Cerium-based sealing treatment was developed for Mg-Al hydrotalcite film on AZ91D Mg alloy,and the influence of cerium salt solution was investigated to modify the surface integrity and corrosion resistance.Scanning e...Cerium-based sealing treatment was developed for Mg-Al hydrotalcite film on AZ91D Mg alloy,and the influence of cerium salt solution was investigated to modify the surface integrity and corrosion resistance.Scanning electron microscope(SEM)and X-ray diffraction(XRD)measurements were carried out to analyze the surface morphology and phase composition.The corrosion resistance of Mg-Al hydrotalcite film after sealing treatment was evaluated by the polarization curve and electrochemical impedance spectroscopy(EIS)tests.The results showed that lower concentration of Ce-containing solution was beneficial to seal the micro-cracks on Mg-Al hydrotalcite film,and improve the surface integrity and corrosion resistance;higher concentration of Ce-containing solution could seal fewer micro-cracks,and the corrosion resistance was decreased owing to the disintegration of Mg-Al hydrotalcite film.展开更多
Herein,the relationship between the structure and base properties of Mg–Al hydrotalcite catalysts was comprehensively investigated in relation to heat treatment and rehydration processes,which are well known as memor...Herein,the relationship between the structure and base properties of Mg–Al hydrotalcite catalysts was comprehensively investigated in relation to heat treatment and rehydration processes,which are well known as memory effects of hydrotalcite.The structure of Mg–Al hydrotalcites changed from layered double hydroxide(LDH)to mixed metal oxide and subsequently to a spinel structure during heat treatment,and it was returned from mixed metal oxide to a LDH structure by rehydration.Based on various characterizations,we successfully proposed a detailed mechanism of memory effect.We also confirmed that the Mg–Al hydrotalcites had weak or strong base sites and that their base properties could be systematically tuned by heat treatment and rehydration.The prepared Mg–Al hydrotalcites were applied to a model reaction,isomerization of glucose to fructose,as base catalysts.Among the catalysts tested,the rehydrated Mg–Al hydrotalcite efficiently produced fructose due to its appropriate base and structure properties.We finally concluded that the base sites of Mg–Al hydrotalcites can be designed as desired by heat treatment and rehydration.Moreover,through systematic design of the base sites of Mg–Al hydrotalcites,these can be promising catalysts for various heterogeneous reactions over base catalysts,giving excellent catalytic performances.展开更多
Mg/Al/Fe layered double hydroxide(MAF-LDH1) was prepared by solvothermal method with the sodium dodecyl sulfate as the template, and the ethanol system was benefit to growth of sample. The nature in the resulting MAF-...Mg/Al/Fe layered double hydroxide(MAF-LDH1) was prepared by solvothermal method with the sodium dodecyl sulfate as the template, and the ethanol system was benefit to growth of sample. The nature in the resulting MAF-LDH was investigated by X-ray diffraction, field emission scanning electron microscopy, Fourier transformed infrared spectra, thermogravimetric analysis, and N2 adsorption-desorption.The morphology of MAF-LDH1 is petal-like with the size of 400-500 nm and the thickness about 10-20 nm. The adsorption performance of the samples was evaluated by absorption of the Congo red(CR) solutions. Compared with Mg/Al layered double hydroxide(MA-LDH), the maximum adsorption capacities of the MAF-LDH1 samples were 943.4 mg/g which was greatly enhanced. Furthermore, after seven cycling tests, the adsorption performance was still up to 90%. Theoretical calculation results revealed that the adsorption process was spontaneous and followed the pseudo-second-order kinetic model and Freundlich model. This work provides a promising alternative strategy to enhance the adsorptive properties of hydrotalcite-like materials.展开更多
Trace amounts of noble metal-doped Ni/Mg(AI)O catalysts were pre- pared starting from Mg-Al hydrotalcites (HTs) and tested in daily start-up and shut-down (DSS) operation of steam reforming (SR) of methane or ...Trace amounts of noble metal-doped Ni/Mg(AI)O catalysts were pre- pared starting from Mg-Al hydrotalcites (HTs) and tested in daily start-up and shut-down (DSS) operation of steam reforming (SR) of methane or partial oxidation (PO) of propane. Although Ni/Mg(Al)O catalysts prepared from Mg(Ni)-Al HT exhibited high and stable activity in stationary SR, PO and dry reforming of methane and propane, the Ni/Mg(Al)O catalysts were drastically deactivated due to Ni oxidation by steam as purge gas when they were applied in DSS SR of methane. Such deactivation was effectively suppressed by doping trace amounts of noble metal on the catalysts by using a "memory effect" of HTs. Moreover, the noble metal-doped Ni/Mg(Al)O catalysts exhibited "intelligent" catalytic behaviors, i.e., self-activation and self-regenerative activity, leading to high and sustainable activity during DSS operation. Pt was the most effective among noble metals tested. The self-activation occurred by the reduction of Ni2+ in Mg(Ni,Al)O periclase to Ni^0 assisted by hydrogen spillover from Pt (or Pt-Ni alloy). The self-regenerative activity was accomplished by self-redispersion of active Ni^0 particles due to a reversible reductionoxidation movement of Ni between the outside and the inside of the Mg(Al)O periclase crystal; surface Ni^0 was oxidized to Ni2+ by steam and incorporated into Mg(Ni2+,Al)O periclase, whereas the Ni2+ in the periclase was reduced to Ni^0 by the hydrogen spillover and appeared as the fine Ni^0 particles on the catalyst surface. Further a "green" preparation of the Pt/Ni/[Mg3.sAl]O catalysts was accomplished starting from commercial Mg3.5-AI HT by calcination, followed by sequential impregnation of Ni and Pt.展开更多
