The effect of Na-excess content in the precursor on the structural and electrochemical performances of sodium nickel manganese oxide(NNMO)prepared by sol-gel and electrospinning methods is investigated in this paper.X...The effect of Na-excess content in the precursor on the structural and electrochemical performances of sodium nickel manganese oxide(NNMO)prepared by sol-gel and electrospinning methods is investigated in this paper.X-ray diffraction results of the prepared NNMO without adding Na-excess content indicate sodium loss,while the mixed phase of P2/O′3-type layered NNMO presented after adding Na-excess content.Compared with the sol-gel method,the secondary phase of NiO is more suppressed by using the electrospinning method,which is further confirmed by field emission scanning electron microscope images.N_(2) adsorption-desorption isotherms show no remarkably difference in specific surface areas between different preparation methods and Na-excess contents.The analysis of X-ray absorption near edge structure indicates that the oxidation states of Ni and Mn are+2 and+4,respectively.For the electrochemical properties,superior electrochemical performance is observed in the NNMO electrode with a low Na-excess content of 5wt%.The highest specific capacitance is 36.07 F·g^(-1)at0.1 A·g^(-1)in the NNMO electrode prepared by using the sol-gel method.By contrast,the NNMO electrode prepared using the electrospinning method with decreased Na-excess content shows excellent cycling stability of 100%after charge-discharge measurements for 300 cycles.Therefore,controlling the Na excess in the precursor together with the preparation method is important for improving the electrochemical performance of Na-based electrode materials in supercapacitors.展开更多
The layered Li[Ni1/3Mn1/3Co1/3]O2 was separately synthesized by pretreatment process of ball mill method and solution phase route, using [Ni1/3Co1/3Mn1/3]3O4 and lithium hydroxide as raw materials. The physical and el...The layered Li[Ni1/3Mn1/3Co1/3]O2 was separately synthesized by pretreatment process of ball mill method and solution phase route, using [Ni1/3Co1/3Mn1/3]3O4 and lithium hydroxide as raw materials. The physical and electrochemical behaviors of Li[Ni1/3Mn1/3Co1/3]O2 were characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM）, field emission scanning electron microscopy （FESEM） and electrochemical charge/discharge cycling tests. The results show that the difference in pretreatment process results in the difference in compound Li[Ni1/3Co1/3Mn1/3]O2 structure, morphology and the electrochemical characteristics. The Li[Ni1/3Mn1/3Co1/3]O2 prepared by solution phase route maintains the uniform spherical morphology of the [Ni1/3Co1/3Mn1/3]3O4, and it exhibits a higher capacity retention and better rate capability than that prepared by ball mill method. The initial discharge capacity of this sample reaches 178 mA-h/g and the capacity retention after 50 cycles is 98.7% at a current density of 20 mA/g. Moreover, it delivers high discharge capacity of 135 mA-h/g at a current density of 1 000 mA/g.展开更多
A microwave-H202 process for sludge pretreatment exhibited high efticiencies of releasing organics, nitrogen, and phosphorus, but large quantifies of H202 residues were detected. A uniform design method was thus emplo...A microwave-H202 process for sludge pretreatment exhibited high efticiencies of releasing organics, nitrogen, and phosphorus, but large quantifies of H202 residues were detected. A uniform design method was thus employed in this study to further optimize H202 dosage by investigating effects of pH and H202 dosage on the amount of 1-I202 residue and releases of organics, nitrogen, and phosphorus. A regression model was established with pH and H202 dosage as the independent variables, and H202 residue and releases of organics, nitrogen, and phosphorus as the dependent variables. In the optimized microwave-H202 process, the pH value of the sludge was firstly adjusted to 11.0, then the sludge was heated to 80~C and H202 was dosed at a H202 ：mixed liquor suspended solids （MLSS） ratio of 0.2, and the sludge was finally heated to 100~C by microwave irradiation. Compared to the microwave-H202 process without optimization, the H202 dosage and the utilization rate of H202 in the optimized microwave-H202 process were reduced by 80% and greatly improved by 3.87 times, respectively, when the H202：MLSS dosage ratio was decreased from 1.0 to 0.2, resulting in nearly the same release rate of soluble chemical oxygen demand in the microwave-H202 process without optimization at H202：MLSS ratio of 0.5.展开更多
