P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phas...P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.展开更多
Physical vapor deposition(PVD)can be used to produce high-quality Gd_(2)O_(3)-doped CeO2(GDC)films.Among various PVD methods,reactive sputtering provides unique benefits,such as high deposition rates and easy upscalin...Physical vapor deposition(PVD)can be used to produce high-quality Gd_(2)O_(3)-doped CeO2(GDC)films.Among various PVD methods,reactive sputtering provides unique benefits,such as high deposition rates and easy upscaling for industrial applications.GDC thin films were successfully fabricated through reactive sputtering using a Gd_(0.2)Ce_(0.8)(at%)metallic target,and their application in solid oxide fuel cells,such as buffer layers between yttria-stabilized zirconia(YSZ)/La0.6Sr0.4Co0.2Fe0.8O_(3−δ)and as sublayers in the steel/coating system,was evaluated.First,the direct current(DC)reactive-sputtering behavior of the GdCe metallic target was determined.Then,the GDC films were deposited on NiO-YSZ/YSZ half-cells to investigate the influence of oxygen flow rate on the quality of annealed GDC films.The results demonstrated that reactive sputtering can be used to prepare thin and dense GDC buffer layers without high-temperature sintering.Furthermore,the cells with a sputtered GDC buffer layer showed better electrochemical performance than those with a screen-printed GDC buffer layer.In addition,the insertion of a GDC sublayer between the SUS441 interconnects and the Mn-Co spinel coatings contributed to the reduction of the oxidation rate for SUS441 at operating temperatures,according to the area-specific resistance tests.展开更多
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
Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and N...Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles (NGVs) operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction (XRD) and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction (H2-TPR) and oxygen storage capacity (OSC) measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost.展开更多
Characteristics of carbon deposition of CH 4 and C 2H 4 decomposition over supported Ni and Ni Ce catalysts were studied by using a pulse reaction as well as BET, TPR, XPS and hydrogen chemisorption techniques. It...Characteristics of carbon deposition of CH 4 and C 2H 4 decomposition over supported Ni and Ni Ce catalysts were studied by using a pulse reaction as well as BET, TPR, XPS and hydrogen chemisorption techniques. It is found that there is a metal semiconductor interaction (MScI) in the Ni Ce catalyst, and the effect of MScI on the carbon deposition of CH 4 decomposition is opposite to that of C 2H 4. A novel model of carbon deposition of CH 4 or C 2H 4 decomposition was proposed.展开更多
Test alloys ZG40Cr24 with alloying of 3 wt% aluminium were cast by intermediate frequency induction furnace. The oxidation resistance of test alloys at 1 000 ℃ for 500 hours was examined according to oxidation weight...Test alloys ZG40Cr24 with alloying of 3 wt% aluminium were cast by intermediate frequency induction furnace. The oxidation resistance of test alloys at 1 000 ℃ for 500 hours was examined according to oxidation weight gain method. The scale morphology and composition were studied using scanning electron microscope (SEM) and X-ray diffraction (XRD) respectively. By energy dispersive spectroscopy (EDS) studies, a kind of composite oxide scale compounded highly by Cr2O3, Al2O3 and spinel MCr2O4 in molecule scale came into being at high temperature. With flat and compact structure, fine and even grains, such composite scale granted complete oxidation resistance to alloy ZG40Cr24. The oxidation resistance mechanism was studied deeply in electrochemistry corrosion. The P+N semiconductor composite scale composed plenty of inner PN junctions, of which the unilateral conductive and the out-of-order arrangement endowed itself insulating in all directions. The positive and negative charges in scale could not move, and the mobile number and transferring rate of them both dropped enormously, as a result, the oxidation rate of the matrix metal was cut down greatly. So the composite scale presented excellent oxidation resistance.展开更多
