Following publication of the original article[1],the authors found that they pasted the same data when drawing XRD for sample NCO-1 and NCO-2 in Fig.2a,however,the XRD of all four samples in the manuscript was tested,...Following publication of the original article[1],the authors found that they pasted the same data when drawing XRD for sample NCO-1 and NCO-2 in Fig.2a,however,the XRD of all four samples in the manuscript was tested,and XRD raw data were kept and can be offered.The correct Fig.2 has been provided in this Correction.展开更多
Binary metal oxide（MnOx-A/TiO2）catalysts were prepared by adding the second metal to manganese oxides supported on titanium dioxide（TiO2）,where,A indicates Fe2O3,WO3,MoO3,and Cr2O3.Their catalytic activity,N2 sele...Binary metal oxide（MnOx-A/TiO2）catalysts were prepared by adding the second metal to manganese oxides supported on titanium dioxide（TiO2）,where,A indicates Fe2O3,WO3,MoO3,and Cr2O3.Their catalytic activity,N2 selectivity,and SO2 poisonous tolerance were investigated.The catalytic performance at low temperatures decreased in the following order：Mn-W/TiO2〉Mn-Fe/TiO2〉Mn-Cr/TiO2〉Mn-Mo/TiO2,whereas the N2 selectivity decreased in the order：Mn-Fe/TiO2〉Mn-W/TiO2〉Mn-Mo/TiO2〉Mn-Cr/TiO2.In the presence of 0.01%SO2 and 6%H2O,the NOx conversions in the presence of Mn-W/TiO2,Mn-Fe/TiO2,or Mn-Mo/TiO2 maintain 98.5%,95.8%and 94.2%, respectively,after 8 h at 120°C at GHSV 12600 h？ 1 .As effective promoters,WO3 and Fe2O3 can increase N2 selectivity and the resistance to SO2 of MnOx/TiO2 significantly.The Fourier transform infrared（FTIR）spectra of NH3 over WO3 show the presence of Lewis acid sites.The results suggest that WO3 is the best promoter of MnOx/TiO2,and Mn-W/TiO2 is one of the most active catalysts for the low temperature selective catalytic reduction of NO with NH3.展开更多
Non-thermal plasma(NTP)has been demonstrated as one of the promising technologies that can degrade volatile organic compounds(VOCs)under ambient condition.However,one of the key challenges of VOCs degradation in NTP i...Non-thermal plasma(NTP)has been demonstrated as one of the promising technologies that can degrade volatile organic compounds(VOCs)under ambient condition.However,one of the key challenges of VOCs degradation in NTP is its relatively low mineralization rate,which needs to be addressed by introducing catalysts.Therefore,the design and optimization of catalysts have become the focus of NTP coupling catalysis research.In thiswork,a series of two-dimensional nanosheet Co-Ni metal oxides were synthesized by microwave method and investigated for the catalytic oxidation of benzene in an NTP-catalysis coupling system.Among them,Co_(2)Ni_(1)O_(x)achieves 60%carbon dioxide(CO_(2))selectivity(SCO_(2))when the benzene removal efficiency(REbenzene)reaches more than 99%,which is a significant enhancement compared with the CO_(2)selectivity obtained without any catalysts(38%)under the same input power.More intriguingly,this SCO_(2)is also significantly higher than that of single metal oxides,NiO or Co_(3)O_(4),which is only around 40%.Such improved performance of this binary metal oxide catalyst is uniquely attributed to the synergistic effects of Co and Ni in Co_(2)Ni_(1)O_(x)catalyst.The introduction of Co_(2)Ni_(1)O_(x)was found to promote the generation of acrolein significantly,one of the key intermediates found in NTP alone system reported previously,suggest the benzene ring open reaction is promoted.Compared with monometallic oxides NiO and Co_(3)O_(4),Co_(2)Ni_(1)O_(x)also shows higher active oxygen proportion,better oxygenmobility,and stronger low-temperature redox capability.The above factors result in the improved catalytic performance of Co_(2)Ni_(1)O_(x)in the NTP coupling removal of benzene.展开更多
The thermal decomposition characteristic of ammonium perchlorate(AP)represents a critical factor in determining the performance of solid propellants,which has aroused significant interest on the structure and performa...The thermal decomposition characteristic of ammonium perchlorate(AP)represents a critical factor in determining the performance of solid propellants,which has aroused significant interest on the structure and performance improvement of kinds of catalysts.In this study,bimetallic metal-organic frameworks(MOFs),such as CuCo-BTC(BTC=1,3,5-Benzenetricarboxylic acid,H_(3)BTC),CuNi-BTC,and CoNi-BTC,were synthesized by solvothermal(ST)and spray-drying(SD)methods,and then calcined at 400℃for 2 h to form metal oxides.The catalysts as well as their catalytic effects for AP decomposition were characterized by FTIR,XRD,SEM,XPS,TG,DSC,TG-IR,EIS,CV,and LSV.It was found that the rapid coordination of metal ions with ligands during spray drying may lead to catalytic structural defects,promoting the exposure of reactive active sites and