The preparation of ZnAlLa-hydrotalcite-like compounds [ZnAlLa-HTLcs] wasstudied. ZnAlLa-HTLcs were synthesized by a method of variable pH with the raw materials ofZn(NO_3)_2, Al(NO_3)_3, La(NO_3)_3, and NaOH. The eS...The preparation of ZnAlLa-hydrotalcite-like compounds [ZnAlLa-HTLcs] wasstudied. ZnAlLa-HTLcs were synthesized by a method of variable pH with the raw materials ofZn(NO_3)_2, Al(NO_3)_3, La(NO_3)_3, and NaOH. The eS'ccts of some factors (i.e. pH values, the moleratio of Al^(3+) to La^(3+), temperature and the period of hydrothermal treatment) on thepreparation of HTLcs were discussed systematically. XRD, TG-DTA, FT-IR spectroscopy, and ICP wereperformed to characterize ZnAlLa-HTLcs samples, and the thermal stability of HTLcs was alsodiscussed. It was shown that unique ZnAlLa-HTLcs with high crystallinity can be prepared, under theconditions of pH = 5.5-6.5, n(Zn^(2+))/n(Al^(3+) + La^(3+))=2 and the atomic ratio of La^(3+) toAl^(3+) ranging from 0.07 to 2, hydrothermal treatment at 120 ℃ for 5 h. When the calcination ofthe HTLcs is performed at temperatures above 200 ℃, ZnO phase is detected with Al_2O_3 and La_2O_3spreading on its top. The complex metal oxides derived from ZnAlLa-HTLcs at 500 ℃ have highercatalytic activity and selectivity than those from ZnAl-HTLcs for the esterification of acetic acidwith n-butanol under the same reaction conditions.展开更多
MgCoAl-hydrotalcite-like compounds (MgCoAI-HTLcs) were synthesized using the coprecipitation method of variable pH values. The effect of each factor on the preparation of HTLcs was discussed systematically, which in...MgCoAl-hydrotalcite-like compounds (MgCoAI-HTLcs) were synthesized using the coprecipitation method of variable pH values. The effect of each factor on the preparation of HTLcs was discussed systematically, which included pH values, mole ratios of Mg2+ to Co2+, the concentrations of the solution, and the temperature and time of the hydrothermal treatment. Besides, the thermal decomposition of MgCoAI-HTLcs was discussed. X-ray diffraction, thermogravimetric analysis, and FT-IR spectroscopy were performed to characterize the MgCoAI-HTLcs samples. The results showed that when the pH = 7.6-8.5 or 5.5-6.2, atomic ratios of (Mg^2++Co2+)/Al^3+ 2 and Mg^2+/Co^2+ ranging from 1.00 to 2.00, temperature and time of hydrothermal treatment being 110℃ and 6 h, unique MgCoAI-HTLcs with high crystallinity could be obtained. When the calcination temperature was up to 250℃, the MgO phase was detected coexisting with Al2O3 and MgAl2O4 was highly spreaded on the derived mixed oxides. The synthesis reaction of benzoin methyl ether with methanol and benzaldehyde was chosen to study the catalytic activity of MgCoAI-HTLcs. The catalyst showed high activity and high stability in the synthesis of benzoin methyl ether in the feasible condition.展开更多
The particles of ferric aluminum magnesium hydrotalcite-like compounds (Fe-Al-Mg_HTlc) were synthesized by co-precipitation method. It was found that when n(Fe)/n(Al+Mg+Fe)<0.30 and n(Al)/n(Al+Mg+Fe)<0.30, pure...The particles of ferric aluminum magnesium hydrotalcite-like compounds (Fe-Al-Mg_HTlc) were synthesized by co-precipitation method. It was found that when n(Fe)/n(Al+Mg+Fe)<0.30 and n(Al)/n(Al+Mg+Fe)<0.30, pure HTlc can be formed; when the molar ratio of Al/ (Fe+Al+Mg)>0.30, Al(OH)3 will emerge; when the molar ratio of Fe/(Fe+Al+Mg) >0.30, the amorphous composition will appear. Hence Fe3+ and Al3+ have no concentration superposition effect on the crystal structure of the samples.展开更多