V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction (XRD), N2 adsorption-desorption (BET), X-ray photoelectron spectroscopy ...V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction (XRD), N2 adsorption-desorption (BET), X-ray photoelectron spectroscopy (XPS) and catalytic removal of ethanol, acetaldehyde and nitrogen oxides at low temperature (〈300 ?C) were used to assess the properties of the catalysts. The results showed that the sample with 1wt% vanadium exhibited an excellent catalytic performance for simultaneous removal of ethanol, acetaldehyde and nitrogen oxides. The conversions of ethanol, acetaldehyde and nitrogen oxides at 250 ?C were 100%, 74.4% and 98.7%, respectively. V-Pd/γ-Al2O3-TiO2 catalyst with 1 wt% vanadium showed the largest surface area and higher dispersion of vanadium oxide on the catalyst surface, and possessed a larger mole fraction of V4+ species and unique PdO species on the surface, which can be attributed to the strong synergistic effect among palladium, vanadium and the carriers. The higher activity of V-Pd/γ-Al2O3-TiO2 catalyst is related to the V4+ and Pd2+ species on the surface, which might be favorable for the formation of active sites.展开更多
The La2O3/Fe2O3-CeO2 composite oxide catalysts were prepared by coprecipitation method, sol-gel method and hydrothermal method. The effect of preparation methods on structure morphology and photocatalytic properties o...The La2O3/Fe2O3-CeO2 composite oxide catalysts were prepared by coprecipitation method, sol-gel method and hydrothermal method. The effect of preparation methods on structure morphology and photocatalytic properties of La2O3/Fe2O3-CeO2 samples was investigated. The results show that the cubic CeO2 structure can be obtained at 600℃. The rod-shaped sample prepared by coprecipitation method, displays the highest crystalline and the strongest diffraction peak intensity. The spherical sample is acquired from sol-gel method, while the small granular sample prepared by hydrothermal method tends to aggregate. The maximum specific surface area of the sample prepared by coprecipitation method is 76.21 m2/g, the minimum specific area of the sample from sol-gel method is 32.66 m2/g and the maximum pore size is 13.84 nm, while the minimum pore volume and pore size of the sample by hydrothermal method are 0.038 cm3/g and 3.95 nm respectively. The band gap energy of catalyst samples is in the following order: sample-CP < sample-SG < sample-HT. The sample obtained by coprecipitation method has the best catalytic degradation performance for methylene blue. Under the excitation of visible light, the degradation rate was 99.58% at 50 minutes, which was higher than those of sol-gel method and hydrothermal method by 5.58% and 9.54% respectively. The catalytic degradation reaction is a first-order kinetic model: ln (c0/ct) = kt + qe. The maximum k-value of the sample degradation process obtained by coprecipitation method is 0.074 min-1.展开更多
In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can r...In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can reduce silver ions to generate crystalline silver nanoparticles(Ag NPs)of good dispersion and uniformity on the alumina surface,leading to the formation of Ag/γ-Al_(2)O_(3)catalysts in a green manner without traditional chemical reductants.Ag/γ-Al_(2)O_(3)exhibited good catalytic activity and stability in CO oxidation reactions,and the activity increased with increase in the Ag content.For catalysts with more than 2 wt%Ag,100%CO conversion can be achieved at 300°C.The catalytic activity of the Ag/γ-Al_(2)O_(3)catalysts is also closely related to the size of theγ-alumina,where Ag/nano-γ-Al_(2)O_(3)catalysts demonstrate better performance than Ag/micro-γ-Al_(2)O_(3)catalysts with the same Ag content.In addition,the catalytic properties of plasma-generated Ag/nano-γ-Al_(2)O_(3)(Ag/γ-Al_(2)O_(3)-P)catalysts were compared with those of Ag/nano-γ-Al_(2)O_(3)catalysts prepared by the traditional calcination approach(Ag/γ-Al_(2)O_(3)-C),with the plasma-generated samples demonstrating better overall performance.This simple,rapid and green plasma process is considered to be applicable for the synthesis of diverse noble metal-based catalysts.展开更多
The catalyst of CUOx/Al2O3 was prepared by the dipping-sedimentation method using y-Al2O3 as a supporter. CuO and Cu2O were loaded on the surface of Al2O3, characterized by X-ray diffraction (XRD) and X-ray photoele...The catalyst of CUOx/Al2O3 was prepared by the dipping-sedimentation method using y-Al2O3 as a supporter. CuO and Cu2O were loaded on the surface of Al2O3, characterized by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). In the presence of CuOx/Al2O3, the microwave-induced chlorine dioxide (ClO2) catalytic oxidation process was conducted for the treatment of synthetic wastewater containing 100 mg/L phenol. The factors influencing phenol removal were investigated and the results showed that microwave-induced C102-CuOx/ml203 process could effectively degrade contaminants in a short