Mg-Al hydrotalcites were synthesized using different preparation methods(a co-precipitation method, a urea method, and a simple one) to analyze their effect on the catalytic activity of these solid base catalysts. The...Mg-Al hydrotalcites were synthesized using different preparation methods(a co-precipitation method, a urea method, and a simple one) to analyze their effect on the catalytic activity of these solid base catalysts. The method strongly affected the structure of their layers(e.g., the growth and stacking of the layers, and the type of intercalated anions) and, accordingly, their catalytic activity. The Mg-Al hydrotalcite prepared by co-precipitation showed the best catalytic performance in the isomerization of glucose into fructose, due to the small crystallite size and sand rose morphology enhancing the exposure of surface active sites to reactants.展开更多
Water pollution with dye chemicals from apparel industries is a serious problem in the world.Since most of dyes are potentially have toxic and carcinogenic effects on human,it is important to remove them before they a...Water pollution with dye chemicals from apparel industries is a serious problem in the world.Since most of dyes are potentially have toxic and carcinogenic effects on human,it is important to remove them before they are discharged to the environment.Among many methods available for dyes removal in water,adsorption is the easiest and economically feasible that has no major obstacle for practical applications.In the present study,we tested calcined Mg/Al hydrotalcite(Mg/Al CHT)prepared by coprecipitation technique as an adsorbent for the removal of Navy Blue(NB)and Yellow F3G(YF3G)dyes.Mg/Al CHT was characterized by using a Fourier transform infrared(FTIR)spectrometer,an X-ray diffractometer(XRD)and a scanning electron microscope(SEM).The results showed that Mg/Al CHT was highly effective as an adsorbent for the removal of NB and YF3G under mild-acidic condition(pH 4)with removal capacities(b)according to Langmuir isotherm model were 7.97×10^(–4) and 5.80×10^(–4)mol·g^(-1),respectively.Kinetics study showed that the adsorption of NB and YF3D on Mg/Al CHT followed pseudosecond order with rate constant(k_(p2))11.57×10^(3) and 11.75×103 g·mol^(-1)·min-1,respectively.The spent adsorbent can be easily regenerated by simply calcining it at 450℃ for 3 h.Adsorption test on the mixture of NB and YF3G showed that the adsorption capacity of Mg/Al CHT was eightfold higher than that of Mg/Al HT and the value was maintained with repeated use.展开更多
The highly pure nano-crystal Mg,Al-hydrotalcite with titania doping was synthesized by one-step liquid reaction method at atmospheric pressure. The preparation of the Mg,Al-hydrotalcite nano-crystal after doping titan...The highly pure nano-crystal Mg,Al-hydrotalcite with titania doping was synthesized by one-step liquid reaction method at atmospheric pressure. The preparation of the Mg,Al-hydrotalcite nano-crystal after doping titania was investigated according to the results of XRD, TEM, IR and DSC. Moreover, based on the DSC test results, the thermal mechanism functions of the Mg,Al-hydrotalcite with titania doping were studied after calculation and comparison.展开更多
The geometry and electronic topology properties of Mg/Al hydrotalcite cluster models were comparatively investigated by means of density functional theory at GGA/DND levels.The results suggested that cluster model con...The geometry and electronic topology properties of Mg/Al hydrotalcite cluster models were comparatively investigated by means of density functional theory at GGA/DND levels.The results suggested that cluster model containing seven octahedral cations was the smallest size to be employed to simulate other properties.The fact that the n+ charge of cluster models containing n aluminum atoms can reflect electronic properties of anionic clay layer sheet.The bond lengths of clusters can be modified by terminating with or without OH-/H2O groups in terms of principle of bond order conservation.展开更多
基金supported by the National Natural Science Foundation of China(No.51701093)the Natural Science Foundation of Jiangsu Province(No.BK20170764)+2 种基金the Six Talent Peaks(No.2015-XCL-025)the Qing Lan Project of Jiangsu Province,the Practice Innovation Program for graduate students of Jiangsu Province(No.SJZZ16_0292)the Research Fund of Nanjing Institute of Technology(No.JCYJ201603).
