatures could cause the dissolution–recrystallization of the precursors and promote the Ostwald ripening process, and finally polyhedral CeO2 could be obtained via thermal decomposition of the precursors. The catalytic oxidation properties were investigated using the catalytic oxidation of CO over CeO2 and the catalytic combustion of 1,2-dichloroethane over VOx/CeO2. Compared with traditional CeO2 nanoparticles, the ceria nanosheets showed excellent catalytic oxidation activities.
Co-reporter:Qiguang Dai;Shuxing Bai;Guanzhong Lu
Journal of Porous Materials 2014 Volume 21( Issue 6) pp:1041-1049
Publication Date(Web):2014 December
DOI:10.1007/s10934-014-9854-z
ZSM-5 zeolites with controllable crystal morphologies (microsphere self-assembled from nanorod crystals, round-boat and cross shape) were synthesized in extremely diluted solutions (H2O/SiO2 = 350) by only adjusting the tetrapropylammonium hydroxide concentration under dynamic or static condition. The synthesized ZSM-5 were characterized by X-ray diffraction, infrared spectra, scanning electron microscopy, transmission electron microscopy, N2 sorption and NH3 temperature programmed desorption, and compared with the commercial ZSM-5 zeolite. Catalytic tests for the formation of p-xylene from o-xylene isomerization and the catalytic oxidation of chlorinated hydrocarbons showed that ZSM-5 microsphere composed of nanorod crystals exhibited both high conversion and improved p-xylene selectivity, and high catalytic activities for 1,2-dichloroethane and chlorobenzene oxidation and low selectivity to chlorinated by-products, which were attributed to the existence of nanosized ZSM-5 crystals and mesopores, high internal surface area and total acidity.
Co-reporter:Zhonghao Jin;Dao Li;Qin Xiao
Chinese Journal of Chemistry 2010 Volume 28( Issue 1) pp:16-20
Publication Date(Web):
DOI:10.1002/cjoc.201090029
Abstract
A range of different nitrophenol derivatives were converted in one-pot to the corresponding secondary alkyl aminophenols in good to excellent yields by using ketones as alkyl source and hydrogen over 10 wt% Pd/C as reducing agent. In all examples, except for one, the secondary amine was the sole alkylation product isolated. When aldehydes were used as alkyl source, the corresponding tertiary amine as a sole alkylation product was isolated.
Co-reporter:Zhonghao Jin, Chao Yu, Xingyi Wang, Ying Wan, Dao Li and Guanzhong Lu
Chemical Communications 2009 (Issue 29) pp:4438-4440
Publication Date(Web):12 Jun 2009
DOI:10.1039/B907846K
Pd/mesoporous silica–carbon nanocomposites with 3.2 nm Pd particles, prepared by a simple wetness impregnation method, have demonstrated high activity at 258 K for the hydrodechlorination of chlorophenols with a high selectivity.
Co-reporter:Xingyi Wang;Yuan Li;Weiwei Liao;Jing Gu ;Dao Li
Polymers for Advanced Technologies 2008 Volume 19( Issue 8) pp:1055-1061
Publication Date(Web):
DOI:10.1002/pat.1077
Abstract
Melamine salt of tripentaerythriol phosphate (MTP), as a new intumescent flame-retardant, was prepared from tripentaerythritol (TPE), polyphosphoric acid, phosphoric pentoxide, and melamine, and then incorporated into polypropylene (PP) to obtain flame-retarded PP-MTP. FT-IR analysis showed that MTP was in the form of cage structure. The flammability, combustion behavior, and thermal degradation and stability of flame-retarded PP were characterized by using LOI, UL-94 test, cone calorimetry, and TGA, respectively. By SEM, the char structure of PP-MTP was analyzed. XRD diffraction tests showed that PP-matrix of PP-MTP presented better crystallized phases, when MTP was modified by methyl hydrogen siloxane. The relations of the dispersion of MTP in PP matrix to the compatibility between PP and MTP, and to the flame retardancy were discussed. Copyright © 2008 John Wiley & Sons, Ltd.