increasing the catalytic active region.The results showed that the addition of 2 wt%binary transition metal oxides(BTMOs)as catalysts significantly reduced the high-temperature decomposition(HTD)temperature of AP and enhanced its heat release.Of particular significance is the observation that SD-CoNiO_(x),prepared by spray-drying,reduced the decomposition temperature of AP from 413.26℃(pure AP)to 306℃and enhanced the heat release from 256.79 J/g(pure AP)to 1496.82 J/g,while concomitantly reducing the activation energy by 42%.By analysing the gaseous products during the decomposition of AP+SD-CoNiO_(x)and AP+ST-CoNiO_(x),it was found that SD-CoNiO_(x)could significantly increase the content of high-valent nitrogen oxides during the AP decomposition reaction,which indicates that the BTMOs prepared by spray-drying in the reaction system are more conducive to accelerating the electron transfer in the thermal decomposition process of AP,and can provide a high concentration of reactive oxygen species that oxidize AP to high-valent nitrogen oxide-containing compounds.The present study shows that the structure selectivity of the spray-drying technique influences surfactant molecular arrangement on catalyst surfaces,resulting in their ability to promote higher electron transfer during the catalytic process.Therefore,BTMOs prepared by spray drying method have higher potential for application.展开更多
The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based so...The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based solids with oxides from alkali (Li2O), alkaline earth (CaO), and transition metal groups (WO3 or MnO). The presence of the peroxide (O2-2) active sites on the Li2O2, revealed by Raman spectroscopy, may be the key factor in the enhanced performance of some of the Li2O/MgO catalysts. The high reducibility of the CeO2 catalyst, an important factor in the CO2-OCM catalyst activity, may be enhanced by the presence of manganese oxide species. The manganese oxide species increases oxygen mobility and oxygen vacancies in the CeO2 catalyst. Raman and Fourier Transform Infra Red (FT-IR) spectroscopies revealed the presence of lattice vibrations of metal-oxygen bondings and active sites in which the peaks corresponding to the bulk crystalline structures of Li2O, CaO, WO3 and MnO are detected. The performance of 5%MnO/15%CaO/CeO2 catalyst is the most potential among the CeO2-based catalysts, although lower than the 2%Li2O/MgO catalyst. The 2%Li2O/MgO catalyst showed the most promising C2+ hydrocarbons selectivity and yield at 98.0% and 5.7%, respectively.展开更多
Because of the intensified electrochemical activities,mixed metal oxides as a representative for pseudocapacitive materials play a key role for high performance supercapacitor electrodes.Nevertheless,low ion and elect...Because of the intensified electrochemical activities,mixed metal oxides as a representative for pseudocapacitive materials play a key role for high performance supercapacitor electrodes.Nevertheless,low ion and electron transfer rate and poor cycling performance in the electrode practically restrict further promotion of their electrochemical performance.In order to offset the defect,a novel copper(Cu)foamsupported nickel molybdate nanosheet decorated carbon nanotube wrapped copper oxide nanowire array(NiMoO4 NSs-CNTs-CuO NWAs/Cu foam)flexible electrode is constructed.The as-prepared electrode demonstrates a unique core-shell holey nanostructure with a large active surface area,which can provide a large number of active sites for redox reactions.Besides,the CNTs networks supply improved conductivity,which can hasten electron transport.Through this simple and efficient design method,the spatial distribution of each component in the flexible electrode is more orderly,short and fast electron transport path with low intrinsic resistance.As a result,the NiMoO4 NSs-CNTs-CuO NWAs/Cu foam as an adhesiveless supercapacitor electrode material exhibits excellent ene rgy storage perfo rmance with high specific areal capacitance of 23.40 F cm^(-2)at a current density of 2 mA cm^(-2),which outperforms most of the flexible electrodes re ported recently.The assembled asymmetric supercapacitor demonstrates an energy density up to 96.40 mW h cm^(-3)and a power density up to 0.4 W cm^(-3)under a working voltage window of 1.7 V.In addition,outstanding flexibility of up to 100°bend and good cycling stability with the capacitance retention of 82.53%after 10,000 cycles can be obtained.展开更多
文摘Following publication of the original article[1],the authors found that they pasted the same data when drawing XRD for sample NCO-1 and NCO-2 in Fig.2a,however,the XRD of all four samples in the manuscript was tested,and XRD raw data were kept and can be offered.The correct Fig.2 has been provided in this Correction.
