This review paper aims at analysing the state of the art for partial oxidation and oxidative dehydrogenation(ODH) reactions of lower alkanes C–Cinto olefins and oxygenated products(aldehydes, anhydrides,carboxylic...This review paper aims at analysing the state of the art for partial oxidation and oxidative dehydrogenation(ODH) reactions of lower alkanes C–Cinto olefins and oxygenated products(aldehydes, anhydrides,carboxylic acids) on metal oxide catalysts with cations of variable oxidation state, such as Mo and V in particular. Key parameters to be met by the catalysts, such as their redox properties, their structural aspects, active sites composed of ensembles of atoms isolated one from the others, mechanisms of reactions, are discussed. Main features of the different reactions of C–Calkanes and catalysts are analysed and their generalisation for determining more active and more selective catalysts is attempted. Prospective views for the future of the domain are proposed.展开更多
Labile organic carbon(LOC) is one of the most important indicators of soil organic matter quality and dynamics elevation and plays important function in the Tibetan Plateau climate. However, it is unknown what the s...Labile organic carbon(LOC) is one of the most important indicators of soil organic matter quality and dynamics elevation and plays important function in the Tibetan Plateau climate. However, it is unknown what the sources and causes of LOC contamination are. In this study, soil organic carbon(SOC), total nitrogen(TN), microbial biomass carbon(MBC), microbial biomass nitrogen(MBN) and LOC were analyzed based on different soil horizons and elevations using turnover time in an experimental site(3700 m to 4300 m area) in Sygera. SOC and LOC in higher-elevation vegetation types were higher than that of in lower-elevation vegetation types. Our results presented that the soil microbial biomass carbon(SMBC) and soil microbial biomass nitrogen(SMBN)were positively correlated with SOC. The content of easily oxidized carbon(EOC), particulate organic carbon(POC) and light fraction organic carbon(LFOC) decreased with depth increasing and the content were the lowest in the 60 cm to 100 cm depth.The total SOC, ROC and POC contents decreased with increasing soil horizons. The SOC, TN, MBC and MBN contents increased with increasing altitude in the Sygera Mountains. The MBC and MBN contents weredifferent with the changes of SOC(p<0.05),meanwhile, both LFOC and POC were related to total SOC(p<0.05). The physical and chemical properties of soil, including temperature, humidity, and altitude,were involved in the regulation of SOC, TN, MBC,MBN and LFOC contents in the Sygera Mountains,Tibetan Plateau.展开更多
The utilization of lighter alkanes into useful chemical products is essential for modern chemistry and reducing the CO_(2)emission.Particularly,n-butane has gained special attention across the globe due to the abundan...The utilization of lighter alkanes into useful chemical products is essential for modern chemistry and reducing the CO_(2)emission.Particularly,n-butane has gained special attention across the globe due to the abundant production of maleic anhydride(MA).Vanadium phosphorous oxide(VPO)is the most effective catalyst for selective oxidation of n-butane to MA so far.Interestingly,the VPO complex exists in more or less fifteen different structures,each one having distinct phase composition and exclusive surface morphology and physiochemical properties such as valence state,lattice oxygen,acidity etc.,which relies on precursor preparation method and the activation conditions of catalysts.The catalytic performance of VPO catalyst is improved by adding different promoters or co-catalyst such as various metals dopants,or either introducing template or structural-directing agents.Meanwhile,new preparation strategies such as electrospinning,ball milling,hydrothermal,barothermal,ultrasound,microwave irradiation,calcination,sol-gel method and solvothermal synthesis are also employed for introducing improvement in catalytic performance.Research in above-mentioned different aspects will be ascribed in current review in addition to summarizing overall catalysis activity and final yield.To analyze the performance of the catalytic precursor,the reaction mechanism and reaction kinetics both are discussed in this review to help clarify the key issues such as strong exothermic reaction,phosphorus supplement,water supplement,deactivation,and air/n-butane pretreatment etc.related to the various industrial applications of VPO.展开更多