文摘Cerium-based sealing treatment was developed for Mg-Al hydrotalcite film on AZ91D Mg alloy,and the influence of cerium salt solution was investigated to modify the surface integrity and corrosion resistance.Scanning electron microscope(SEM)and X-ray diffraction(XRD)measurements were carried out to analyze the surface morphology and phase composition.The corrosion resistance of Mg-Al hydrotalcite film after sealing treatment was evaluated by the polarization curve and electrochemical impedance spectroscopy(EIS)tests.The results showed that lower concentration of Ce-containing solution was beneficial to seal the micro-cracks on Mg-Al hydrotalcite film,and improve the surface integrity and corrosion resistance;higher concentration of Ce-containing solution could seal fewer micro-cracks,and the corrosion resistance was decreased owing to the disintegration of Mg-Al hydrotalcite film.
基金supported by C1 Gas Refinery Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT&Future Planning(2015M3D3A1A01064908)supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(No.2015R1D1A1A01059724)。
文摘Herein,the relationship between the structure and base properties of Mg–Al hydrotalcite catalysts was comprehensively investigated in relation to heat treatment and rehydration processes,which are well known as memory effects of hydrotalcite.The structure of Mg–Al hydrotalcites changed from layered double hydroxide(LDH)to mixed metal oxide and subsequently to a spinel structure during heat treatment,and it was returned from mixed metal oxide to a LDH structure by rehydration.Based on various characterizations,we successfully proposed a detailed mechanism of memory effect.We also confirmed that the Mg–Al hydrotalcites had weak or strong base sites and that their base properties could be systematically tuned by heat treatment and rehydration.The prepared Mg–Al hydrotalcites were applied to a model reaction,isomerization of glucose to fructose,as base catalysts.Among the catalysts tested,the rehydrated Mg–Al hydrotalcite efficiently produced fructose due to its appropriate base and structure properties.We finally concluded that the base sites of Mg–Al hydrotalcites can be designed as desired by heat treatment and rehydration.Moreover,through systematic design of the base sites of Mg–Al hydrotalcites,these can be promising catalysts for various heterogeneous reactions over base catalysts,giving excellent catalytic performances.
基金Funded by the Science and Technology Development Plan Project of Shandong Province,China(No.2013GSF11714)the Open Project of Hunan Sustentation Fund:Key Laboratory of Applied Environmental Photocatalysis,China(No.ccsu-KF-1501)
文摘Mg/Al/Fe layered double hydroxide(MAF-LDH1) was prepared by solvothermal method with the sodium dodecyl sulfate as the template, and the ethanol system was benefit to growth of sample. The nature in the resulting MAF-LDH was investigated by X-ray diffraction, field emission scanning electron microscopy, Fourier transformed infrared spectra, thermogravimetric analysis, and N2 adsorption-desorption.The morphology of MAF-LDH1 is petal-like with the size of 400-500 nm and the thickness about 10-20 nm. The adsorption performance of the samples was evaluated by absorption of the Congo red(CR) solutions. Compared with Mg/Al layered double hydroxide(MA-LDH), the maximum adsorption capacities of the MAF-LDH1 samples were 943.4 mg/g which was greatly enhanced. Furthermore, after seven cycling tests, the adsorption performance was still up to 90%. Theoretical calculation results revealed that the adsorption process was spontaneous and followed the pseudo-second-order kinetic model and Freundlich model. This work provides a promising alternative strategy to enhance the adsorptive properties of hydrotalcite-like materials.