Europium orthophosphate monohydrate （EuPO4·H2O） nanorods with typical dimensions of about 10-30 nm in diameter and 300-500 nm in length were prepared by using the soft template method. The effects of using diet...Europium orthophosphate monohydrate （EuPO4·H2O） nanorods with typical dimensions of about 10-30 nm in diameter and 300-500 nm in length were prepared by using the soft template method. The effects of using diethylene glycol （DEG） and polyethylene glycol （PEG） polymers as well as the pH values on the size, crystalline structure and morphology of EuPO4·H2O nanorods were investigated. Field emission scanning electron microscopy （FESEM） and X-ray diffraction （XRD） data of the prepared samples were elucidated. The nanorods were highly uniform and their mean length was reduced by using DEG and PEG as soft template agents. For all prepared samples, the rhabdophanetype hexagonal EuPO4·H2O was the dominated phase. The photoluminescence （PL） spectroscopy measurements of EuPO4·H2O nanorods revealed that, under UV excitation, EuPO4·H2O nanorods exhibited strong luminescence with narrow bands corresponding to the intra-4f transitions of ^5D0→^7Fj （j=1, 2, 3, 4） of Eu^3＋ ions. The peaks were found at 594 nm （^5D0→^7F1）, 619 nm （^5D0→^7F2）, 652 nm （^5D0→^7F3）, and 697 nm （^5D0→^7F4）, with the strongest emission at 594 nm.展开更多
Niobium doped Zincoxide nanoparticles has been synthesized through electrochemical method and characterized by UV-Visible spectroscopy, IR Spectroscopy, SEM, XRD, ICPMS and EDAX data. The UV-Visible spectroscopy resul...Niobium doped Zincoxide nanoparticles has been synthesized through electrochemical method and characterized by UV-Visible spectroscopy, IR Spectroscopy, SEM, XRD, ICPMS and EDAX data. The UV-Visible spectroscopy result reveals that the band gap energy of ZnO/Nb2O5 nanoparticles to be 3.8 eV. The XRD results show that the crystallite size is to be 31.9 nm. The ICPMS data indicate the presence of 3,3461,328 counts of 93 Nb and 577,906,390 counts of 66 Zn. An improvement in the photocatalytic degradation of Indigocarmine dye (IC) in comparison to commercially available pure ZnO was observed. The photodegradation efficiency for ZnO/Nb2O5 and ZnO were found to be 97.4% and 52.1% respectively. The enhancement in photocatalytic activity of ZnO/ Nb2O5 was ascribed to the extended light absorption range and suppression of electron hole pair recombination upon Nb loading. The antibacterial activity of ZnO/Nb2O5 nanoparticles was investigated. These particles were shown to have an effective bactericide.展开更多
The ordered bimodal mesoporous silica MCM-48 spheres were facile synthesized by mild- temperature post-synthesis H2O2 hydrothermal treatment of as-synthesized MCM-48. The results showed that H2O2 is indispensable for ...The ordered bimodal mesoporous silica MCM-48 spheres were facile synthesized by mild- temperature post-synthesis H2O2 hydrothermal treatment of as-synthesized MCM-48. The results showed that H2O2 is indispensable for simultaneously removing organic templates and forming ordered bimodal mesoporous silica MCM-48 spheres. The bimodal mesoporous MCM-48 was characterized by X-ray diffraction, transmission electron micrographs, FT-IR, and N2 adsorption-desorption, and a possible mechanism was proposed for the formation of bimodal mesoporous MCM-48.展开更多
The oxysulfide La3NbS2O5 was synthesized by sulfurization using H2S and characterized by X-ray diffraction （XRD）, UV-Vis diffuse reflectance spectroscopy （DRS） and field emission scanning electron microscopy （FE-...The oxysulfide La3NbS2O5 was synthesized by sulfurization using H2S and characterized by X-ray diffraction （XRD）, UV-Vis diffuse reflectance spectroscopy （DRS） and field emission scanning electron microscopy （FE-SEM）. The relationship between the sulfurization conditions and the photocatalytic activities for H2 evolution was investigated. Sulfurization method allowed for synthesis of La3NbS2O5 at much lower temperatures and significantly shortened reaction time of 1 h compared with conventional solid-state techniques. The particle morphologies were regular platelike with sizes of 0.1-0.6μm and smooth surfaces. The highest activity for H2 evolution was obtained at 1073 K for 1 h, which was about 1.83 times that of La3NbS2O5 prepared by solid-state method.展开更多
The controllable synthesis of tantalate K1.9Na0.1Ta2O6·2H2O has been successfully achieved by a two-step technique,namely,the molten salt and hydrothermal methods,at a low temperature. By simply varying the KOH c...The controllable synthesis of tantalate K1.9Na0.1Ta2O6·2H2O has been successfully achieved by a two-step technique,namely,the molten salt and hydrothermal methods,at a low temperature. By simply varying the KOH concentration in the hydrothermal process,K1.9Na0.1Ta2O6·2H2O particles with spherical,cuboctahedral,and durian-like morphologies were synthesized. The photocatalytic activity of the obtained samples for the degradation of rhodamine B was studied under ultraviolet light,which indicates that the photocatalytic properties of the samples are highly dependent on their morphologies. The K1.9Na0.1Ta2O6·2H2O nanospheres,with rough surfaces and the highest specific surface area,exhibit the best performance. The present work provides a unique approach for the controlled synthesis of tantalate photocatalysts,which are difficult to achieve through other synthetic approaches.展开更多