Advanced oxidation technologies are a friendly environmental approach for the remediation of industrial wastewaters. Here, one pot synthesis of mesoporous WO3 and WO3-graphene oxide(GO) nanocomposites has been perfo...Advanced oxidation technologies are a friendly environmental approach for the remediation of industrial wastewaters. Here, one pot synthesis of mesoporous WO3 and WO3-graphene oxide(GO) nanocomposites has been performed through the sol–gel method. Then, platinum(Pt) nanoparticles were deposited onto the WO3 and WO3-GO nanocomposite through photochemical reduction to produce mesoporous Pt/WO3 and Pt/WO3-GO nanocomposites. X-ray diffraction(XRD) findings exhibit a formation of monoclinic and triclinic WO3 phases. Transmission Electron Microscope(TEM) images of Pt/WO3-GO nanocomposites exhibited that WO3 nanoparticles are obviously agglomerated and the particle sizes of Pt and WO3 are ~ 10 nm and 20–50 nm, respectively. The mesoporous Pt/WO3 and Pt/WO3-GO nanocomposites were assessed for photocatalytic degradation of Methylene Blue(MB) as a probe molecule under visible light illumination.The findings showed that mesoporous Pt/WO3, WO3-GO and Pt/WO3-GO nanocomposites exhibited much higher photocatalytic efficiencies than the pure WO3. The photodegradation rates by mesoporous Pt/WO3-GO nanocomposites are 3, 2 and 1.15 times greater than those by mesoporous WO3, WO3-GO, and Pt/WO3, respectively. The key factors of the enhanced photocatalytic performance of Pt/WO3-GO nanocomposites could be explained by the highly freedom electron transfer through the synergetic effect between WO3 and GO sheets, in addition to the Pt nanoparticles that act as active sites for O2 reduction, which suppresses the electron hole pair recombination in the Pt/WO3-GO nanocomposites.展开更多
The present work aims to investigate the recovery of light rare earth elements(LREEs) oxides from end-oflife NiMH batteries using a hydro metallurgical process followed by effective precipitation.The operational leach...The present work aims to investigate the recovery of light rare earth elements(LREEs) oxides from end-oflife NiMH batteries using a hydro metallurgical process followed by effective precipitation.The operational leaching parameters such as phosphoric acid concentration,temperature,and the solid-liquid ratio were first optimized by Box-Behnken design.The results reveal that under optimum conditions([H_(3)PO_(4)]=2 mol/L,T=80℃,and S/L=1:10 g/mL) the leaching efficiencies of Ni,Co reach 98.1% and99.3%.While La,Ce,and Nd elements remain in the leaching residue as(La,Ce,Nd)PO_(4) with yields of 98.2%,98.6%,and 99.6% for La,Ce,and Nd,respectively.Afterward,the(La,Ce,Nd)PO_(4) is leached with HCl acid,then the rare earth oxalate was precipitated using oxalic acid at a pH of 1.8 and then the product was calcined at 800℃ for 2 h in order to synthesize the(Nd,La,Ce)_(2)O_(3).The analysis using scanning electron microscopy(SEM) coupled with energy dispersive X-ray spectroscopy(EDX) confirms the homogeneity of(Nd,La,Ce)_(2)O_(3) particles that have two morphologies,i.e.,flower and sticks with a particle size between 3and 6 μm.The unit cell parameters of(Nd,La,Ce)_(2)O_(3) were calculated after Rietveld refinement of the XRD patterns,in the space group of Fm-3m are a=b=c=0.57921 nm and the volume equal to 0.194322 nm^(3).展开更多
One of the core issues in the photocatalytic oxidation of nitric oxide is the effective co nversion of NO into the final product(nitrate).More than just improving the visible light photocatalytic performance of BiOCl,...One of the core issues in the photocatalytic oxidation of nitric oxide is the effective co nversion of NO into the final product(nitrate).More than just improving the visible light photocatalytic performance of BiOCl,we aim to inhibit the generation of toxic by-product NO_(2) during this process.In this study,we demonstrate that the oxygen vacancies(OVs)modulate its surface photogene rated carrier transfer to inflect the NO conversion pathway by a facile mixed solvent method to induce OVs on the surface of BiOCl.The photocatalytic NO removal efficiency under visible light increased from 5.6%to 36.4%.In addition,the production rate of NO_(2) is effectively controlled.The effects of OVs on the generation of reactive oxygen species,electronic transfer,optical properties,and photocatalytic NO oxidation are investigated by combining density functional theory(DFT)theoretical calculations,the in situ FTIR spectra and experimental characterization.The OVs on the surface of BiOCl speed the trapping and transfer of localized electrons to activate the O_(2),producing O_(2)·,which avoid NO_(2) formation,resulting in complete oxidation of NO(NO+O_(2)·→NO_(3)).These findings can serve as the basis for controlling and blocking the generation of highly toxic intermediates through regulating the reactive species during the NO oxidation.It also can help us to understand the role of OV on the BiOCl surface and application of photocatalytic technology for safe air purification.展开更多
文摘This review paper aims at analysing the state of the art for partial oxidation and oxidative dehydrogenation(ODH) reactions of lower alkanes C–Cinto olefins and oxygenated products(aldehydes, anhydrides,carboxylic acids) on metal oxide catalysts with cations of variable oxidation state, such as Mo and V in particular. Key parameters to be met by the catalysts, such as their redox properties, their structural aspects, active sites composed of ensembles of atoms isolated one from the others, mechanisms of reactions, are discussed. Main features of the different reactions of C–Calkanes and catalysts are analysed and their generalisation for determining more active and more selective catalysts is attempted. Prospective views for the future of the domain are proposed.