文摘Binary metal oxide（MnOx-A/TiO2）catalysts were prepared by adding the second metal to manganese oxides supported on titanium dioxide（TiO2）,where,A indicates Fe2O3,WO3,MoO3,and Cr2O3.Their catalytic activity,N2 selectivity,and SO2 poisonous tolerance were investigated.The catalytic performance at low temperatures decreased in the following order：Mn-W/TiO2〉Mn-Fe/TiO2〉Mn-Cr/TiO2〉Mn-Mo/TiO2,whereas the N2 selectivity decreased in the order：Mn-Fe/TiO2〉Mn-W/TiO2〉Mn-Mo/TiO2〉Mn-Cr/TiO2.In the presence of 0.01%SO2 and 6%H2O,the NOx conversions in the presence of Mn-W/TiO2,Mn-Fe/TiO2,or Mn-Mo/TiO2 maintain 98.5%,95.8%and 94.2%, respectively,after 8 h at 120°C at GHSV 12600 h？ 1 .As effective promoters,WO3 and Fe2O3 can increase N2 selectivity and the resistance to SO2 of MnOx/TiO2 significantly.The Fourier transform infrared（FTIR）spectra of NH3 over WO3 show the presence of Lewis acid sites.The results suggest that WO3 is the best promoter of MnOx/TiO2,and Mn-W/TiO2 is one of the most active catalysts for the low temperature selective catalytic reduction of NO with NH3.
基金supported by the National Key Research and Development Program of China(No.2017YFE0127500)National Natural Science Foundation of China(No.U1832155).
文摘Non-thermal plasma(NTP)has been demonstrated as one of the promising technologies that can degrade volatile organic compounds(VOCs)under ambient condition.However,one of the key challenges of VOCs degradation in NTP is its relatively low mineralization rate,which needs to be addressed by introducing catalysts.Therefore,the design and optimization of catalysts have become the focus of NTP coupling catalysis research.In thiswork,a series of two-dimensional nanosheet Co-Ni metal oxides were synthesized by microwave method and investigated for the catalytic oxidation of benzene in an NTP-catalysis coupling system.Among them,Co_(2)Ni_(1)O_(x)achieves 60%carbon dioxide(CO_(2))selectivity(SCO_(2))when the benzene removal efficiency(REbenzene)reaches more than 99%,which is a significant enhancement compared with the CO_(2)selectivity obtained without any catalysts(38%)under the same input power.More intriguingly,this SCO_(2)is also significantly higher than that of single metal oxides,NiO or Co_(3)O_(4),which is only around 40%.Such improved performance of this binary metal oxide catalyst is uniquely attributed to the synergistic effects of Co and Ni in Co_(2)Ni_(1)O_(x)catalyst.The introduction of Co_(2)Ni_(1)O_(x)was found to promote the generation of acrolein significantly,one of the key intermediates found in NTP alone system reported previously,suggest the benzene ring open reaction is promoted.Compared with monometallic oxides NiO and Co_(3)O_(4),Co_(2)Ni_(1)O_(x)also shows higher active oxygen proportion,better oxygenmobility,and stronger low-temperature redox capability.The above factors result in the improved catalytic performance of Co_(2)Ni_(1)O_(x)in the NTP coupling removal of benzene.