The relation of the isoelectric point (IEP) and the point of zero net charge (PZNC) of the hydrotalcite-like compounds was discussed. It was found that the IEP does not equal to the PZNC and the IEP is higher than th...The relation of the isoelectric point (IEP) and the point of zero net charge (PZNC) of the hydrotalcite-like compounds was discussed. It was found that the IEP does not equal to the PZNC and the IEP is higher than the PZNC. The structural positive charges existing in the HTlc, which cause the difference between the IEP and the PZNC. The effects of the structural positive charges of the HTlc on its IEP and PZNC are the same as the specific adsorption of metal cations.展开更多
The X-CoMnMgAl hydrotalcite-like precursors(X-LDHs) were first synthesized by the coprecipitation method using Cl-, CO32-, NO3- and SO42- as the corresponding guest anions, which were further used to prepare X-CoMnMgA...The X-CoMnMgAl hydrotalcite-like precursors(X-LDHs) were first synthesized by the coprecipitation method using Cl-, CO32-, NO3- and SO42- as the corresponding guest anions, which were further used to prepare X-CoMnMgAl complex oxides(X-LDOs) through calcination. The structure and the surface morphology of the as-prepared samples were characterized by FT–IR, XRD, N2 adsorption-desorption and SEM. These as-prepared X-LDOs could act as sulfur-transfer catalysts for desulfurization. The activity of SOx adsorption and regeneration was evaluated via a self-assembled fixed-bed reactor simulating the conditions found in the fluid catalytic cracking units. These four types of sulfur-transfer catalysts with the same phase but different structure displayed the following order of desulfurization efficiency: CO3-LDO >Cl-LDO >NO3-LDO > SO4-LDO.展开更多
A new method for regulating the synthesis of Ni Mg Fe hydrotalcites(NMF LDHs) with the addition of hydroxyl compounds was proposed. A series of NMF LDHs were prepared by the above method, and then were calcined to obt...A new method for regulating the synthesis of Ni Mg Fe hydrotalcites(NMF LDHs) with the addition of hydroxyl compounds was proposed. A series of NMF LDHs were prepared by the above method, and then were calcined to obtain the Ni Mg FeOx(NMFOx) samples. The NMFOxsamples were characterized by XRD,SEM, TG-DTG, XPS and CO2-TPD, respectively. The catalytic performance of NMFOxfor depolymerizing calcium lignosulfonate(CLS) was evaluated by hydrothermal reaction. The results showed that the addition of hydroxyl compounds favored reducing the particle sizes of NMF LDHs. For the depolymerization of CSL, the yield of liquid product increased from 45% to 75.8% with the addition of NMFOx-ethanol(NMFOxET). The liquid products were mainly phenolics, aromatics, ketones and esters. The total selectivity of oxy-containing compounds was over 90.6%, among them, the phenolics were approximately 35.2%. The valence of Ni and Fe, crystalline phase and basicity almost remained unchanged. The NMFOx-ET samples were recycled for the depolymerization of CLS, moreover, the NMFOx-ET samples had high activity and stability after 4 cycles.展开更多
In this study, Mg-Al-CO3 hydrotalcite was synthesized from a kaolinite as natural source aluminium using two simple methods. The first method uses the kaolinite in natural solid state, the second method use the filtra...In this study, Mg-Al-CO3 hydrotalcite was synthesized from a kaolinite as natural source aluminium using two simple methods. The first method uses the kaolinite in natural solid state, the second method use the filtrate of the kaolinite after dissolution by acidic solutions. The structure of the materials was characterized by X-ray diffraction, Fourier transform infrared spectroscopy, differential scanning calorimetry (DSC) and Brunauer, Emmett, and Teller (BET) measurements.展开更多
Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was inves...Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was investigated with dry reforming of methane.Experimental results showed that the hydrotalcite-like precursors could be completely decomposed and partly reduced by cold plasma jet,and the Nicontained catalysts exhibited much higher activity than the catalyst without Ni.Especially,the catalyst with Ni/Co ratio of 8/2 achieved not only the highest conversions of 80.3%and 69.3%for CH4 and CO2,respectively,but also the best stability in 100 h testing.The catalysts were characterized by XRD,XPS,TEM and N2 adsorption techniques,and the results showed that the better performance of the 8Ni2Co bimetallic catalyst was attributed to its higher metal dispersion,smaller metal particle size,as well as the interaction effect between Ni and Co,which were brought by the special catalyst preparation method.展开更多
A series of calcined HTLcs catalysts were prepared and modified with potassium phosphate by impregnation method to clarify the influence of catalyst alkalinity on the side chain alkylation of toluene with methanol for...A series of calcined HTLcs catalysts were prepared and modified with potassium phosphate by impregnation method to clarify the influence of catalyst alkalinity on the side chain alkylation of toluene with methanol for synthesis of ethylbenzene and styrene.The catalysts were characterized by X-ray diffraction(XRD),N_(2)physical adsorption-desorption,Fourier-transform infrared spectroscopy(FT-IR),Scanning electron microscopy(SEM),X-ray photoelectron spectrometry(XPS),NH_(3)temperature-programmed desorption(NH_(3)-TPD)and CO_(2)temperature-programmed desorption(CO_(2)-TPD).It was found that the selectivity of styrene was highest(39.25%)when the K_(3)PO_(4)loading was 7.5 wt%.And the total yield of styrene and ethylbenzene could reach 65.08%with 10 wt%K_(3)PO_(4)loading.This might due to the fact that the addition of K_(3)PO_(4)could adjust the acid and basic sites of catalysts.In addition,appropriate strength and amount of basic sites were favorable to producing more styrene.展开更多
The urea decomposition property at high temperature has been used to control the pH value in the synthesis of layer compounds. The hydrotalcites of Mg-Al and Ni-Al with high crystallinity were synthesized by using th...The urea decomposition property at high temperature has been used to control the pH value in the synthesis of layer compounds. The hydrotalcites of Mg-Al and Ni-Al with high crystallinity were synthesized by using this property.展开更多
基金Supported by Shanxi Province Natural Science Funds.(20001015)
文摘The preparation of ZnAlLa-hydrotalcite-like compounds [ZnAlLa-HTLcs] wasstudied. ZnAlLa-HTLcs were synthesized by a method of variable pH with the raw materials ofZn(NO_3)_2, Al(NO_3)_3, La(NO_3)_3, and NaOH. The eS'ccts of some factors (i.e. pH values, the moleratio of Al^(3+) to La^(3+), temperature and the period of hydrothermal treatment) on thepreparation of HTLcs were discussed systematically. XRD, TG-DTA, FT-IR spectroscopy, and ICP wereperformed to characterize ZnAlLa-HTLcs samples, and the thermal stability of HTLcs was alsodiscussed. It was shown that unique ZnAlLa-HTLcs with high crystallinity can be prepared, under theconditions of pH = 5.5-6.5, n(Zn^(2+))/n(Al^(3+) + La^(3+))=2 and the atomic ratio of La^(3+) toAl^(3+) ranging from 0.07 to 2, hydrothermal treatment at 120 ℃ for 5 h. When the calcination ofthe HTLcs is performed at temperatures above 200 ℃, ZnO phase is detected with Al_2O_3 and La_2O_3spreading on its top. The complex metal oxides derived from ZnAlLa-HTLcs at 500 ℃ have highercatalytic activity and selectivity than those from ZnAl-HTLcs for the esterification of acetic acidwith n-butanol under the same reaction conditions.
基金Supported by the Natural Science Foundation of Shanxi Province(20001015).
