Mesostructured Co3O4-CeO2 composite was found to be an effective catalytic material for the complete oxidation of benzene. The Co3O4-CeO2 catalysts with different Co/Ce ratios （mol/mol） were prepared via the nanocas...Mesostructured Co3O4-CeO2 composite was found to be an effective catalytic material for the complete oxidation of benzene. The Co3O4-CeO2 catalysts with different Co/Ce ratios （mol/mol） were prepared via the nanocasting method and the mesostructure was replicated from two-dimensional （2D） hexagonal SBA-15 and three-dimensional （3D） cubic KIT-6 silicas, respectively. All the obtained Co3O4-CeO2 catalysts exhibited the similar symmetry with the parent silicas and well ordered mesostructures. The Co3O4- CeO2 catalysts with 2D mesostructure showed lower catalytic activities than the corresponding 3D materials. The Co3O4-CeO2 catalyst nanocasted from KIT-6 and with the Co/Ce ratio of 16/1 possessed the best catalytic benzene oxidation activity due to larger quantities of surface hydroxyl groups and surface oxygenated species. The mesostructured Co3O4-CeO2 material thus shows great potential as a promising eco-environmental catalyst for benzene effective elimination.展开更多
CO and formaldehyde(HCHO)oxidation reactions were investigated over mesoporous Ag/Co3O4 catalysts prepared by one-pot(OP)and impregnation(IM)methods.It was found that the one-pot method was superior to the impregnatio...CO and formaldehyde(HCHO)oxidation reactions were investigated over mesoporous Ag/Co3O4 catalysts prepared by one-pot(OP)and impregnation(IM)methods.It was found that the one-pot method was superior to the impregnation method for synthesizing Ag/Co3O4 catalysts with high activity for both reactions.It was also found that the catalytic behavior of mesoporous Co3O4 and Ag/Co3O4 catalysts for the both reactions was different.And the addition of silver on mesoporous Co3O4 did not always enhance the catalytic activity of final catalyst for CO oxidation at room temperature(20 C),but could significantly improve the catalytic activity of final catalyst for HCHO oxidation at low temperature(90 C).The high surface area,uniform pore structure and the pretty good dispersion degree of the silver particle should be responsible for the excellent low-temperature CO oxidation activity.However,for HCHO oxidation,the addition of silver played an important role in the activity enhancement.And the silver particle size and the reducibility of Co3O4 should be indispensable for the high activity of HCHO oxidation at low temperature.展开更多
Up to this date,researchers are still facing difficulties to expand the technology of direct methanol fuel cells(DMFCs) because of the high overpotential required to oxidize the methanol and its relatively poor perfor...Up to this date,researchers are still facing difficulties to expand the technology of direct methanol fuel cells(DMFCs) because of the high overpotential required to oxidize the methanol and its relatively poor performance due to CO poisoning of the leading-high cost anode catalyst.In line with this,we have successfully modified the morphological structure and composition of low cost cobalt based-metal oxides,MCo_2O_4(M = Zn and Ni),with the simple and noble use of polyvinyl pyrrolidone(PVP) as growth modifier and surface stabilizer during the synthesis of nanoparticles in our previous reports,which shown high electrocatalytic activity and strong stability.Due to the good performance of our PVP modified MCo_2O_4 towards pseudocapacitor and oxygen evolution reaction applications,we decided to extend our research study to methanol oxidation reaction.Remarkably,PVP modified Ni Co_2O_4 electrode directly grown on nickel foam substrate via a simple hydrothermal process exhibited better performance compared with PVP modified ZnCo_2O_4 and NiCo_2O_4 without PVP.It had obtained a remarkably low onset potential of 0.285 V and high current density of 280 m A cm^(-2),and shown great stability and high poison tolerance during a continuous CV cycling and Chronoamperometry test,which attained high efficiency of 86.86%and 98.52%,respectively.These positive results of PVP modified Ni Co_2O_4 electrode towards MOR might be attributed to its hierarchical 3 D nanostructures with highly mesoporous surface and large surface area which may have provided numerous electroactive sites,and the exceptional corrosion stability of Ni Co_2O_4 electrode in alkaline solution.展开更多
Distinguished from commonly used Fe2O3 and Fe3O4,a three-dimensional multilevel macromicro-mesoporous structure of FeC2O4/graphene composite has been prepared as binderfree electrode for supercapacitors.The as-prepare...Distinguished from commonly used Fe2O3 and Fe3O4,a three-dimensional multilevel macromicro-mesoporous structure of FeC2O4/graphene composite has been prepared as binderfree electrode for supercapacitors.The as-prepared materials are composed of macroporous graphene and microporous/mesoporous ferrous oxalate.Generally,the decomposition voltage of water is 1.23 V and the practical voltage window limit is about 2 V for asymmetric supercapacitors in aqueous electrolytes.When FeC2O4/rGO hydrogel was used as the negative electrode and a pure rGO hydrogel was used as the positive electrode,the asymmetrical supercapacitor voltage window raised to 1.7 V in KOH(1.0 mol/L)electrolyte and reached up to 2.5 V in a neutral aqueous Na2SO4(1.0 mol/L)electrolyte.Correspondingly it also exhibits a high performance with an energy density of 59.7 Wh/kg.By means of combining a metal oxide that owns micro-mesoporous structure with graphene,this work provides a new opportunity for preparing high-voltage aqueous asymmetric supercapacitors without addition of conductive agent and binder.展开更多