基金supported by the National Natural ScienceFoundation of China(Grant No.52203332)。
文摘The thermal decomposition characteristic of ammonium perchlorate(AP)represents a critical factor in determining the performance of solid propellants,which has aroused significant interest on the structure and performance improvement of kinds of catalysts.In this study,bimetallic metal-organic frameworks(MOFs),such as CuCo-BTC(BTC=1,3,5-Benzenetricarboxylic acid,H_(3)BTC),CuNi-BTC,and CoNi-BTC,were synthesized by solvothermal(ST)and spray-drying(SD)methods,and then calcined at 400℃for 2 h to form metal oxides.The catalysts as well as their catalytic effects for AP decomposition were characterized by FTIR,XRD,SEM,XPS,TG,DSC,TG-IR,EIS,CV,and LSV.It was found that the rapid coordination of metal ions with ligands during spray drying may lead to catalytic structural defects,promoting the exposure of reactive active sites and increasing the catalytic active region.The results showed that the addition of 2 wt%binary transition metal oxides(BTMOs)as catalysts significantly reduced the high-temperature decomposition(HTD)temperature of AP and enhanced its heat release.Of particular significance is the observation that SD-CoNiO_(x),prepared by spray-drying,reduced the decomposition temperature of AP from 413.26℃(pure AP)to 306℃and enhanced the heat release from 256.79 J/g(pure AP)to 1496.82 J/g,while concomitantly reducing the activation energy by 42%.By analysing the gaseous products during the decomposition of AP+SD-CoNiO_(x)and AP+ST-CoNiO_(x),it was found that SD-CoNiO_(x)could significantly increase the content of high-valent nitrogen oxides during the AP decomposition reaction,which indicates that the BTMOs prepared by spray-drying in the reaction system are more conducive to accelerating the electron transfer in the thermal decomposition process of AP,and can provide a high concentration of reactive oxygen species that oxidize AP to high-valent nitrogen oxide-containing compounds.The present study shows that the structure selectivity of the spray-drying technique influences surfactant molecular arrangement on catalyst surfaces,resulting in their ability to promote higher electron transfer during the catalytic process.Therefore,BTMOs prepared by spray drying method have higher potential for application.
文摘The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based solids with oxides from alkali (Li2O), alkaline earth (CaO), and transition metal groups (WO3 or MnO). The presence of the peroxide (O2-2) active sites on the Li2O2, revealed by Raman spectroscopy, may be the key factor in the enhanced performance of some of the Li2O/MgO catalysts. The high reducibility of the CeO2 catalyst, an important factor in the CO2-OCM catalyst activity, may be enhanced by the presence of manganese oxide species. The manganese oxide species increases oxygen mobility and oxygen vacancies in the CeO2 catalyst. Raman and Fourier Transform Infra Red (FT-IR) spectroscopies revealed the presence of lattice vibrations of metal-oxygen bondings and active sites in which the peaks corresponding to the bulk crystalline structures of Li2O, CaO, WO3 and MnO are detected. The performance of 5%MnO/15%CaO/CeO2 catalyst is the most potential among the CeO2-based catalysts, although lower than the 2%Li2O/MgO catalyst. The 2%Li2O/MgO catalyst showed the most promising C2+ hydrocarbons selectivity and yield at 98.0% and 5.7%, respectively.
基金supported by the National Natural Science Foundation of China(Nos.51673117,51973118,and 21805193)the Science and Technology Innovation Commission of Shenzhen(Nos.JCYJ20170818093832350,JCYJ20170818112409808,JSGG20170824112840518,JCYJ20180507184711069,JCYJ20170818100112531,JCYJ20170817094628397,and JCYJ20180305125319991)+1 种基金the Key-Area Research and Development Program of Guangdong Province(Nos.2019B010929002 and 2019B010941001)the China Postdoctoral Science Foundation(No.2019M650212)。
文摘Because of the intensified electrochemical activities,mixed metal oxides as a representative for pseudocapacitive materials play a key role for high performance supercapacitor electrodes.Nevertheless,low ion and electron transfer rate and poor cycling performance in the electrode practically restrict further promotion of their electrochemical performance.In order to offset the defect,a novel copper(Cu)foamsupported nickel molybdate nanosheet decorated carbon nanotube wrapped copper oxide nanowire array(NiMoO4 NSs-CNTs-CuO NWAs/Cu foam)flexible electrode is constructed.The as-prepared electrode demonstrates a unique core-shell holey nanostructure with a large active surface area,which can provide a large number of active sites for redox reactions.Besides,the CNTs networks supply improved conductivity,which can hasten electron transport.Through this simple and efficient design method,the spatial distribution of each component in the flexible electrode is more orderly,short and fast electron transport path with low intrinsic resistance.As a result,the NiMoO4 NSs-CNTs-CuO NWAs/Cu foam as an adhesiveless supercapacitor electrode material exhibits excellent ene rgy storage perfo rmance with high specific areal capacitance of 23.40 F cm^(-2)at a current density of 2 mA cm^(-2),which outperforms most of the flexible electrodes re ported recently.The assembled asymmetric supercapacitor demonstrates an energy density up to 96.40 mW h cm^(-3)and a power density up to 0.4 W cm^(-3)under a working voltage window of 1.7 V.In addition,outstanding flexibility of up to 100°bend and good cycling stability with the capacitance retention of 82.53%after 10,000 cycles can be obtained.