Vapor phase catalytic hydrogen peroxide production by oxidation of water is possible by coupling the reaction with oxidation of an organic sacrificial reductant. It is potentially a safer process than direct synthesis...Vapor phase catalytic hydrogen peroxide production by oxidation of water is possible by coupling the reaction with oxidation of an organic sacrificial reductant. It is potentially a safer process than direct synthesis from H2 and O2. Based on mechanistic information available mostly for liquid phase catalytic processes, feasible reaction mechanisms for such coupled reactions are proposed based on which desirable catalyst properties are identified. It is found that the surface-adsorbed oxygen bond is an important parameter for identifying desirable catalysts. Thermodynamics can be used to identify the types of organic oxidation reactions that can couple with water oxidation such that H2O2 formation becomes thermodynamically favorable. Reactions such as epoxidation of alkenes and selective oxidation of alkanes to alcohols cannot provide sufficient thermodynamic driving force, whereas oxidation of alcohols to aldehydes and to acids can. Finally, further research is suggested to identify catalytic properties important for H2O2 decomposition and for coupling selective oxidation of organic compounds to oxidation of H2O in order to facilitate development of H2O2 production coupled with selective organic oxidation.展开更多
A series of Ce, H3PW12O40 co-doped TiO2 hollow fibers photocatalysts have been prepared by sol-gel method using ammonium ceric nitrate, H3PW12O40 and tetrabutyltitanate as precursors and cotton fibers as template, fol...A series of Ce, H3PW12O40 co-doped TiO2 hollow fibers photocatalysts have been prepared by sol-gel method using ammonium ceric nitrate, H3PW12O40 and tetrabutyltitanate as precursors and cotton fibers as template, followed by calcination at 500 ℃ in N2 atmosphere for 2 h. Scanning electron microscopy, X-ray diffraction, nitrogen adsorption-desorption mea- surements, and UV-Vis spectroscopy are employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The photo- catalytic performance of the samples has been studied by photodegradation phenol in water under UV and visible light irradiation. The results show that the TiO2 fiber materials have hollow structures, and the co-doped TiO2 hollow fibers exhibit higher photocatalytic activities for the degradation of phenol than un-doped, single-doped TiO2 hollow fibers under UV and visible light. In addition, the recyclability of co-doped TiO2 fibers is also confirmed that the TiO2 fiber retains ca. 90% of its activity after being used four times. It is shown that the co-doped TiO2 fibers can be activated by visible light and may be potentially applied to the treatment of water contaminated by organic pollutants. The synergistic effect of Ce and H3PW12O40 co-doping plays an important role in improving the photocatalytic activity.展开更多
Electrosynthesis of hydrogen peroxide(H2O2)is an on-site method that enables independent distribution applications in many fields due to its small-scale and sustainable features.The crucial point remains developing hi...Electrosynthesis of hydrogen peroxide(H2O2)is an on-site method that enables independent distribution applications in many fields due to its small-scale and sustainable features.The crucial point remains developing highly active,selective and cost-effective electrocatalysts.The electrosynthesis of H2O2 in acidic media is more practical owing to its stability and no need for further purification.We herein report a phosphorus and selenium tuning Co-based non-precious catalyst(CoPSe)toward two-electron oxygen reduction reaction(2e–ORR)to produce H2O2 in acidic media.The starting point of using both P and Se is finding a balance between strong ORR activity of CoSe and weak activity of CoP.The results demonstrated that the CoPSe catalyst exhibited the optimized 2e–ORR activity compared with CoP and CoSe.It disclosed an onset potential of 0.68 V and the H2O2 selectivity 76%-85%in a wide potential range(0–0.5 V).Notably,the CoPSe catalyst overcomes a significant challenge of a narrow-range selectivity for transitionmetal based 2e–ORR catalysts.Finally,combining with electro-Fenton reaction,an on-site system was constructed for efficient degradation of organic pollutants.This work provides a promising non-precious Co-based electrocatalyst for the electrosynthesis of H2O2 in acidic media.展开更多
Non-enzymatic biosensors based on mixed transition metal oxides are deemed as the most promising devices due to their high sensitivity,selectivity,wide concentration range,low detection limits,and excellent recyclabil...Non-enzymatic biosensors based on mixed transition metal oxides are deemed as the most promising devices due to their high sensitivity,selectivity,wide concentration range,low detection limits,and excellent recyclability.Spinel NiCo2O4 mixed oxides have drawn considerable attention recently due to their outstanding advantages including large specific surface area,high permeability,short electron,and ion diffusion pathways.Because of the rapid development of non-enzyme biosensors,the current state of methods for synthesis of pure and composite/hybrid NiCo2P4 materials and their subsequent electrochemical biosensing applications are systematically and comprehensively reviewed herein.Comparative analysis reveals better electrochemical sensing of bioanalytes by one-dimensional and two-dimensional NiCo2O4 nano-/microstructures than other morphologies.Better biosensing efficiency of NiCo2O4 as compared to corresponding individual metal oxides,viz.NiO and Co3O4,is attributed to the close intrinsic-state redox couples of Ni3+/Ni2+(0.58 V/0.49 V) and Co3+/Co2+(0.53 V/0.51 V).Biosensing performance of NiCo2O4 is also significantly improved by making the composites of NiCo2O4 with conducting carbonaceous materials like graphene,reduced graphene oxide,carbon nanotubes(single and multi-walled),carbon nanofibers;conducting polymers like polypyrrole(PPy),polyaniline(PANI);metal oxides NiO,Co3O4,SnO2,MnO2;and metals like Au,Pd,etc.Various factors affecting the morphologies and biosensing parameters of the nano-/microstructured NiCo2O4 are also highlighted.Finally,some drawbacks and future perspectives related to this promising field are outlined.展开更多