基金supported by CFERN & GENE Award Funds on Ecological Paper
文摘Labile organic carbon(LOC) is one of the most important indicators of soil organic matter quality and dynamics elevation and plays important function in the Tibetan Plateau climate. However, it is unknown what the sources and causes of LOC contamination are. In this study, soil organic carbon(SOC), total nitrogen(TN), microbial biomass carbon(MBC), microbial biomass nitrogen(MBN) and LOC were analyzed based on different soil horizons and elevations using turnover time in an experimental site(3700 m to 4300 m area) in Sygera. SOC and LOC in higher-elevation vegetation types were higher than that of in lower-elevation vegetation types. Our results presented that the soil microbial biomass carbon(SMBC) and soil microbial biomass nitrogen(SMBN)were positively correlated with SOC. The content of easily oxidized carbon(EOC), particulate organic carbon(POC) and light fraction organic carbon(LFOC) decreased with depth increasing and the content were the lowest in the 60 cm to 100 cm depth.The total SOC, ROC and POC contents decreased with increasing soil horizons. The SOC, TN, MBC and MBN contents increased with increasing altitude in the Sygera Mountains. The MBC and MBN contents weredifferent with the changes of SOC(p<0.05),meanwhile, both LFOC and POC were related to total SOC(p<0.05). The physical and chemical properties of soil, including temperature, humidity, and altitude,were involved in the regulation of SOC, TN, MBC,MBN and LFOC contents in the Sygera Mountains,Tibetan Plateau.
基金supported by the National Key Research and Development Program of China(2017YFA0206803)the innovation Academy for Green Manufacture of Chinese Academy of Science(IAGM2020C17)+3 种基金the Key Programs of the Chinese Academy of Sciences(KFZD-SW-413)the National Nature Science Foundation of China(21808223)the Key Programs of Fujian Institute of Innovation,CAS(FJCXY18020203)Chinese Academy of Sciences,the One Hundred Talent Program of CAS。
文摘The utilization of lighter alkanes into useful chemical products is essential for modern chemistry and reducing the CO_(2)emission.Particularly,n-butane has gained special attention across the globe due to the abundant production of maleic anhydride(MA).Vanadium phosphorous oxide(VPO)is the most effective catalyst for selective oxidation of n-butane to MA so far.Interestingly,the VPO complex exists in more or less fifteen different structures,each one having distinct phase composition and exclusive surface morphology and physiochemical properties such as valence state,lattice oxygen,acidity etc.,which relies on precursor preparation method and the activation conditions of catalysts.The catalytic performance of VPO catalyst is improved by adding different promoters or co-catalyst such as various metals dopants,or either introducing template or structural-directing agents.Meanwhile,new preparation strategies such as electrospinning,ball milling,hydrothermal,barothermal,ultrasound,microwave irradiation,calcination,sol-gel method and solvothermal synthesis are also employed for introducing improvement in catalytic performance.Research in above-mentioned different aspects will be ascribed in current review in addition to summarizing overall catalysis activity and final yield.To analyze the performance of the catalytic precursor,the reaction mechanism and reaction kinetics both are discussed in this review to help clarify the key issues such as strong exothermic reaction,phosphorus supplement,water supplement,deactivation,and air/n-butane pretreatment etc.related to the various industrial applications of VPO.
