ZrO2-based mixed metal oxide catalysts for the industrially important dehydrogenation process of ethylbenzene to styrene monomer have been explored by our group for the past 20 years.These efforts were subjected to th...ZrO2-based mixed metal oxide catalysts for the industrially important dehydrogenation process of ethylbenzene to styrene monomer have been explored by our group for the past 20 years.These efforts were subjected to the activation of CO2 over mixed metal oxide catalysts and resulted in several promising benefits to the dehydrogenation processes,such as stabilized conversion and selectivity,suppressed coke formation and commercially-acceptable longevity.In this review,we summarize the most recent developments on ZrO2-based mixed metal oxide catalysts,including the further optimization of sol-gel process in the synthesis of catalysts,rationalizing acid-base properties by doping,co-operative properties between redox and acid-base active sites and additional promoters towards the effective improvement of the longevity of catalysts.展开更多
A series of Mg‐Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine.The structure and surface properties of Mg‐Al oxides ...A series of Mg‐Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine.The structure and surface properties of Mg‐Al oxides are modulated by changing the Mg/Al ratios,calcination temperature and treatment with probe molecules.Detailed characterization,including X‐ray diffraction,27Al magic angle spinning nuclear magnetic resonance spectroscopy,N2‐adsorption,NH3‐temperature‐programmed desorption,CO2‐temperature‐programmed desorption and X‐ray photoelectron spectroscopy are carried out to determine the physicochemical properties of these catalysts.The Mg‐Al oxides with Mg/Al=3exhibit the highest activity in the reaction,which possess a large number of surface weak basic sites and a relatively small number of weak acidic sites.The role of the acidic and basic sites in the reaction process is systematically investigated,and are shown to serve as adsorption and activation sites for amines and alcohols,respectively.Under the synergistic effect of these acid‐base centers,the oxidative coupling process successfully occurs on the surface of Mg‐Al mixed oxides.Compared with the acidic sites,the weak basic sites play a more important role in the catalytic process.The acidic sites are the catalytic centers for the benzyl alcohol activation,which control the reaction rate of the oxidative coupling reaction.展开更多
The design and preparation of suitable supports are of great importance for gold catalysts to attain excellent catalytic performance for alcohol oxidation.In this work,we found that ZnO-CuO mixed oxides supported gold...The design and preparation of suitable supports are of great importance for gold catalysts to attain excellent catalytic performance for alcohol oxidation.In this work,we found that ZnO-CuO mixed oxides supported gold catalysts showed much better catalytic activity for base-free aerobic oxidation of benzyl alcohol than Au/ZnO and Au/CuO catalysts,and among them Au/Zn0.7Cu0.3O displayed the best catalytic performance.In addition,the Au/Zn0.7Cu0.3O catalyst could selectively catalyze the aerobic oxidation of a wide range of alcohols to produce the corresponding carbonyl compounds with high yields under mild conditions without base.Further characterizations indicated that the outstanding catalytic performance of Au/Zn0.7Cu0.3O was correlated with the small size of Au nanoparticles(NPs),good low-temperature reducibility,high concentration of surface oxygen species,and collaborative interaction between Au NPs and mixed oxide.展开更多
There has been increasing interest in devel- oping micro/nanostructured aluminum-based materials for sustainable, dependable and high-efficiency electro- chemical energy storage. This review chiefly discusses the alum...There has been increasing interest in devel- oping micro/nanostructured aluminum-based materials for sustainable, dependable and high-efficiency electro- chemical energy storage. This review chiefly discusses the aluminum-based electrode materials mainly including A1203, AIF3, AIPO4, AI（OH）3, as well as the composites （carbons, silicons, metals and transition metal oxides） for lithium-ion batteries, the development of aluminum-ion batteries, and nickel-metal hydride alkaline secondary batteries, which summarizes the methodologies, related charge-storage mechanisms, the relationship between nanos- tructures and electrochemical properties found in recent years, latest research achievements and their potential ap- plications. In addition, we raise the relevant challenges in recently developed electrode materials and put forward new ideas for further development of micro/nanostructured aluminum-based materials in advanced battery systems.展开更多
基金funded by Saudi Arabia Basic Industries Corporation(Kingdom of Saudi Arabia),the BK21 Plus Project in 2014
文摘ZrO2-based mixed metal oxide catalysts for the industrially important dehydrogenation process of ethylbenzene to styrene monomer have been explored by our group for the past 20 years.These efforts were subjected to the activation of CO2 over mixed metal oxide catalysts and resulted in several promising benefits to the dehydrogenation processes,such as stabilized conversion and selectivity,suppressed coke formation and commercially-acceptable longevity.In this review,we summarize the most recent developments on ZrO2-based mixed metal oxide catalysts,including the further optimization of sol-gel process in the synthesis of catalysts,rationalizing acid-base properties by doping,co-operative properties between redox and acid-base active sites and additional promoters towards the effective improvement of the longevity of catalysts.