reaction time with a low oxidant dosage, extensive pH range. Under a given condition (ClO2 concentration 80 mg/L, microwave power 50 W, contact time 5 latin, catalyst dosage 50 g/L, pH 9), phenol removal percentage approached 92.24%, corresponding to 79.13% of CODcr removal. The removal of phenol by microwave-induced ClO2-CuOx/Al2O3 catalytic oxidation process was a complicated non-homogeneous solid/water reaction, which fitted pseudo-first-order by kinetics. Compared with traditional ClO2 oxidation, ClO2 catalytic oxidation and microwave-induced ClO2 oxidation, microwave-induced ClO2 catalytic oxidation system could significantly enhance the degradation efficiency. It provides an effective technology for the removal of phenol wastewater.展开更多
Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction(XRD),BET areas,H2 temperature-programmed reduction(H2-TPR),and X-ray photoelectron sp...Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction(XRD),BET areas,H2 temperature-programmed reduction(H2-TPR),and X-ray photoelectron spectroscopy(XPS).Through the test of catalytic partial oxidation of methane(CPOM),Ni/CeO2-ZrO2-Al2O3 displayed the highest activity,which resulted from its largest BET area and best NiO dispersion.Furthermore,Ni/CeO2-ZrO2-Al2O3 maintained a long-time stability in CPOM,which was attributed to its best coking resistance among all the prepared catalysts.展开更多
CeO2-Co3O4 catalysts for low-temperature CO oxidation were prepared by a co-precipitation method. In combination with the characterization methods of N2 adsorption/desorption, XRD, temperature-programmed reduction (...CeO2-Co3O4 catalysts for low-temperature CO oxidation were prepared by a co-precipitation method. In combination with the characterization methods of N2 adsorption/desorption, XRD, temperature-programmed reduction (TPR), and FT-IR, the influence of the cerium content on the catalytic performance of CeO2-Co3O4 was investigated. The results indicate that the prepared CeO2-Co3O4 catalysts exhibit a better activity than that of pure CeO2 or pure Co3O4. The catalyst with the Ce/Co atomic ratio 1 : 16 exhibits the best activity, which converts 77% of CO at room temperature and completely oxidizes CO at 45 ℃.展开更多
DBUH-Br_3 catalyzed selective conversion of sulfides to sulfoxides in the presence of H_2O_2 as oxidizing agent is described.The reaction was performed selectively at room temperature and relatively short reaction times.
NF3 decomposition in the absence of water over Al2O3, Fe2O3, Co3O4 and NiO, and transition metal oxides (Fe203, CO3O4 and NiO) coated Al2O3 reagents was investigated. The results show that Al2O3 is an active reagent...NF3 decomposition in the absence of water over Al2O3, Fe2O3, Co3O4 and NiO, and transition metal oxides (Fe203, CO3O4 and NiO) coated Al2O3 reagents was investigated. The results show that Al2O3 is an active reagent for NF3 decomposition with 100% conversion lasting for 8.5 h at 400 ℃. Fe203, Co3O4 and NiO coated Al2O3 reagents are superior to bare Al2O3, and 5%Co3O4/Al2O3 has a high reactivity with NF3 full conversion maintaining for 10.5 h. It is suggested that the presence of transition metal oxide is beneficial to the reactivity of Al2O3, and results in a significant enhancement in the fluorination of Al2O3.展开更多
ZrO2-Y2O3 ceramic coating was produced by plasma electrolytic oxidation (PEO) on ZAlSil2Cu3Ni2 alloy. The microstructure and phase composition of the coating were investigated by SEM and XRD.: The results show that...ZrO2-Y2O3 ceramic coating was produced by plasma electrolytic oxidation (PEO) on ZAlSil2Cu3Ni2 alloy. The microstructure and phase composition of the coating were investigated by SEM and XRD.: The results show that adding an appropriate amount of yttrium ion can improve the growing rate of ceramic coating at different oxidation stages and decrease arc voltage. The thickness of ZrO2-Y2O3 coating is 16 μn thicker than that of ZrO2 coating and the maximum oxidation rate improves by 0.6 μm/min. In addition, the arc voltage decreases from 227 to 172 V. It can be seen that the rate of oxidation firstly increases to some extent and then decreases with the content of yttrium ion increasing. The growth rate reaches the maximum while the content of yttrium ion is 0.05 g-L-1The maximum thickness is 90 μm.Compared to ZrO2 coating, the micropores of ZrO2-Y2O3 coating are less and the ceramic layer is repeatedly deposited by ZrO2 and Y2O3 ceramic particles. Meanwhile, the binding force between coating and substrate is better and the coating is uniform and compact. The ceramic layer is mainly composed of c-Y0.15Zr0.85O1.93□0.07, m-ZrO2, α-Al2O3, ,γ-Al2O3 and Y2O3. It is indicated that ZrO2 has beert fully stabilized by yttrium ion through the formation of solid solution.展开更多