LiCoO2 surface layer is proposed and prepared through sol-gel method. The physical and electrochemical performances of pristine LiMn2O4 and LiCoO2-coated LiMn2O4 cathode materials were investigated by X-ray diffractio...LiCoO2 surface layer is proposed and prepared through sol-gel method. The physical and electrochemical performances of pristine LiMn2O4 and LiCoO2-coated LiMn2O4 cathode materials were investigated by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, electrochemical measurements respectively. Comparing with the pristine LiMn2O4, the LiCoO2- coated LiMn2O4 phase significantly improved cycling stability, especially at 55°C. Additionally, the thermal safety of LiMn2O4 is greatly enhanced after being coated by LiCoO2. ICP-AES measurement, structural analysis, and impedance experiments indicate that the improved electrochemical property of LiCoO2-coated LiMn2O4 should be attributed to the alleviated dissolution loss of manganese, strengthened structural stability.展开更多
A globally accurate potential energy surface is reported for the electronic ground-state H2O＋. The ab initio energies utilized to map the potential energy surface are calculated at the multireference configuration in...A globally accurate potential energy surface is reported for the electronic ground-state H2O＋. The ab initio energies utilized to map the potential energy surface are calculated at the multireference configuration interaction method employing the aug-cc-pVQZ basis set and the full valence complete active space wave function as reference. In order to improve accu- racy of the resulting raw ab initio energies, they are then extrapolated to the complete basis set limit and most importantly to the full configuration-interaction limit by semiempirically correcting the dynamical correlation using the double many- body expansion-scaled external correlation method. The topographical features of the current potential energy surface were examined in detail, which agree nicely with those of other theoretical work.展开更多
Quasi-classical trajectory theory is used to study the reaction of O（3p） with H2 （D2） based on the ground 3A″ potential energy surface （PES）. The reaction cross section of the reaction O＋H2→＋OH＋H is in exce...Quasi-classical trajectory theory is used to study the reaction of O（3p） with H2 （D2） based on the ground 3A″ potential energy surface （PES）. The reaction cross section of the reaction O＋H2→＋OH＋H is in excellent agreement with the previous result. Vector correlations, product rotational alignment parameters （P2（j′. k）） and several polarizeddependent differential cross sections are further calculated for the reaction. The product polarization distribution exhibits different characteristics that can be ascribed to different motion paths on the PES, arising from various collision energies or mass factors.展开更多
The development of a highly efficient and durable electrocatalyst for nitrate reduction reaction(NO_(3)RR)wastewater valorization to ammonia(NH_(3))is a promising strategy.However,it is challenging to design scalable ...The development of a highly efficient and durable electrocatalyst for nitrate reduction reaction(NO_(3)RR)wastewater valorization to ammonia(NH_(3))is a promising strategy.However,it is challenging to design scalable low-cost electrocatalysts with high activity,high selectivity,and long-term stability by a facile and simple method.Herein,we construct this scalable Cu-based nanoarray with muti-oxidation states grown directly on nickel foam(NF)substrate(Cu_(2+1)O@Cu/NF)using a facile molten salt method combined in-situ electrochemical reduction.The as-prepared Cu_(2+1)O@Cu/NF nanoarrays reveal a high NH_(3) yield of 20.14 mg h^(−1) cm^(−2) at−0.95 V vs.a reversible hydrogen electrode(vs.RHE),Faradaic efficiency of 99.38%at−0.55 V vs.RHE in the neutral potassium phosphate(PBS)buffer solution with 50 mM NaNO_(3),which is ascribed to its electron redistribution with abundant oxygen vacancies and favorable charge/mass transfer.展开更多