文摘MgCoAl-hydrotalcite-like compounds (MgCoAI-HTLcs) were synthesized using the coprecipitation method of variable pH values. The effect of each factor on the preparation of HTLcs was discussed systematically, which included pH values, mole ratios of Mg2+ to Co2+, the concentrations of the solution, and the temperature and time of the hydrothermal treatment. Besides, the thermal decomposition of MgCoAI-HTLcs was discussed. X-ray diffraction, thermogravimetric analysis, and FT-IR spectroscopy were performed to characterize the MgCoAI-HTLcs samples. The results showed that when the pH = 7.6-8.5 or 5.5-6.2, atomic ratios of (Mg^2++Co2+)/Al^3+ 2 and Mg^2+/Co^2+ ranging from 1.00 to 2.00, temperature and time of hydrothermal treatment being 110℃ and 6 h, unique MgCoAI-HTLcs with high crystallinity could be obtained. When the calcination temperature was up to 250℃, the MgO phase was detected coexisting with Al2O3 and MgAl2O4 was highly spreaded on the derived mixed oxides. The synthesis reaction of benzoin methyl ether with methanol and benzaldehyde was chosen to study the catalytic activity of MgCoAI-HTLcs. The catalyst showed high activity and high stability in the synthesis of benzoin methyl ether in the feasible condition.
基金The authors are grateful to the National Natural Science Foundation of China for financial support (No.29873026).
文摘The particles of ferric aluminum magnesium hydrotalcite-like compounds (Fe-Al-Mg_HTlc) were synthesized by co-precipitation method. It was found that when n(Fe)/n(Al+Mg+Fe)<0.30 and n(Al)/n(Al+Mg+Fe)<0.30, pure HTlc can be formed; when the molar ratio of Al/ (Fe+Al+Mg)>0.30, Al(OH)3 will emerge; when the molar ratio of Fe/(Fe+Al+Mg) >0.30, the amorphous composition will appear. Hence Fe3+ and Al3+ have no concentration superposition effect on the crystal structure of the samples.
文摘The relation of the isoelectric point (IEP) and the point of zero net charge (PZNC) of the hydrotalcite-like compounds was discussed. It was found that the IEP does not equal to the PZNC and the IEP is higher than the PZNC. The structural positive charges existing in the HTlc, which cause the difference between the IEP and the PZNC. The effects of the structural positive charges of the HTlc on its IEP and PZNC are the same as the specific adsorption of metal cations.
基金the Natural Science Foundation of Jiangsu Province(No.BK20171273)the National Natural Science Foundation of China(No.21774107)+3 种基金the High-level Talent Project “Talents in Six Peak Disciplines”(JNHB-068)the Major Fundamental Research Program of the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(19KJA540001)the “Qing Lan Project” of Jiangsu Province,the Jiangsu Provincial Government Scholarship Programthe Initial Scientific Research Foundation of Yancheng Institute of Technology(No.KJC2014002)for financial support of this research
文摘The X-CoMnMgAl hydrotalcite-like precursors(X-LDHs) were first synthesized by the coprecipitation method using Cl-, CO32-, NO3- and SO42- as the corresponding guest anions, which were further used to prepare X-CoMnMgAl complex oxides(X-LDOs) through calcination. The structure and the surface morphology of the as-prepared samples were characterized by FT–IR, XRD, N2 adsorption-desorption and SEM. These as-prepared X-LDOs could act as sulfur-transfer catalysts for desulfurization. The activity of SOx adsorption and regeneration was evaluated via a self-assembled fixed-bed reactor simulating the conditions found in the fluid catalytic cracking units. These four types of sulfur-transfer catalysts with the same phase but different structure displayed the following order of desulfurization efficiency: CO3-LDO >Cl-LDO >NO3-LDO > SO4-LDO.
