A cobalt-based hydrotalcite-like compound was prepared using a constant-pH coprecipitation method.Cobalt-transition metal oxides(Co2XA10,X=Co,Mg,Ca and Ni)were investigated for the deep catalytic oxidation of o-chloro...A cobalt-based hydrotalcite-like compound was prepared using a constant-pH coprecipitation method.Cobalt-transition metal oxides(Co2XA10,X=Co,Mg,Ca and Ni)were investigated for the deep catalytic oxidation of o-chlorophenol as a typical heteroatom contaminant containing chlorine atoms.The partial substitution of Co by Mg,Ca or Ni in the mixed oxide can promote the catalytic oxidation of o-chlorophenol.The Co2MgA10 catalyst presented the best catalytic activity,and could maintain 90%o-chlorophenol conversion at 167.1℃,compared only 27%conversion for the Co3A10 catalyst.The results demonstrated that the high activity could be attributed to its increased low-temperature reducibility,rich active oxygen species and excellent oxygen mobility.In the existence of acid and base sites,catalysts with strong basicity also showed preferred activity.The organic by-products generated during the o-chlorophenol catalytic oxidation over Co2MgAlO catalyst included carbon tetrachloride,trichloroethylene,2,4-dichlorophenol,and 2,6-dichloro-p-benzoquinon,et al.This work provides a facile method for the preparation of Co-based composite oxide catalysts,which represent promising candidates for typical chlorinated and oxygenated volatile organic compounds.展开更多
An investigation of hydrotalcite-derived ternary Mg-Al-Ce oxides as catalysts for vapour phase condensation of ethanol to 1-butanol in a flow reactor under atmospheric pressure was carried out.The Mg-Al-Ce oxide syste...An investigation of hydrotalcite-derived ternary Mg-Al-Ce oxides as catalysts for vapour phase condensation of ethanol to 1-butanol in a flow reactor under atmospheric pressure was carried out.The Mg-Al-Ce oxide systems with Mg/(Al+Ce)ratio from 1 to 4 were synthesized and characterized by XRD,SEM,NMR,and XPS.The study of acid-base characteristics of the systems with different Mg/(Al+Ce)ratio by NH3/CO_(2)quasi-equilibrium thermal desorption techniques shows that the ratio of the catalyst oxide components(Mg,Al,Ce)can provide acid/base capacity ratio close to 3 for the effectivity of the target process.The highest selectivity 68%is reached over Mg-Al-Ce oxide catalyst with the ratio of Mg/(Al+Ce)=2.展开更多
<p align="justify"> <span style="font-family:Verdana;">The review outcome represents the optimum catalytic conditions </span><span><span><span style="font-fami...<p align="justify"> <span style="font-family:Verdana;">The review outcome represents the optimum catalytic conditions </span><span><span><span style="font-family:'Minion Pro Capt','serif';"><span style="font-family:Verdana;">for the pro</span><span style="font-family:Verdana;">duction of hydrogen using hydrotalcite derived catalysts. It covers dr</span><span style="font-family:Verdana;">y and ste</span><span style="font-family:Verdana;">am reforming of methane, steam reforming of methanol and ethanol t</span><span style="font-family:Verdana;">o hydrogen. The review also revealed the specific properties of hydrotalcite der</span><span style="font-family:Verdana;">ived catalysts for the reactions. Among catalyst investigated, Ni & Fe</span><span style="font-family:Verdana;"> promoted Al-Mg containing hydrotalcite catalyst perform best (99%) for dry reforming of methane at 250°C. For steam methane reforming, Ni containing </span><span style="font-family:Verdana;">ca-aluminates hydrotalcite catalyst act as the best (99%) at 550°C. Cu-supporte</span><span style="font-family:Verdana;">d Zn-Al-containing catalyst performs the best (99.98%) for steam reforming of methanol at 300°C whereas Cu impregnated Mg-Al containing hydrotalcite is </span><span style="font-family:Verdana;">the best (99%) for steam reforming of ethanol at 200°C - 600°C. It’s (HT</span><span style="font-family:Verdana;">) tunable and versatile textural and morphological properties showed excellent catalytic performances for different industrial processes and in sustainable hydrogen production.</span></span></span></span> </p>展开更多
A highly efficient and stable hydrotalcite-derived Cu-MgAlO catalyst was developed for the partial oxidation of cyclohexane with molecular oxygen.The physical–chemical properties of Cu-MgAlO catalysts were studied,an...A highly efficient and stable hydrotalcite-derived Cu-MgAlO catalyst was developed for the partial oxidation of cyclohexane with molecular oxygen.The physical–chemical properties of Cu-MgAlO catalysts were studied,and the results indicated that the copper component had been successfully introduced into the hydrotalcite unit layer structure.The catalytic reaction results showed that copper as the active species could activate CAH bond and effectively promote the decomposition of cyclohexyl hydroperoxide(CHHP)to the mixture of cyclohexanol and cyclohexanone(KA oil).8.3%of cyclohexane conversion and 82.9%of selectivity for KA oil were obtained over 9%Cu-MgAlO catalyst at 150℃with 0.6 MPa of oxygen pressure for 2 h.Especially,its catalytic performance was still stable after five runs.展开更多
基金This work is financially supported by the National Natural Science Foundation of China(Grant Nos.21677160 and 21477149)Beijing Municipal Science&Technology Commission(Nos.Z181100000118003 and Z 181100005418011).