To enhance the electrochemical performances of LiMn2O4 at elevated temperature (55°C), we proposed a sol-gel method to synthesize LiNi0.5Mn1.5O4 modified LiMn2O4. The physical and electrochemical performances of ...To enhance the electrochemical performances of LiMn2O4 at elevated temperature (55°C), we proposed a sol-gel method to synthesize LiNi0.5Mn1.5O4 modified LiMn2O4. The physical and electrochemical performances of pristine and LiNi0.5Mn1.5O4-coated LiMn2O4 cathode materials were investigated by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy and electrochemical measurements, respectively. The results indicated that about 4-5 nm thick layer of LiNi0.5Mn1.5O4 was formed on the surface of the LiMn2O4 powders. The modified LiMn2O4 exhibited excellent storage performance at 55°C compared to the pristine one, which was attributed to the suppression of electrolyte decomposition and the reduction of Mn dissolution.展开更多
基金financially supported by (i) Suranaree University of Technology,(ii) Thailand Science Research and Innovation,and (iii) National Science,Research and Innovation Fund(project codes 90464 and 160363)。
文摘The effect of Na-excess content in the precursor on the structural and electrochemical performances of sodium nickel manganese oxide(NNMO)prepared by sol-gel and electrospinning methods is investigated in this paper.X-ray diffraction results of the prepared NNMO without adding Na-excess content indicate sodium loss,while the mixed phase of P2/O′3-type layered NNMO presented after adding Na-excess content.Compared with the sol-gel method,the secondary phase of NiO is more suppressed by using the electrospinning method,which is further confirmed by field emission scanning electron microscope images.N_(2) adsorption-desorption isotherms show no remarkably difference in specific surface areas between different preparation methods and Na-excess contents.The analysis of X-ray absorption near edge structure indicates that the oxidation states of Ni and Mn are+2 and+4,respectively.For the electrochemical properties,superior electrochemical performance is observed in the NNMO electrode with a low Na-excess content of 5wt%.The highest specific capacitance is 36.07 F·g^(-1)at0.1 A·g^(-1)in the NNMO electrode prepared by using the sol-gel method.By contrast,the NNMO electrode prepared using the electrospinning method with decreased Na-excess content shows excellent cycling stability of 100%after charge-discharge measurements for 300 cycles.Therefore,controlling the Na excess in the precursor together with the preparation method is important for improving the electrochemical performance of Na-based electrode materials in supercapacitors.
基金Project(20871101)supported by the National Natural Science Foundation of ChinaProject(2009WK2007)supported by Key Project of Science and Technology Department of Hunan Province,ChinaProject(CX2009B133)supported by Colleges and Universities in Hunan Province Plans to Graduate Research and Innovation,China
文摘The layered Li[Ni1/3Mn1/3Co1/3]O2 was separately synthesized by pretreatment process of ball mill method and solution phase route, using [Ni1/3Co1/3Mn1/3]3O4 and lithium hydroxide as raw materials. The physical and electrochemical behaviors of Li[Ni1/3Mn1/3Co1/3]O2 were characterized by X-ray diffraction （XRD）, scanning electron microscopy （SEM）, field emission scanning electron microscopy （FESEM） and electrochemical charge/discharge cycling tests. The results show that the difference in pretreatment process results in the difference in compound Li[Ni1/3Co1/3Mn1/3]O2 structure, morphology and the electrochemical characteristics. The Li[Ni1/3Mn1/3Co1/3]O2 prepared by solution phase route maintains the uniform spherical morphology of the [Ni1/3Co1/3Mn1/3]3O4, and it exhibits a higher capacity retention and better rate capability than that prepared by ball mill method. The initial discharge capacity of this sample reaches 178 mA-h/g and the capacity retention after 50 cycles is 98.7% at a current density of 20 mA/g. Moreover, it delivers high discharge capacity of 135 mA-h/g at a current density of 1 000 mA/g.
基金supported by the National Natural Science Foundation of China (No. 51008297)the Hi-Tech Research and Development Program (863) of China(No. 2007AA06Z347)the National Major Science & Technology Projects for Water Pollution Control and Management (No. 2012ZX07202-005)
文摘A microwave-H202 process for sludge pretreatment exhibited high efticiencies of releasing organics, nitrogen, and phosphorus, but large quantifies of H202 residues were detected. A uniform design method was thus employed in this study to further optimize H202 dosage by investigating effects of pH and H202 dosage on the amount of 1-I202 residue and releases of organics, nitrogen, and phosphorus. A regression model was established with pH and H202 dosage as the independent variables, and H202 residue and releases of organics, nitrogen, and phosphorus as the dependent variables. In the optimized microwave-H202 process, the pH value of the sludge was firstly adjusted to 11.0, then the sludge was heated to 80~C and H202 was dosed at a H202 ：mixed liquor suspended solids （MLSS） ratio of 0.2, and the sludge was finally heated to 100~C by microwave irradiation. Compared to the microwave-H202 process without optimization, the H202 dosage and the utilization rate of H202 in the optimized microwave-H202 process were reduced by 80% and greatly improved by 3.87 times, respectively, when the H202：MLSS dosage ratio was decreased from 1.0 to 0.2, resulting in nearly the same release rate of soluble chemical oxygen demand in the microwave-H202 process without optimization at H202：MLSS ratio of 0.5.