Solubilities and properties (density, conductivity and pH value) of solutions in the quaternary system Li +,K +//CO 2- 3,B 4O 2- 7-H 2O at 288 K were experimentally studied with the isothermal equilibrium method. The ...Solubilities and properties (density, conductivity and pH value) of solutions in the quaternary system Li +,K +//CO 2- 3,B 4O 2- 7-H 2O at 288 K were experimentally studied with the isothermal equilibrium method. The phase diagram of the system consisted of two invariant points E and F, five univariant curves, and four crystallization fields that belonged to K 2CO 3·3/2H 2O,Li 2 B 4O 7·3H 2O, K 2 B 4O 7 ·4H 2O and Li 2CO 3. The composition of the solution corresponding to E was w(CO 2- 3)=2.27 %, w(B 4O 2- 7) =6.05 %, w(K + ) =4.30%,w(Li + )=0.30 % and the equilibrium solids were Li 2 B 4O 7· 3H 2O+K 2 B 4O 7·4H 2O+Li 2CO 3;The composition of the solution for F was w(CO 2- 3) =22.45%,w(B 4O 2- 7)=1.88%,w(K + )=29.96%,w(Li + )=0.03% and the equilibrium solids were K 2CO 3·3/2H 2O+ K 2 B 4O 7·4H 2O+Li 2CO 3. K 2CO 3 possesses strong salting-out effect on K 2 B 4O 7,Li 2CO 3 and Li 2 B 4O 7.展开更多
Compound [Co 3(BTC)(HBTC)(H 2BTC)(C 2H 4O 2) 3]·3(DMF)·6(H 3O) was synthesized under mild conditions and its crystal structure was determined by using single crystal X-ray diffraction. The crystal structure ...Compound [Co 3(BTC)(HBTC)(H 2BTC)(C 2H 4O 2) 3]·3(DMF)·6(H 3O) was synthesized under mild conditions and its crystal structure was determined by using single crystal X-ray diffraction. The crystal structure was solved by direct method and refined by full-matrix least-square method. The crystal is monoclinic and belongs to space group Cc with a=2.645 3(5) nm, b= 1.670 4(3) nm, c=1\^821 6(4) nm, β=128.16(3) °, V=6.329(2) nm 3, Z=2 , D c=20.200 Mg/m 3, M r= 1 314.744, μ=10.274 mm -1, F(000) =38 226, GOF=0.99, R=0.094 1, ωR=0.257 3.展开更多
基金supported by the National Natural Science Funds for Distinguished Young Scholar (No.20725723)the National Basic Research Program of China(No. 2010CB732300)the National High Technology Research and Development Program of China (No.2006AA06A310)
文摘Mesostructured Co3O4-CeO2 composite was found to be an effective catalytic material for the complete oxidation of benzene. The Co3O4-CeO2 catalysts with different Co/Ce ratios （mol/mol） were prepared via the nanocasting method and the mesostructure was replicated from two-dimensional （2D） hexagonal SBA-15 and three-dimensional （3D） cubic KIT-6 silicas, respectively. All the obtained Co3O4-CeO2 catalysts exhibited the similar symmetry with the parent silicas and well ordered mesostructures. The Co3O4- CeO2 catalysts with 2D mesostructure showed lower catalytic activities than the corresponding 3D materials. The Co3O4-CeO2 catalyst nanocasted from KIT-6 and with the Co/Ce ratio of 16/1 possessed the best catalytic benzene oxidation activity due to larger quantities of surface hydroxyl groups and surface oxygenated species. The mesostructured Co3O4-CeO2 material thus shows great potential as a promising eco-environmental catalyst for benzene effective elimination.
基金supported financially by the Program for New Century Excellent Talents in University (NCET-09-0256)the Fundamental Research Funds for the Central Universities (DUT13LK27)the National Nature Science Foundation of China (No.21377016)
文摘CO and formaldehyde(HCHO)oxidation reactions were investigated over mesoporous Ag/Co3O4 catalysts prepared by one-pot(OP)and impregnation(IM)methods.It was found that the one-pot method was superior to the impregnation method for synthesizing Ag/Co3O4 catalysts with high activity for both reactions.It was also found that the catalytic behavior of mesoporous Co3O4 and Ag/Co3O4 catalysts for the both reactions was different.And the addition of silver on mesoporous Co3O4 did not always enhance the catalytic activity of final catalyst for CO oxidation at room temperature(20 C),but could significantly improve the catalytic activity of final catalyst for HCHO oxidation at low temperature(90 C).The high surface area,uniform pore structure and the pretty good dispersion degree of the silver particle should be responsible for the excellent low-temperature CO oxidation activity.However,for HCHO oxidation,the addition of silver played an important role in the activity enhancement.And the silver particle size and the reducibility of Co3O4 should be indispensable for the high activity of HCHO oxidation at low temperature.