文摘A cobalt-based hydrotalcite-like compound was prepared using a constant-pH coprecipitation method.Cobalt-transition metal oxides(Co2XA10,X=Co,Mg,Ca and Ni)were investigated for the deep catalytic oxidation of o-chlorophenol as a typical heteroatom contaminant containing chlorine atoms.The partial substitution of Co by Mg,Ca or Ni in the mixed oxide can promote the catalytic oxidation of o-chlorophenol.The Co2MgA10 catalyst presented the best catalytic activity,and could maintain 90%o-chlorophenol conversion at 167.1℃,compared only 27%conversion for the Co3A10 catalyst.The results demonstrated that the high activity could be attributed to its increased low-temperature reducibility,rich active oxygen species and excellent oxygen mobility.In the existence of acid and base sites,catalysts with strong basicity also showed preferred activity.The organic by-products generated during the o-chlorophenol catalytic oxidation over Co2MgAlO catalyst included carbon tetrachloride,trichloroethylene,2,4-dichlorophenol,and 2,6-dichloro-p-benzoquinon,et al.This work provides a facile method for the preparation of Co-based composite oxide catalysts,which represent promising candidates for typical chlorinated and oxygenated volatile organic compounds.
基金the Program of National Academy of Sciences of Ukraine KPKVK 6541230“Support for the development of priority areas of scientific research”(0120U101212).
文摘An investigation of hydrotalcite-derived ternary Mg-Al-Ce oxides as catalysts for vapour phase condensation of ethanol to 1-butanol in a flow reactor under atmospheric pressure was carried out.The Mg-Al-Ce oxide systems with Mg/(Al+Ce)ratio from 1 to 4 were synthesized and characterized by XRD,SEM,NMR,and XPS.The study of acid-base characteristics of the systems with different Mg/(Al+Ce)ratio by NH3/CO_(2)quasi-equilibrium thermal desorption techniques shows that the ratio of the catalyst oxide components(Mg,Al,Ce)can provide acid/base capacity ratio close to 3 for the effectivity of the target process.The highest selectivity 68%is reached over Mg-Al-Ce oxide catalyst with the ratio of Mg/(Al+Ce)=2.
文摘<p align="justify"> <span style="font-family:Verdana;">The review outcome represents the optimum catalytic conditions </span><span><span><span style="font-family:'Minion Pro Capt','serif';"><span style="font-family:Verdana;">for the pro</span><span style="font-family:Verdana;">duction of hydrogen using hydrotalcite derived catalysts. It covers dr</span><span style="font-family:Verdana;">y and ste</span><span style="font-family:Verdana;">am reforming of methane, steam reforming of methanol and ethanol t</span><span style="font-family:Verdana;">o hydrogen. The review also revealed the specific properties of hydrotalcite der</span><span style="font-family:Verdana;">ived catalysts for the reactions. Among catalyst investigated, Ni & Fe</span><span style="font-family:Verdana;"> promoted Al-Mg containing hydrotalcite catalyst perform best (99%) for dry reforming of methane at 250°C. For steam methane reforming, Ni containing </span><span style="font-family:Verdana;">ca-aluminates hydrotalcite catalyst act as the best (99%) at 550°C. Cu-supporte</span><span style="font-family:Verdana;">d Zn-Al-containing catalyst performs the best (99.98%) for steam reforming of methanol at 300°C whereas Cu impregnated Mg-Al containing hydrotalcite is </span><span style="font-family:Verdana;">the best (99%) for steam reforming of ethanol at 200°C - 600°C. It’s (HT</span><span style="font-family:Verdana;">) tunable and versatile textural and morphological properties showed excellent catalytic performances for different industrial processes and in sustainable hydrogen production.</span></span></span></span> </p>
基金the financial support by the National Natural Science Foundation of China (21676226 and 21776067)Natural Science Foundation for Distinguished Young Scholars in Hunan Province (2018JJ1023 and 2020JJ2014)+3 种基金Natural Science Foundation in Hunan Province (2018JJ3144)Key Research and Development Program in Hunan Province (2019GK2041)Scientific Research Fund of Hunan Provincial Education Department (17C0630)PhD Startup Foundation of Hunan University of Science and Technology (E51756)
文摘A highly efficient and stable hydrotalcite-derived Cu-MgAlO catalyst was developed for the partial oxidation of cyclohexane with molecular oxygen.The physical–chemical properties of Cu-MgAlO catalysts were studied,and the results indicated that the copper component had been successfully introduced into the hydrotalcite unit layer structure.The catalytic reaction results showed that copper as the active species could activate CAH bond and effectively promote the decomposition of cyclohexyl hydroperoxide(CHHP)to the mixture of cyclohexanol and cyclohexanone(KA oil).8.3%of cyclohexane conversion and 82.9%of selectivity for KA oil were obtained over 9%Cu-MgAlO catalyst at 150℃with 0.6 MPa of oxygen pressure for 2 h.Especially,its catalytic performance was still stable after five runs.