Due to the easily controllable interlayer anions, metal cation composition proportion and thickness, which is beneficial to modify surface chemical state and tune bandgap, layered double hydroxides(LDHs) have great pr...Due to the easily controllable interlayer anions, metal cation composition proportion and thickness, which is beneficial to modify surface chemical state and tune bandgap, layered double hydroxides(LDHs) have great promising potential for photocatalytic applications. In this study,we have successfully synthesized the ZnAl–LDH intercalated the single anion between ZnAl cationic interlayer without anionic impurities by using a facile calcining and reconstructing routes. The electron structure and surface chemical state of the prepared products have been investigated by combining the DFT calculation and experimental characterization methods. UV–vis DRS was used to certify the light absorption of the prepared products, and we performed the DFT calculation to demonstrate the density of state and activation of reactant. These results suggested that the ZnAl–LDH–CO3 possessed the more proper band structure and superior ability to activate NO and O2 for accelerating the photocatalytic NO oxidation activity. Moreover, the in situ DRIFTS with dynamically monitoring intermediates and products over the ZnAl–LDH–CO3 was adopted to declare the photocatalytic NO oxidized process during the photocatalytic reaction process. This work illustrated the influence of different interlayer anions to the electron structure and surface chemical state of ZnAl–LDH structure through the experimental verification combined DFT calculation and the photocatalytic NO oxidized process via in situ DRIFTS analyzing, which would provide a novel way to design and fabricate the efficient photocatalysis, and understand the reaction process.展开更多
Charge separation and transformation are some of the key requirements for high-efficiency photocatalysis. The photocatalytic reaction mechanism provides a guideline for the development and commercialization of high-ef...Charge separation and transformation are some of the key requirements for high-efficiency photocatalysis. The photocatalytic reaction mechanism provides a guideline for the development and commercialization of high-efficiency photocatalysts. In this study, we designed and favorably synthesized BMO@BOC heterojunctions via a facile solvothermal route and applied the heat treatment method for application in high-efficiency photocatalytic NO removal. More importantly, both continuous stream and intermittent stream methods with in situ diffuse reflectance infrared Fourier transform spectroscopy were applied to intuitively and dynamically investigate the adsorption process and oxidation process of NO removal over the photocatalyst surface. The intermediate products(NO-, NO2-, and NO2) were explicitly detected in both the adsorption process and oxidation process, whilst the final product(NO3-) appeared only in the oxidation process, owing to the separation, migration, and conversion of photoinduced electron-hole pairs.展开更多
High electrochemically active bimessite is always desirable pseudocapacitive material for supercapacitor.Here,two-dimensional(2D)compulsive malposition parallel bimessite standing on β-MnO_(2) interconnected networks...High electrochemically active bimessite is always desirable pseudocapacitive material for supercapacitor.Here,two-dimensional(2D)compulsive malposition parallel bimessite standing on β-MnO_(2) interconnected networks have been designed.Due to the retrition of β-MnO_(2),compulsi ve malposition,slippage of MnO6 slab,occured in bimessite resulting in weaken bi nding force between bimessi te slab and interlayer cations,which enhanced their electrochemical performances.Additionally,the electrical conductivity of the structure was largely promoted by the 2D charge transfer route and double-exchange mechanism in bimessite,also leading to desirable electro-chemical properties.Based on the fraction of as-prepared nanostructure,the par all bimessite exhibited good pseudocapacitance performance(660 F g^(-1))with high rate capability.In addition,the asymmetrice supercapacitor assembled by reduced graphene oxide(RGO)and as-prepared nanostructure,which respectively served as the negative and positive eletrode,delivered an energy density of 33.1 Wh kg^(-1) and a mad mum power density of 64.0 kW kg^(-1) with excellent cyeling stability(95.8% after 10000 cycles).Finally,the study opens new avenwes for synthesizing high eletrochemically actiwe bimessite structure for high-performance energy storage devices.展开更多
Supercapacitors with good electrochemical performance and flexibility are in great demand.In this paper,the concept of preparing 3D porous carbon monoliths via direct calcination of melamine sponge is presented.This p...Supercapacitors with good electrochemical performance and flexibility are in great demand.In this paper,the concept of preparing 3D porous carbon monoliths via direct calcination of melamine sponge is presented.This preparation method is simple and has good control of the structure.Porous carbon composite nickel-manga nese oxides can be obtained by hydrothermal method followed with calcination.The electrochemical performances were tested and porous carbon monoliths with NiMn oxides exhibited a specific capacitance of 870 F/g in 1 mol/L KOH at a charge/discharge current density of 0.5 A/g and a capacity retention of 89.9% after 5000 times charge and discharge.展开更多
基金financial support of the Fundamental Research Funds for the Central Universities (2018CDYJSY0055, 106112017CDJXSYY0001, 106112017C DJQJ138802, 106112017CDJXSYY0001, 106112017CDJS K04XK11, and 2018CDQYCL0027)the National Natural Science Foundation of China (Grant no. 21576034)+2 种基金the Innovative Research Team of Chongqing (CXTDG201602014)Project funded by Chongqing Special Postdoctoral Science Foundation (XmT2018043)Technological projects of Chongqing Municipal Education Commission (KJZDK201800801)
文摘Due to the easily controllable interlayer anions, metal cation composition proportion and thickness, which is beneficial to modify surface chemical state and tune bandgap, layered double hydroxides(LDHs) have great promising potential for photocatalytic applications. In this study,we have successfully synthesized the ZnAl–LDH intercalated the single anion between ZnAl cationic interlayer without anionic impurities by using a facile calcining and reconstructing routes. The electron structure and surface chemical state of the prepared products have been investigated by combining the DFT calculation and experimental characterization methods. UV–vis DRS was used to certify the light absorption of the prepared products, and we performed the DFT calculation to demonstrate the density of state and activation of reactant. These results suggested that the ZnAl–LDH–CO3 possessed the more proper band structure and superior ability to activate NO and O2 for accelerating the photocatalytic NO oxidation activity. Moreover, the in situ DRIFTS with dynamically monitoring intermediates and products over the ZnAl–LDH–CO3 was adopted to declare the photocatalytic NO oxidized process during the photocatalytic reaction process. This work illustrated the influence of different interlayer anions to the electron structure and surface chemical state of ZnAl–LDH structure through the experimental verification combined DFT calculation and the photocatalytic NO oxidized process via in situ DRIFTS analyzing, which would provide a novel way to design and fabricate the efficient photocatalysis, and understand the reaction process.