基金supported by the New Energy and Industrial Technology Development Organization (NEDO),Japan
文摘Trace amounts of noble metal-doped Ni/Mg(AI)O catalysts were pre- pared starting from Mg-Al hydrotalcites (HTs) and tested in daily start-up and shut-down (DSS) operation of steam reforming (SR) of methane or partial oxidation (PO) of propane. Although Ni/Mg(Al)O catalysts prepared from Mg(Ni)-Al HT exhibited high and stable activity in stationary SR, PO and dry reforming of methane and propane, the Ni/Mg(Al)O catalysts were drastically deactivated due to Ni oxidation by steam as purge gas when they were applied in DSS SR of methane. Such deactivation was effectively suppressed by doping trace amounts of noble metal on the catalysts by using a "memory effect" of HTs. Moreover, the noble metal-doped Ni/Mg(Al)O catalysts exhibited "intelligent" catalytic behaviors, i.e., self-activation and self-regenerative activity, leading to high and sustainable activity during DSS operation. Pt was the most effective among noble metals tested. The self-activation occurred by the reduction of Ni2+ in Mg(Ni,Al)O periclase to Ni^0 assisted by hydrogen spillover from Pt (or Pt-Ni alloy). The self-regenerative activity was accomplished by self-redispersion of active Ni^0 particles due to a reversible reductionoxidation movement of Ni between the outside and the inside of the Mg(Al)O periclase crystal; surface Ni^0 was oxidized to Ni2+ by steam and incorporated into Mg(Ni2+,Al)O periclase, whereas the Ni2+ in the periclase was reduced to Ni^0 by the hydrogen spillover and appeared as the fine Ni^0 particles on the catalyst surface. Further a "green" preparation of the Pt/Ni/[Mg3.sAl]O catalysts was accomplished starting from commercial Mg3.5-AI HT by calcination, followed by sequential impregnation of Ni and Pt.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea funded by the Ministry of Education (NRF-2015R1D1A1A01059724)
文摘Mg-Al hydrotalcites were synthesized using different preparation methods(a co-precipitation method, a urea method, and a simple one) to analyze their effect on the catalytic activity of these solid base catalysts. The method strongly affected the structure of their layers(e.g., the growth and stacking of the layers, and the type of intercalated anions) and, accordingly, their catalytic activity. The Mg-Al hydrotalcite prepared by co-precipitation showed the best catalytic performance in the isomerization of glucose into fructose, due to the small crystallite size and sand rose morphology enhancing the exposure of surface active sites to reactants.
基金financial support from Directorate General of Higher Education,Republic of Indonesia through a research scheme of Penelitian Pascasarjana 2018 with contract number 1783/UN1/DITLIT/DIT-LIT/LT/2018。
文摘Water pollution with dye chemicals from apparel industries is a serious problem in the world.Since most of dyes are potentially have toxic and carcinogenic effects on human,it is important to remove them before they are discharged to the environment.Among many methods available for dyes removal in water,adsorption is the easiest and economically feasible that has no major obstacle for practical applications.In the present study,we tested calcined Mg/Al hydrotalcite(Mg/Al CHT)prepared by coprecipitation technique as an adsorbent for the removal of Navy Blue(NB)and Yellow F3G(YF3G)dyes.Mg/Al CHT was characterized by using a Fourier transform infrared(FTIR)spectrometer,an X-ray diffractometer(XRD)and a scanning electron microscope(SEM).The results showed that Mg/Al CHT was highly effective as an adsorbent for the removal of NB and YF3G under mild-acidic condition(pH 4)with removal capacities(b)according to Langmuir isotherm model were 7.97×10^(–4) and 5.80×10^(–4)mol·g^(-1),respectively.Kinetics study showed that the adsorption of NB and YF3D on Mg/Al CHT followed pseudosecond order with rate constant(k_(p2))11.57×10^(3) and 11.75×103 g·mol^(-1)·min-1,respectively.The spent adsorbent can be easily regenerated by simply calcining it at 450℃ for 3 h.Adsorption test on the mixture of NB and YF3G showed that the adsorption capacity of Mg/Al CHT was eightfold higher than that of Mg/Al HT and the value was maintained with repeated use.
基金Project (2004E113) Supported by Natural Science Basic Research Plan of Shaanxi Province of China
文摘The highly pure nano-crystal Mg,Al-hydrotalcite with titania doping was synthesized by one-step liquid reaction method at atmospheric pressure. The preparation of the Mg,Al-hydrotalcite nano-crystal after doping titania was investigated according to the results of XRD, TEM, IR and DSC. Moreover, based on the DSC test results, the thermal mechanism functions of the Mg,Al-hydrotalcite with titania doping were studied after calculation and comparison.
基金supported by China University of Petroleum (East China) (grant 09CX04045A)
文摘The geometry and electronic topology properties of Mg/Al hydrotalcite cluster models were comparatively investigated by means of density functional theory at GGA/DND levels.The results suggested that cluster model containing seven octahedral cations was the smallest size to be employed to simulate other properties.The fact that the n+ charge of cluster models containing n aluminum atoms can reflect electronic properties of anionic clay layer sheet.The bond lengths of clusters can be modified by terminating with or without OH-/H2O groups in terms of principle of bond order conservation.