基金Project supported by Vietnam's National Foundation for Science and Technology Development (103.06.46.09)
文摘Europium orthophosphate monohydrate （EuPO4·H2O） nanorods with typical dimensions of about 10-30 nm in diameter and 300-500 nm in length were prepared by using the soft template method. The effects of using diethylene glycol （DEG） and polyethylene glycol （PEG） polymers as well as the pH values on the size, crystalline structure and morphology of EuPO4·H2O nanorods were investigated. Field emission scanning electron microscopy （FESEM） and X-ray diffraction （XRD） data of the prepared samples were elucidated. The nanorods were highly uniform and their mean length was reduced by using DEG and PEG as soft template agents. For all prepared samples, the rhabdophanetype hexagonal EuPO4·H2O was the dominated phase. The photoluminescence （PL） spectroscopy measurements of EuPO4·H2O nanorods revealed that, under UV excitation, EuPO4·H2O nanorods exhibited strong luminescence with narrow bands corresponding to the intra-4f transitions of ^5D0→^7Fj （j=1, 2, 3, 4） of Eu^3＋ ions. The peaks were found at 594 nm （^5D0→^7F1）, 619 nm （^5D0→^7F2）, 652 nm （^5D0→^7F3）, and 697 nm （^5D0→^7F4）, with the strongest emission at 594 nm.
文摘Niobium doped Zincoxide nanoparticles has been synthesized through electrochemical method and characterized by UV-Visible spectroscopy, IR Spectroscopy, SEM, XRD, ICPMS and EDAX data. The UV-Visible spectroscopy result reveals that the band gap energy of ZnO/Nb2O5 nanoparticles to be 3.8 eV. The XRD results show that the crystallite size is to be 31.9 nm. The ICPMS data indicate the presence of 3,3461,328 counts of 93 Nb and 577,906,390 counts of 66 Zn. An improvement in the photocatalytic degradation of Indigocarmine dye (IC) in comparison to commercially available pure ZnO was observed. The photodegradation efficiency for ZnO/Nb2O5 and ZnO were found to be 97.4% and 52.1% respectively. The enhancement in photocatalytic activity of ZnO/ Nb2O5 was ascribed to the extended light absorption range and suppression of electron hole pair recombination upon Nb loading. The antibacterial activity of ZnO/Nb2O5 nanoparticles was investigated. These particles were shown to have an effective bactericide.
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.20872135） and the China National Tobacco Corporation （No.110200701007）.
文摘The ordered bimodal mesoporous silica MCM-48 spheres were facile synthesized by mild- temperature post-synthesis H2O2 hydrothermal treatment of as-synthesized MCM-48. The results showed that H2O2 is indispensable for simultaneously removing organic templates and forming ordered bimodal mesoporous silica MCM-48 spheres. The bimodal mesoporous MCM-48 was characterized by X-ray diffraction, transmission electron micrographs, FT-IR, and N2 adsorption-desorption, and a possible mechanism was proposed for the formation of bimodal mesoporous MCM-48.
基金Projects(11JJ3020,10JJ9015)supported by Hunan Provincial Natural Science Foundation of ChinaProject supported by the Construct Program of the Key Discipline in Hunan Province,China
文摘The oxysulfide La3NbS2O5 was synthesized by sulfurization using H2S and characterized by X-ray diffraction （XRD）, UV-Vis diffuse reflectance spectroscopy （DRS） and field emission scanning electron microscopy （FE-SEM）. The relationship between the sulfurization conditions and the photocatalytic activities for H2 evolution was investigated. Sulfurization method allowed for synthesis of La3NbS2O5 at much lower temperatures and significantly shortened reaction time of 1 h compared with conventional solid-state techniques. The particle morphologies were regular platelike with sizes of 0.1-0.6μm and smooth surfaces. The highest activity for H2 evolution was obtained at 1073 K for 1 h, which was about 1.83 times that of La3NbS2O5 prepared by solid-state method.
基金supported by the National Natural Science Foundation of China(U140319321473261+3 种基金41305112)the Excellent Youth Foundation of Xinjiang Uygur Autonomous Region(2013711004)the CAS "Light of West China" Program(YB201303)the CAS/SAFEA International Partnership Program for Creative Research Teams~~
文摘The controllable synthesis of tantalate K1.9Na0.1Ta2O6·2H2O has been successfully achieved by a two-step technique,namely,the molten salt and hydrothermal methods,at a low temperature. By simply varying the KOH concentration in the hydrothermal process,K1.9Na0.1Ta2O6·2H2O particles with spherical,cuboctahedral,and durian-like morphologies were synthesized. The photocatalytic activity of the obtained samples for the degradation of rhodamine B was studied under ultraviolet light,which indicates that the photocatalytic properties of the samples are highly dependent on their morphologies. The K1.9Na0.1Ta2O6·2H2O nanospheres,with rough surfaces and the highest specific surface area,exhibit the best performance. The present work provides a unique approach for the controlled synthesis of tantalate photocatalysts,which are difficult to achieve through other synthetic approaches.