基金Supported by the Program for National Natural Science Foundation of China(No.51674089)Excellent Youth Foundation of Heilongjiang Province of China(No.JC2018002)+2 种基金Postdoctoral Scientific Research Development Fund of Heilongjiang Province of China(No.LBH-Q16037)the Youth Fund of Northeast Petroleum University(No.2018QNL-17)the Postgraduate Innovative Research Projects of Northeast Petroleum University(No.YJSCX2017-014NEPU)
文摘A new method for regulating the synthesis of Ni Mg Fe hydrotalcites(NMF LDHs) with the addition of hydroxyl compounds was proposed. A series of NMF LDHs were prepared by the above method, and then were calcined to obtain the Ni Mg FeOx(NMFOx) samples. The NMFOxsamples were characterized by XRD,SEM, TG-DTG, XPS and CO2-TPD, respectively. The catalytic performance of NMFOxfor depolymerizing calcium lignosulfonate(CLS) was evaluated by hydrothermal reaction. The results showed that the addition of hydroxyl compounds favored reducing the particle sizes of NMF LDHs. For the depolymerization of CSL, the yield of liquid product increased from 45% to 75.8% with the addition of NMFOx-ethanol(NMFOxET). The liquid products were mainly phenolics, aromatics, ketones and esters. The total selectivity of oxy-containing compounds was over 90.6%, among them, the phenolics were approximately 35.2%. The valence of Ni and Fe, crystalline phase and basicity almost remained unchanged. The NMFOx-ET samples were recycled for the depolymerization of CLS, moreover, the NMFOx-ET samples had high activity and stability after 4 cycles.
文摘In this study, Mg-Al-CO3 hydrotalcite was synthesized from a kaolinite as natural source aluminium using two simple methods. The first method uses the kaolinite in natural solid state, the second method use the filtrate of the kaolinite after dissolution by acidic solutions. The structure of the materials was characterized by X-ray diffraction, Fourier transform infrared spectroscopy, differential scanning calorimetry (DSC) and Brunauer, Emmett, and Teller (BET) measurements.
基金supported by the National Natural Science Foundation of China(11075113)
文摘Ni-Co bimetallic catalysts with different Ni/Co content were derived from cold plasma jet decomposition and reduction of hydrotalcite-like compounds containing Ni,Co,Mg and Al,and their catalytic performance was investigated with dry reforming of methane.Experimental results showed that the hydrotalcite-like precursors could be completely decomposed and partly reduced by cold plasma jet,and the Nicontained catalysts exhibited much higher activity than the catalyst without Ni.Especially,the catalyst with Ni/Co ratio of 8/2 achieved not only the highest conversions of 80.3%and 69.3%for CH4 and CO2,respectively,but also the best stability in 100 h testing.The catalysts were characterized by XRD,XPS,TEM and N2 adsorption techniques,and the results showed that the better performance of the 8Ni2Co bimetallic catalyst was attributed to its higher metal dispersion,smaller metal particle size,as well as the interaction effect between Ni and Co,which were brought by the special catalyst preparation method.
基金financial support from the National Key Technology Research&Development Program(Grant No.2013BAC14B04)the National Natural Science Foundation of China(Grant No.21336006)+1 种基金the Shanxi Province Key Research&Development Program(international cooperation,Grant No.201803D421099)Supported by Shanxi Scholarship Council of China(Grant No.2017-035)。
文摘A series of calcined HTLcs catalysts were prepared and modified with potassium phosphate by impregnation method to clarify the influence of catalyst alkalinity on the side chain alkylation of toluene with methanol for synthesis of ethylbenzene and styrene.The catalysts were characterized by X-ray diffraction(XRD),N_(2)physical adsorption-desorption,Fourier-transform infrared spectroscopy(FT-IR),Scanning electron microscopy(SEM),X-ray photoelectron spectrometry(XPS),NH_(3)temperature-programmed desorption(NH_(3)-TPD)and CO_(2)temperature-programmed desorption(CO_(2)-TPD).It was found that the selectivity of styrene was highest(39.25%)when the K_(3)PO_(4)loading was 7.5 wt%.And the total yield of styrene and ethylbenzene could reach 65.08%with 10 wt%K_(3)PO_(4)loading.This might due to the fact that the addition of K_(3)PO_(4)could adjust the acid and basic sites of catalysts.In addition,appropriate strength and amount of basic sites were favorable to producing more styrene.
文摘The urea decomposition property at high temperature has been used to control the pH value in the synthesis of layer compounds. The hydrotalcites of Mg-Al and Ni-Al with high crystallinity were synthesized by using this property.