Co-reporter:Ogtour M'Ramadj, Bo Zhang, Dao Li, Xingyi Wang, Guanzhong Lu
Journal of Natural Gas Chemistry (September 2007) Volume 16(Issue 3) pp:258-265
Publication Date(Web):1 September 2007
DOI:10.1016/S1003-9953(07)60057-7
Two series of Cu/ZSM-5 catalysts, loading from 5 to 20 wt% CuO, were prepared by the deposition-precipitation and impregnation methods, respectively. The catalysts prepared by the impregnation method showed better catalytic performances than those prepared by the deposition-precipitation method and the increase of copper loading favored methane conversion. 20Cu(I)/ZSM-5 had the highest activity with T90% of 746 K, and for 20Cu(D)/ZSM-5, T90% was as high as 804 K. The characterization of X-ray diffraction (XRD), temperature-programmed reduction (TPR), temperature-programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS) revealed that the dispersion of copper species could be improved by using the deposition-precipitation method instead of the impregnation method, but the fraction of surface CuO, corresponding to active sites for methane oxidation, was larger on 20Cu(I)/ZSM-5 than 20Cu(D)/ZSM-5. The results of Pyridine-Fourier transform infrared spectrum (Py-FT-IR) showed that a majority of Lewis acidity and a minority of Brønsted acidity were present on Cu/ZSM-5 catalysts. 20Cu(I)/ZSM-5 presented more Lewis acid sites. The number of Lewis acid sites changed significantly with preadsorption of oxygen. Adsorption of methane and oxygen on acid sites was observed. The properties of Cu/ZSM-5 catalysts were correlated with the activity for methane oxidation.
Co-reporter:Bo Zhang, Xingyi Wang, Ogtour M'Ramadj, Dao Li, ... Guanzhong Lu
Journal of Natural Gas Chemistry (March 2008) Volume 17(Issue 1) pp:87-92
Publication Date(Web):1 March 2008
DOI:10.1016/S1003-9953(08)60031-6
Palladium-based catalysts were prepared using impregnation (I) and ion-exchange method (E) with ZSM-5 as support. Pd-ZSM-5(I) and Pd-ZSM-5(E) catalysts presented the high activity for the combustion of methane. The order of activity was consistent with Brønsted acidity of the catalysts: Pd-ZSM-5(I)>Pd-ZSM-5(E). It was shown by FT-IR that methane was adsorbed on the acidic bridging hydroxyl groups of ZSM-5-supported Pd catalysts. The effect of water on the activity of Pd-ZSM-5 was investigated. The inhibition effect of water on the conversion of methane was observed. However, water promoted the stability of Pd-ZSM-5 obviously during extended time periods. XPS measurement showed that Pd/Si ratio near the surface of Pd-ZSM-5(E) decreased more pronouncedly with time in dry stream than that of Pd-ZSM-5(I), this is attributed to the dispersion of Pd into the micropores. The addition of water, however, retarded Pd dispersion. And high partial pressure of methane reduced this effect of water vapor. The decrease in activity during the stability test can be explained on the basis of the reduction of Pd/Si ratio.
Co-reporter:Wei Deng, Qiguang Dai, Yijie Lao, Bingbing Shi, Xingyi Wang
Applied Catalysis B: Environmental (February 2016) Volume 181() pp:848-861
Publication Date(Web):February 2016
DOI:10.1016/j.apcatb.2015.07.053
Co-reporter:Dao Li, Yi Zheng, Xingyi Wang
Applied Catalysis A: General (15 May 2008) Volume 340(Issue 1) pp:33-41
Publication Date(Web):15 May 2008
DOI:10.1016/j.apcata.2008.01.035
Co-reporter:Meng Wu, Xingyi Wang, Qiguang Dai, Dao Li
Catalysis Communications (1 July 2010) Volume 11(Issue 12) pp:1022-1025
Publication Date(Web):1 July 2010
DOI:10.1016/j.catcom.2010.04.011
Mn–Ce–Mg/Al2O3 catalyst prepared by a wet impregnation method was investigated in the catalytic combustion of chlorobenzene. The addition of Mg decreased the interaction of Mn and Ce species with Al2O3 and promotes the dispersion of Mn and Ce species and the formation of Ce–Mn–O solid solution. High activity, good selectivity and desired stability of Mn–Ce–Mg/Al2O3 catalyst were observed.
Co-reporter:Zhonghao Jin, Chao Yu, Xingyi Wang, Ying Wan, Dao Li and Guanzhong Lu
Chemical Communications 2009(Issue 29) pp:NaN4440-4440
Publication Date(Web):2009/06/12
DOI:10.1039/B907846K
Pd/mesoporous silica–carbon nanocomposites with 3.2 nm Pd particles, prepared by a simple wetness impregnation method, have demonstrated high activity at 258 K for the hydrodechlorination of chlorophenols with a high selectivity.