基金supported by the Korea Institute of Energy Technology Evaluation and Planning (KETEP) - Grants funded by the Ministry of Trade,Industry and Energy (MOTIE) (No.20174010201160)the National Research Foundation of Korea (NRF) - Grant funded by the Ministry of Education (No.20090093816),Republic of Korea
文摘Up to this date,researchers are still facing difficulties to expand the technology of direct methanol fuel cells(DMFCs) because of the high overpotential required to oxidize the methanol and its relatively poor performance due to CO poisoning of the leading-high cost anode catalyst.In line with this,we have successfully modified the morphological structure and composition of low cost cobalt based-metal oxides,MCo_2O_4(M = Zn and Ni),with the simple and noble use of polyvinyl pyrrolidone(PVP) as growth modifier and surface stabilizer during the synthesis of nanoparticles in our previous reports,which shown high electrocatalytic activity and strong stability.Due to the good performance of our PVP modified MCo_2O_4 towards pseudocapacitor and oxygen evolution reaction applications,we decided to extend our research study to methanol oxidation reaction.Remarkably,PVP modified Ni Co_2O_4 electrode directly grown on nickel foam substrate via a simple hydrothermal process exhibited better performance compared with PVP modified ZnCo_2O_4 and NiCo_2O_4 without PVP.It had obtained a remarkably low onset potential of 0.285 V and high current density of 280 m A cm^(-2),and shown great stability and high poison tolerance during a continuous CV cycling and Chronoamperometry test,which attained high efficiency of 86.86%and 98.52%,respectively.These positive results of PVP modified Ni Co_2O_4 electrode towards MOR might be attributed to its hierarchical 3 D nanostructures with highly mesoporous surface and large surface area which may have provided numerous electroactive sites,and the exceptional corrosion stability of Ni Co_2O_4 electrode in alkaline solution.
基金supported by the National Natural Science Foundation of China (No.51673180 and No. 51673180)
文摘Distinguished from commonly used Fe2O3 and Fe3O4,a three-dimensional multilevel macromicro-mesoporous structure of FeC2O4/graphene composite has been prepared as binderfree electrode for supercapacitors.The as-prepared materials are composed of macroporous graphene and microporous/mesoporous ferrous oxalate.Generally,the decomposition voltage of water is 1.23 V and the practical voltage window limit is about 2 V for asymmetric supercapacitors in aqueous electrolytes.When FeC2O4/rGO hydrogel was used as the negative electrode and a pure rGO hydrogel was used as the positive electrode,the asymmetrical supercapacitor voltage window raised to 1.7 V in KOH(1.0 mol/L)electrolyte and reached up to 2.5 V in a neutral aqueous Na2SO4(1.0 mol/L)electrolyte.Correspondingly it also exhibits a high performance with an energy density of 59.7 Wh/kg.By means of combining a metal oxide that owns micro-mesoporous structure with graphene,this work provides a new opportunity for preparing high-voltage aqueous asymmetric supercapacitors without addition of conductive agent and binder.
文摘Solubilities and properties (density, conductivity and pH value) of solutions in the quaternary system Li +,K +//CO 2- 3,B 4O 2- 7-H 2O at 288 K were experimentally studied with the isothermal equilibrium method. The phase diagram of the system consisted of two invariant points E and F, five univariant curves, and four crystallization fields that belonged to K 2CO 3·3/2H 2O,Li 2 B 4O 7·3H 2O, K 2 B 4O 7 ·4H 2O and Li 2CO 3. The composition of the solution corresponding to E was w(CO 2- 3)=2.27 %, w(B 4O 2- 7) =6.05 %, w(K + ) =4.30%,w(Li + )=0.30 % and the equilibrium solids were Li 2 B 4O 7· 3H 2O+K 2 B 4O 7·4H 2O+Li 2CO 3;The composition of the solution for F was w(CO 2- 3) =22.45%,w(B 4O 2- 7)=1.88%,w(K + )=29.96%,w(Li + )=0.03% and the equilibrium solids were K 2CO 3·3/2H 2O+ K 2 B 4O 7·4H 2O+Li 2CO 3. K 2CO 3 possesses strong salting-out effect on K 2 B 4O 7,Li 2CO 3 and Li 2 B 4O 7.
基金Research Project from Department of Science and Technology of Shandong Province(2012GGA01012)Scientific ResearchFoundation for the Returned Overseas Chinese Scholars of State Education Ministry(2004-527)
文摘Compound [Co 3(BTC)(HBTC)(H 2BTC)(C 2H 4O 2) 3]·3(DMF)·6(H 3O) was synthesized under mild conditions and its crystal structure was determined by using single crystal X-ray diffraction. The crystal structure was solved by direct method and refined by full-matrix least-square method. The crystal is monoclinic and belongs to space group Cc with a=2.645 3(5) nm, b= 1.670 4(3) nm, c=1\^821 6(4) nm, β=128.16(3) °, V=6.329(2) nm 3, Z=2 , D c=20.200 Mg/m 3, M r= 1 314.744, μ=10.274 mm -1, F(000) =38 226, GOF=0.99, R=0.094 1, ωR=0.257 3.