基金supported by the Fundamental Research Funds for the Central Universities(2018CDYJSY0055)the National Natural Science Foundation of China(21576034)+3 种基金Joint Funds of the National Natural Science Foundation of China-Guangdong(U1801254)the project funded by Chongqing Special Postdoctoral Science Foundation(Xm T2018043)Technological projects of Chongqing Municipal Education Commission(KJZDK201800801)the Innovative Research Team of Chongqing(CXTDG201602014)~~
文摘Charge separation and transformation are some of the key requirements for high-efficiency photocatalysis. The photocatalytic reaction mechanism provides a guideline for the development and commercialization of high-efficiency photocatalysts. In this study, we designed and favorably synthesized BMO@BOC heterojunctions via a facile solvothermal route and applied the heat treatment method for application in high-efficiency photocatalytic NO removal. More importantly, both continuous stream and intermittent stream methods with in situ diffuse reflectance infrared Fourier transform spectroscopy were applied to intuitively and dynamically investigate the adsorption process and oxidation process of NO removal over the photocatalyst surface. The intermediate products(NO-, NO2-, and NO2) were explicitly detected in both the adsorption process and oxidation process, whilst the final product(NO3-) appeared only in the oxidation process, owing to the separation, migration, and conversion of photoinduced electron-hole pairs.
基金the National Natural Science Foundation of China(Grant No.51908092)Projects(No.2020CDJXZ001,2020CDCGJ006 and 2020CDCGCL004)supported by the Fundamental Research Funds for the Central Universities,the Joint Funds of the National Natural Science Foundation of China-Guangdong(Grant No.U1801254)+5 种基金the project funded by Chongqing Special Postdoctoral Science Foundation(XmT2018043)the Chongqing Research Program of Basic Research and Frontier Technology(cstc2017jcyjBX0080)Natural Science Foundation Project of Chongqing for Post-doctor(cstc2019jcyjbsh0079,cstc2019jcyjbshX0085)Technological projects of Chongqing Municipal Education Commission(KJZDK201800801)the Innovative Research Team of Chongqing(CXTDG201602014)the Innovative technology of New materials and metallurgy(2019CDXYCL0031).
文摘High electrochemically active bimessite is always desirable pseudocapacitive material for supercapacitor.Here,two-dimensional(2D)compulsive malposition parallel bimessite standing on β-MnO_(2) interconnected networks have been designed.Due to the retrition of β-MnO_(2),compulsi ve malposition,slippage of MnO6 slab,occured in bimessite resulting in weaken bi nding force between bimessi te slab and interlayer cations,which enhanced their electrochemical performances.Additionally,the electrical conductivity of the structure was largely promoted by the 2D charge transfer route and double-exchange mechanism in bimessite,also leading to desirable electro-chemical properties.Based on the fraction of as-prepared nanostructure,the par all bimessite exhibited good pseudocapacitance performance(660 F g^(-1))with high rate capability.In addition,the asymmetrice supercapacitor assembled by reduced graphene oxide(RGO)and as-prepared nanostructure,which respectively served as the negative and positive eletrode,delivered an energy density of 33.1 Wh kg^(-1) and a mad mum power density of 64.0 kW kg^(-1) with excellent cyeling stability(95.8% after 10000 cycles).Finally,the study opens new avenwes for synthesizing high eletrochemically actiwe bimessite structure for high-performance energy storage devices.
基金financial support from the National Natural Science Foundation of China(Nos.21576034 and 51908092)the State Education Ministry and Fundamental Research Funds for the Central Universities(Nos.2019CDQYCL042,2019CDXYCL0031,2018CDYJSY0055,2018CDQYCL0027,106112017CDJQJ138802,106112017CDJSK04XK11 and 106112017CDJXSYY0001)the Joint Funds of the National Natural Science Foundation of ChinaGuangdong(No.U1801254)。
文摘Supercapacitors with good electrochemical performance and flexibility are in great demand.In this paper,the concept of preparing 3D porous carbon monoliths via direct calcination of melamine sponge is presented.This preparation method is simple and has good control of the structure.Porous carbon composite nickel-manga nese oxides can be obtained by hydrothermal method followed with calcination.The electrochemical performances were tested and porous carbon monoliths with NiMn oxides exhibited a specific capacitance of 870 F/g in 1 mol/L KOH at a charge/discharge current density of 0.5 A/g and a capacity retention of 89.9% after 5000 times charge and discharge.