Ce x Ti 1- x O 2 mixed oxides of different mole ratios ( x =0, 0.1, 0.2~0.9, 1.0) were prepared by co precipitation of TiCl 4 with Ce(NO 3) 3 and then loaded with different amounts of CuO. The effe...Ce x Ti 1- x O 2 mixed oxides of different mole ratios ( x =0, 0.1, 0.2~0.9, 1.0) were prepared by co precipitation of TiCl 4 with Ce(NO 3) 3 and then loaded with different amounts of CuO. The effects of CuO on NO+CO reaction were investigated, and the structure and reductive properties of various CuO/Ce x Ti 1- x O 2 were characterized by the methodologies of BET, TPR and XRD. The results show that different Ce/Ti mole ratios and calcination temperatures induce changes of structure and reductive properties of the Ce x Ti 1- x O 2 mixed oxides. When x =0.1~0.5, amorphous CeTi 2O 6 phase mainly forms at 650 ℃ compared to the formation of CeTi 2O 6 which crystallizes at 800 ℃. When x >0.6, some TiO 2 enters the CeO 2 lattice and a CeO 2 TiO 2 solid solution is formed. The activity of 6%CuO/Ce x Ti 1- x O 2 calcined at 650 ℃ is largely affected by the x values, which is the highest when x =0.3, 0.4 and 0.9. The NO conversion reaches 70% at a reaction temperature of 150 ℃. By comparison, the x values have little effect on the activity of 6%CuO/Ce x Ti 1- x O 2 calcined at 800 ℃ . There are strong interactions between CuO and CeTi 2O 6, i.e., formation of the CeTi 2O 6 phase shifts the CuO reduction peak temperature from 380 to 200 ℃, and CuO, in turn, shifts the CeTi 2O 6 reduction peak temperature from 600 to 300 ℃.展开更多
Polycrystalline particles of Ca3-xErxCo2O6 (x=0.0, 0.15, 0.3, 0.45 and 0.6) were synthesized using sol-gel method combined with Low Temperature Sintering procedure (LTS) to evaluate the effect of Er substitution o...Polycrystalline particles of Ca3-xErxCo2O6 (x=0.0, 0.15, 0.3, 0.45 and 0.6) were synthesized using sol-gel method combined with Low Temperature Sintering procedure (LTS) to evaluate the effect of Er substitution on the thermoelectric properties of Ca3Co2O6. The crystal structure and microstructure were investigated using X-ray diffraction, infrared spectroscopy and scanning electron microscope. The electrical conductivity and Seebeck coefficient of the complex oxides were measured from 300 to 1073 K. The results showed that all the sampies were p-type semiconductors. The electrical conductivity increased with the increase in temperature. Er substitutions at Ca site affected carrier concentrations and carder mobility, resulting an increase in Seebeck coefficient and decrease in electrical conductivity. The power factor of Ca2.85Er0.15Co2O6 reached 10.66 μw/mK^2 at 1073 K.展开更多
基金supported by the National Natural Science Foundation of China (22169002)the Chongzuo Key Research and Development Program of China (20220603)the Counterpart Aid Project for Discipline Construction from Guangxi University(2023M02)
文摘P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.
基金financially supported by the National Key R&D Program of China (No. 2018YFB1502203-1)the Guangdong Basic and Applied Basic Research Foundation (No. 2021B1515120087)the Stable Supporting Fund of Shenzhen, China (No. GXWD20201230155427003-202007 28114835006)
文摘Physical vapor deposition(PVD)can be used to produce high-quality Gd_(2)O_(3)-doped CeO2(GDC)films.Among various PVD methods,reactive sputtering provides unique benefits,such as high deposition rates and easy upscaling for industrial applications.GDC thin films were successfully fabricated through reactive sputtering using a Gd_(0.2)Ce_(0.8)(at%)metallic target,and their application in solid oxide fuel cells,such as buffer layers between yttria-stabilized zirconia(YSZ)/La0.6Sr0.4Co0.2Fe0.8O_(3−δ)and as sublayers in the steel/coating system,was evaluated.First,the direct current(DC)reactive-sputtering behavior of the GdCe metallic target was determined.Then,the GDC films were deposited on NiO-YSZ/YSZ half-cells to investigate the influence of oxygen flow rate on the quality of annealed GDC films.The results demonstrated that reactive sputtering can be used to prepare thin and dense GDC buffer layers without high-temperature sintering.Furthermore,the cells with a sputtered GDC buffer layer showed better electrochemical performance than those with a screen-printed GDC buffer layer.In addition,the insertion of a GDC sublayer between the SUS441 interconnects and the Mn-Co spinel coatings contributed to the reduction of the oxidation rate for SUS441 at operating temperatures,according to the area-specific resistance tests.