文摘A series of Mg‐Al mixed oxide catalysts are prepared and introduced as efficient irreducible catalysts for the oxidative coupling of alcohols and amines to imine.The structure and surface properties of Mg‐Al oxides are modulated by changing the Mg/Al ratios,calcination temperature and treatment with probe molecules.Detailed characterization,including X‐ray diffraction,27Al magic angle spinning nuclear magnetic resonance spectroscopy,N2‐adsorption,NH3‐temperature‐programmed desorption,CO2‐temperature‐programmed desorption and X‐ray photoelectron spectroscopy are carried out to determine the physicochemical properties of these catalysts.The Mg‐Al oxides with Mg/Al=3exhibit the highest activity in the reaction,which possess a large number of surface weak basic sites and a relatively small number of weak acidic sites.The role of the acidic and basic sites in the reaction process is systematically investigated,and are shown to serve as adsorption and activation sites for amines and alcohols,respectively.Under the synergistic effect of these acid‐base centers,the oxidative coupling process successfully occurs on the surface of Mg‐Al mixed oxides.Compared with the acidic sites,the weak basic sites play a more important role in the catalytic process.The acidic sites are the catalytic centers for the benzyl alcohol activation,which control the reaction rate of the oxidative coupling reaction.
基金supported by the National Natural Science Foundation of China(21606219)the “Transformational Technologies for Clean Energy and Demonstration”,Strategic Priority Research Program of the Chinese Academy of Sciences(XDA21030900)~~
文摘The design and preparation of suitable supports are of great importance for gold catalysts to attain excellent catalytic performance for alcohol oxidation.In this work,we found that ZnO-CuO mixed oxides supported gold catalysts showed much better catalytic activity for base-free aerobic oxidation of benzyl alcohol than Au/ZnO and Au/CuO catalysts,and among them Au/Zn0.7Cu0.3O displayed the best catalytic performance.In addition,the Au/Zn0.7Cu0.3O catalyst could selectively catalyze the aerobic oxidation of a wide range of alcohols to produce the corresponding carbonyl compounds with high yields under mild conditions without base.Further characterizations indicated that the outstanding catalytic performance of Au/Zn0.7Cu0.3O was correlated with the small size of Au nanoparticles(NPs),good low-temperature reducibility,high concentration of surface oxygen species,and collaborative interaction between Au NPs and mixed oxide.
基金supported by the Program for New Century Excellent Talents of the University in China (NCET-13-0645)the National Natural Science Foundation of China (21201010, 21671170 and 21673203)+5 种基金the Innovation Scientists and Technicians Troop Construction Projects of Henan Province (164200510018)the Program for Innovative Research Team (in Science and Technology) in the University of Henan Province (14IRTSTHN004)the Six Talent Plan (2015-XCL030)Qinglan Projectthe Priority Academic Program Development of Jiangsu Higher Education Institutionsthe Undergraduate Scientific Research Innovation Projects in Jiangsu province (201611117047Y)
文摘There has been increasing interest in devel- oping micro/nanostructured aluminum-based materials for sustainable, dependable and high-efficiency electro- chemical energy storage. This review chiefly discusses the aluminum-based electrode materials mainly including A1203, AIF3, AIPO4, AI（OH）3, as well as the composites （carbons, silicons, metals and transition metal oxides） for lithium-ion batteries, the development of aluminum-ion batteries, and nickel-metal hydride alkaline secondary batteries, which summarizes the methodologies, related charge-storage mechanisms, the relationship between nanos- tructures and electrochemical properties found in recent years, latest research achievements and their potential ap- plications. In addition, we raise the relevant challenges in recently developed electrode materials and put forward new ideas for further development of micro/nanostructured aluminum-based materials in advanced battery systems.