文摘Advanced oxidation technologies are a friendly environmental approach for the remediation of industrial wastewaters. Here, one pot synthesis of mesoporous WO3 and WO3-graphene oxide(GO) nanocomposites has been performed through the sol–gel method. Then, platinum(Pt) nanoparticles were deposited onto the WO3 and WO3-GO nanocomposite through photochemical reduction to produce mesoporous Pt/WO3 and Pt/WO3-GO nanocomposites. X-ray diffraction(XRD) findings exhibit a formation of monoclinic and triclinic WO3 phases. Transmission Electron Microscope(TEM) images of Pt/WO3-GO nanocomposites exhibited that WO3 nanoparticles are obviously agglomerated and the particle sizes of Pt and WO3 are ~ 10 nm and 20–50 nm, respectively. The mesoporous Pt/WO3 and Pt/WO3-GO nanocomposites were assessed for photocatalytic degradation of Methylene Blue(MB) as a probe molecule under visible light illumination.The findings showed that mesoporous Pt/WO3, WO3-GO and Pt/WO3-GO nanocomposites exhibited much higher photocatalytic efficiencies than the pure WO3. The photodegradation rates by mesoporous Pt/WO3-GO nanocomposites are 3, 2 and 1.15 times greater than those by mesoporous WO3, WO3-GO, and Pt/WO3, respectively. The key factors of the enhanced photocatalytic performance of Pt/WO3-GO nanocomposites could be explained by the highly freedom electron transfer through the synergetic effect between WO3 and GO sheets, in addition to the Pt nanoparticles that act as active sites for O2 reduction, which suppresses the electron hole pair recombination in the Pt/WO3-GO nanocomposites.
文摘The present work aims to investigate the recovery of light rare earth elements(LREEs) oxides from end-oflife NiMH batteries using a hydro metallurgical process followed by effective precipitation.The operational leaching parameters such as phosphoric acid concentration,temperature,and the solid-liquid ratio were first optimized by Box-Behnken design.The results reveal that under optimum conditions([H_(3)PO_(4)]=2 mol/L,T=80℃,and S/L=1:10 g/mL) the leaching efficiencies of Ni,Co reach 98.1% and99.3%.While La,Ce,and Nd elements remain in the leaching residue as(La,Ce,Nd)PO_(4) with yields of 98.2%,98.6%,and 99.6% for La,Ce,and Nd,respectively.Afterward,the(La,Ce,Nd)PO_(4) is leached with HCl acid,then the rare earth oxalate was precipitated using oxalic acid at a pH of 1.8 and then the product was calcined at 800℃ for 2 h in order to synthesize the(Nd,La,Ce)_(2)O_(3).The analysis using scanning electron microscopy(SEM) coupled with energy dispersive X-ray spectroscopy(EDX) confirms the homogeneity of(Nd,La,Ce)_(2)O_(3) particles that have two morphologies,i.e.,flower and sticks with a particle size between 3and 6 μm.The unit cell parameters of(Nd,La,Ce)_(2)O_(3) were calculated after Rietveld refinement of the XRD patterns,in the space group of Fm-3m are a=b=c=0.57921 nm and the volume equal to 0.194322 nm^(3).
基金the National Natural Science Foundation of China(Nos.21822601,21777011 and 21501016)the Plan for"National Youth Talents"of the Organization Department of the Central Committee。
文摘One of the core issues in the photocatalytic oxidation of nitric oxide is the effective co nversion of NO into the final product(nitrate).More than just improving the visible light photocatalytic performance of BiOCl,we aim to inhibit the generation of toxic by-product NO_(2) during this process.In this study,we demonstrate that the oxygen vacancies(OVs)modulate its surface photogene rated carrier transfer to inflect the NO conversion pathway by a facile mixed solvent method to induce OVs on the surface of BiOCl.The photocatalytic NO removal efficiency under visible light increased from 5.6%to 36.4%.In addition,the production rate of NO_(2) is effectively controlled.The effects of OVs on the generation of reactive oxygen species,electronic transfer,optical properties,and photocatalytic NO oxidation are investigated by combining density functional theory(DFT)theoretical calculations,the in situ FTIR spectra and experimental characterization.The OVs on the surface of BiOCl speed the trapping and transfer of localized electrons to activate the O_(2),producing O_(2)·,which avoid NO_(2) formation,resulting in complete oxidation of NO(NO+O_(2)·→NO_(3)).These findings can serve as the basis for controlling and blocking the generation of highly toxic intermediates through regulating the reactive species during the NO oxidation.It also can help us to understand the role of OV on the BiOCl surface and application of photocatalytic technology for safe air purification.