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supported by the National Natural Science Foundation of China (No. 20773090, 20803049)the National High Technology Researchand Development Program of China (863 Program, No. 2006AA06Z347)the Specialized Research Fund for the Doctoral Program of Higher Education(20070610026)
文摘Composite supports CeO2-ZrO2-Al2O3(CZA) and CeO2-ZrO2-Al2O3-La2O3(CZALa) were prepared by co-precipitation method. Palladium catalysts were prepared by impregnation and their purification ability for CH4, CO and NOx in the mixture gas simulated the exhaust from natural gas vehicles (NGVs) operated under stoichiometric condition was investigated. The effect of La2O3 on the physicochemical properties of supports and catalysts was characterized by various techniques. The characterizations with X-ray diffraction (XRD) and Raman spectroscopy revealed that the doping of La2O3 restrained effectively the sintering of crystallite particles, maintained the crystallite particles in nanoscale and stabilized the crystal phase after calcination at 1000 ℃. The results of N2-adsorption, H2-temperatnre-programmed reduction (H2-TPR) and oxygen storage capacity (OSC) measurements indicated that La2O3 improved the textural properties, reducibility and OSC of composite supports. Activity testing results showed that the catalysts exhibit excellent activities for the simultaneous removal of methane, CO and NOx in the simulated exhaust gas. The catalysts supported on CZALa showed remarkable thermal stability and catalytic activity for the three pollutants, especially for NOx. The prepared palladium catalysts have high ability to remove NOx, CH4 and CO, and they can be used as excellent catalysts for the purification of exhaust from NGVs operated under stoichiometric condition. The catalysts reported in this work also have significant potential in industrial application because of their high performance and low cost.
文摘Characteristics of carbon deposition of CH 4 and C 2H 4 decomposition over supported Ni and Ni Ce catalysts were studied by using a pulse reaction as well as BET, TPR, XPS and hydrogen chemisorption techniques. It is found that there is a metal semiconductor interaction (MScI) in the Ni Ce catalyst, and the effect of MScI on the carbon deposition of CH 4 decomposition is opposite to that of C 2H 4. A novel model of carbon deposition of CH 4 or C 2H 4 decomposition was proposed.
文摘Test alloys ZG40Cr24 with alloying of 3 wt% aluminium were cast by intermediate frequency induction furnace. The oxidation resistance of test alloys at 1 000 ℃ for 500 hours was examined according to oxidation weight gain method. The scale morphology and composition were studied using scanning electron microscope (SEM) and X-ray diffraction (XRD) respectively. By energy dispersive spectroscopy (EDS) studies, a kind of composite oxide scale compounded highly by Cr2O3, Al2O3 and spinel MCr2O4 in molecule scale came into being at high temperature. With flat and compact structure, fine and even grains, such composite scale granted complete oxidation resistance to alloy ZG40Cr24. The oxidation resistance mechanism was studied deeply in electrochemistry corrosion. The P+N semiconductor composite scale composed plenty of inner PN junctions, of which the unilateral conductive and the out-of-order arrangement endowed itself insulating in all directions. The positive and negative charges in scale could not move, and the mobile number and transferring rate of them both dropped enormously, as a result, the oxidation rate of the matrix metal was cut down greatly. So the composite scale presented excellent oxidation resistance.
基金supported by the National Natural Science Foundation of China (No. 21073131)the Shanxi Natural Science Foundation(No. 2009011011-3)
文摘V-Pd/γ-Al2O3-TiO2 catalysts with different vanadium contents were prepared by a combined sol-gel and impregnation method. X-ray diffraction (XRD), N2 adsorption-desorption (BET), X-ray photoelectron spectroscopy (XPS) and catalytic removal of ethanol, acetaldehyde and nitrogen oxides at low temperature (〈300 ?C) were used to assess the properties of the catalysts. The results showed that the sample with 1wt% vanadium exhibited an excellent catalytic performance for simultaneous removal of ethanol, acetaldehyde and nitrogen oxides. The conversions of ethanol, acetaldehyde and nitrogen oxides at 250 ?C were 100%, 74.4% and 98.7%, respectively. V-Pd/γ-Al2O3-TiO2 catalyst with 1 wt% vanadium showed the largest surface area and higher dispersion of vanadium oxide on the catalyst surface, and possessed a larger mole fraction of V4+ species and unique PdO species on the surface, which can be attributed to the strong synergistic effect among palladium, vanadium and the carriers. The higher activity of V-Pd/γ-Al2O3-TiO2 catalyst is related to the V4+ and Pd2+ species on the surface, which might be favorable for the formation of active sites.