基金support by Northwestern University through a gift from Dr.Warren Haug is greatly appreciated
文摘Vapor phase catalytic hydrogen peroxide production by oxidation of water is possible by coupling the reaction with oxidation of an organic sacrificial reductant. It is potentially a safer process than direct synthesis from H2 and O2. Based on mechanistic information available mostly for liquid phase catalytic processes, feasible reaction mechanisms for such coupled reactions are proposed based on which desirable catalyst properties are identified. It is found that the surface-adsorbed oxygen bond is an important parameter for identifying desirable catalysts. Thermodynamics can be used to identify the types of organic oxidation reactions that can couple with water oxidation such that H2O2 formation becomes thermodynamically favorable. Reactions such as epoxidation of alkenes and selective oxidation of alkanes to alcohols cannot provide sufficient thermodynamic driving force, whereas oxidation of alcohols to aldehydes and to acids can. Finally, further research is suggested to identify catalytic properties important for H2O2 decomposition and for coupling selective oxidation of organic compounds to oxidation of H2O in order to facilitate development of H2O2 production coupled with selective organic oxidation.
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.41373127） and Liaon- ing Provincial Natural Science Foundation of China （No.2013020121）.
文摘A series of Ce, H3PW12O40 co-doped TiO2 hollow fibers photocatalysts have been prepared by sol-gel method using ammonium ceric nitrate, H3PW12O40 and tetrabutyltitanate as precursors and cotton fibers as template, followed by calcination at 500 ℃ in N2 atmosphere for 2 h. Scanning electron microscopy, X-ray diffraction, nitrogen adsorption-desorption mea- surements, and UV-Vis spectroscopy are employed to characterize the morphology, crystal structure, surface structure, and optical absorption properties of the samples. The photo- catalytic performance of the samples has been studied by photodegradation phenol in water under UV and visible light irradiation. The results show that the TiO2 fiber materials have hollow structures, and the co-doped TiO2 hollow fibers exhibit higher photocatalytic activities for the degradation of phenol than un-doped, single-doped TiO2 hollow fibers under UV and visible light. In addition, the recyclability of co-doped TiO2 fibers is also confirmed that the TiO2 fiber retains ca. 90% of its activity after being used four times. It is shown that the co-doped TiO2 fibers can be activated by visible light and may be potentially applied to the treatment of water contaminated by organic pollutants. The synergistic effect of Ce and H3PW12O40 co-doping plays an important role in improving the photocatalytic activity.
基金the National Natural Science Foundation of China(Nos.21805052,21974031,2278092)Science and Technology Research Project of Guangzhou(Nos.202102020787 and 202201000002)+2 种基金Department of Science&Technology of Guangdong Province(No.2022A156)Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.20225546)the Innovation&Entrepreneurship for the College Students of Guangzhou University(No.XJ202111078175).
文摘Electrosynthesis of hydrogen peroxide(H2O2)is an on-site method that enables independent distribution applications in many fields due to its small-scale and sustainable features.The crucial point remains developing highly active,selective and cost-effective electrocatalysts.The electrosynthesis of H2O2 in acidic media is more practical owing to its stability and no need for further purification.We herein report a phosphorus and selenium tuning Co-based non-precious catalyst(CoPSe)toward two-electron oxygen reduction reaction(2e–ORR)to produce H2O2 in acidic media.The starting point of using both P and Se is finding a balance between strong ORR activity of CoSe and weak activity of CoP.The results demonstrated that the CoPSe catalyst exhibited the optimized 2e–ORR activity compared with CoP and CoSe.It disclosed an onset potential of 0.68 V and the H2O2 selectivity 76%-85%in a wide potential range(0–0.5 V).Notably,the CoPSe catalyst overcomes a significant challenge of a narrow-range selectivity for transitionmetal based 2e–ORR catalysts.Finally,combining with electro-Fenton reaction,an on-site system was constructed for efficient degradation of organic pollutants.This work provides a promising non-precious Co-based electrocatalyst for the electrosynthesis of H2O2 in acidic media.
文摘Non-enzymatic biosensors based on mixed transition metal oxides are deemed as the most promising devices due to their high sensitivity,selectivity,wide concentration range,low detection limits,and excellent recyclability.Spinel NiCo2O4 mixed oxides have drawn considerable attention recently due to their outstanding advantages including large specific surface area,high permeability,short electron,and ion diffusion pathways.Because of the rapid development of non-enzyme biosensors,the current state of methods for synthesis of pure and composite/hybrid NiCo2P4 materials and their subsequent electrochemical biosensing applications are systematically and comprehensively reviewed herein.Comparative analysis reveals better electrochemical sensing of bioanalytes by one-dimensional and two-dimensional NiCo2O4 nano-/microstructures than other morphologies.Better biosensing efficiency of NiCo2O4 as compared to corresponding individual metal oxides,viz.NiO and Co3O4,is attributed to the close intrinsic-state redox couples of Ni3+/Ni2+(0.58 V/0.49 V) and Co3+/Co2+(0.53 V/0.51 V).Biosensing performance of NiCo2O4 is also significantly improved by making the composites of NiCo2O4 with conducting carbonaceous materials like graphene,reduced graphene oxide,carbon nanotubes(single and multi-walled),carbon nanofibers;conducting polymers like polypyrrole(PPy),polyaniline(PANI);metal oxides NiO,Co3O4,SnO2,MnO2;and metals like Au,Pd,etc.Various factors affecting the morphologies and biosensing parameters of the nano-/microstructured NiCo2O4 are also highlighted.Finally,some drawbacks and future perspectives related to this promising field are outlined.
文摘LiCoO2 surface layer is proposed and prepared through sol-gel method. The physical and electrochemical performances of pristine LiMn2O4 and LiCoO2-coated LiMn2O4 cathode materials were investigated by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, electrochemical measurements respectively. Comparing with the pristine LiMn2O4, the LiCoO2- coated LiMn2O4 phase significantly improved cycling stability, especially at 55°C. Additionally, the thermal safety of LiMn2O4 is greatly enhanced after being coated by LiCoO2. ICP-AES measurement, structural analysis, and impedance experiments indicate that the improved electrochemical property of LiCoO2-coated LiMn2O4 should be attributed to the alleviated dissolution loss of manganese, strengthened structural stability.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11304185 and 11074151)China Postdoctoral Science Foundation(Grant No.2014M561957)+1 种基金the Postdoctoral Innovation Project of Shandong Province,China(Grant No.201402013)the Shandong Provincial Natural Science Foundation,China(Grant No.ZR2014AM022)
文摘A globally accurate potential energy surface is reported for the electronic ground-state H2O＋. The ab initio energies utilized to map the potential energy surface are calculated at the multireference configuration interaction method employing the aug-cc-pVQZ basis set and the full valence complete active space wave function as reference. In order to improve accu- racy of the resulting raw ab initio energies, they are then extrapolated to the complete basis set limit and most importantly to the full configuration-interaction limit by semiempirically correcting the dynamical correlation using the double many- body expansion-scaled external correlation method. The topographical features of the current potential energy surface were examined in detail, which agree nicely with those of other theoretical work.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.60977063 and 10574039)the Innovation Scientists and Technicians Troop Construction Projects of Henan Province of China (Grant No.084100510011)
文摘Quasi-classical trajectory theory is used to study the reaction of O（3p） with H2 （D2） based on the ground 3A″ potential energy surface （PES）. The reaction cross section of the reaction O＋H2→＋OH＋H is in excellent agreement with the previous result. Vector correlations, product rotational alignment parameters （P2（j′. k）） and several polarizeddependent differential cross sections are further calculated for the reaction. The product polarization distribution exhibits different characteristics that can be ascribed to different motion paths on the PES, arising from various collision energies or mass factors.
基金the National Natural Science Foundation of China(Nos.21975106 and 21403232)MOE&SAFEA,111 Project(B13025)for financial support.
文摘The development of a highly efficient and durable electrocatalyst for nitrate reduction reaction(NO_(3)RR)wastewater valorization to ammonia(NH_(3))is a promising strategy.However,it is challenging to design scalable low-cost electrocatalysts with high activity,high selectivity,and long-term stability by a facile and simple method.Herein,we construct this scalable Cu-based nanoarray with muti-oxidation states grown directly on nickel foam(NF)substrate(Cu_(2+1)O@Cu/NF)using a facile molten salt method combined in-situ electrochemical reduction.The as-prepared Cu_(2+1)O@Cu/NF nanoarrays reveal a high NH_(3) yield of 20.14 mg h^(−1) cm^(−2) at−0.95 V vs.a reversible hydrogen electrode(vs.RHE),Faradaic efficiency of 99.38%at−0.55 V vs.RHE in the neutral potassium phosphate(PBS)buffer solution with 50 mM NaNO_(3),which is ascribed to its electron redistribution with abundant oxygen vacancies and favorable charge/mass transfer.
文摘To enhance the electrochemical performances of LiMn2O4 at elevated temperature (55°C), we proposed a sol-gel method to synthesize LiNi0.5Mn1.5O4 modified LiMn2O4. The physical and electrochemical performances of pristine and LiNi0.5Mn1.5O4-coated LiMn2O4 cathode materials were investigated by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy and electrochemical measurements, respectively. The results indicated that about 4-5 nm thick layer of LiNi0.5Mn1.5O4 was formed on the surface of the LiMn2O4 powders. The modified LiMn2O4 exhibited excellent storage performance at 55°C compared to the pristine one, which was attributed to the suppression of electrolyte decomposition and the reduction of Mn dissolution.