文摘The La2O3/Fe2O3-CeO2 composite oxide catalysts were prepared by coprecipitation method, sol-gel method and hydrothermal method. The effect of preparation methods on structure morphology and photocatalytic properties of La2O3/Fe2O3-CeO2 samples was investigated. The results show that the cubic CeO2 structure can be obtained at 600℃. The rod-shaped sample prepared by coprecipitation method, displays the highest crystalline and the strongest diffraction peak intensity. The spherical sample is acquired from sol-gel method, while the small granular sample prepared by hydrothermal method tends to aggregate. The maximum specific surface area of the sample prepared by coprecipitation method is 76.21 m2/g, the minimum specific area of the sample from sol-gel method is 32.66 m2/g and the maximum pore size is 13.84 nm, while the minimum pore volume and pore size of the sample by hydrothermal method are 0.038 cm3/g and 3.95 nm respectively. The band gap energy of catalyst samples is in the following order: sample-CP < sample-SG < sample-HT. The sample obtained by coprecipitation method has the best catalytic degradation performance for methylene blue. Under the excitation of visible light, the degradation rate was 99.58% at 50 minutes, which was higher than those of sol-gel method and hydrothermal method by 5.58% and 9.54% respectively. The catalytic degradation reaction is a first-order kinetic model: ln (c0/ct) = kt + qe. The maximum k-value of the sample degradation process obtained by coprecipitation method is 0.074 min-1.
基金financial support from National Natural Science Foundation of China(Nos.52004102 and 22078125)Postdoctoral Science Foundation of China(No.2021M690068)+2 种基金Fundamental Research Funds for the Central Universities(Nos.JUSRP221018 and JUSRP622038)Key Laboratory of Green Cleaning Technology and Detergent of Zhejiang Province(No.Q202204)Open Project of Key Laboratory of Green Chemical Engineering Process of Ministry of Education(No.GCP202112)。
文摘In this study,Ag/γ-Al_(2)O_(3)catalysts were synthesized by an Ar dielectric barrier discharge plasma using silver nitrate as the Ag source andγ-alumina(γ-Al_(2)O_(3))as the support.It is revealed that plasma can reduce silver ions to generate crystalline silver nanoparticles(Ag NPs)of good dispersion and uniformity on the alumina surface,leading to the formation of Ag/γ-Al_(2)O_(3)catalysts in a green manner without traditional chemical reductants.Ag/γ-Al_(2)O_(3)exhibited good catalytic activity and stability in CO oxidation reactions,and the activity increased with increase in the Ag content.For catalysts with more than 2 wt%Ag,100%CO conversion can be achieved at 300°C.The catalytic activity of the Ag/γ-Al_(2)O_(3)catalysts is also closely related to the size of theγ-alumina,where Ag/nano-γ-Al_(2)O_(3)catalysts demonstrate better performance than Ag/micro-γ-Al_(2)O_(3)catalysts with the same Ag content.In addition,the catalytic properties of plasma-generated Ag/nano-γ-Al_(2)O_(3)(Ag/γ-Al_(2)O_(3)-P)catalysts were compared with those of Ag/nano-γ-Al_(2)O_(3)catalysts prepared by the traditional calcination approach(Ag/γ-Al_(2)O_(3)-C),with the plasma-generated samples demonstrating better overall performance.This simple,rapid and green plasma process is considered to be applicable for the synthesis of diverse noble metal-based catalysts.
基金Project supported by the National Nature Science Foundation of China(No.50678045).
文摘The catalyst of CUOx/Al2O3 was prepared by the dipping-sedimentation method using y-Al2O3 as a supporter. CuO and Cu2O were loaded on the surface of Al2O3, characterized by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). In the presence of CuOx/Al2O3, the microwave-induced chlorine dioxide (ClO2) catalytic oxidation process was conducted for the treatment of synthetic wastewater containing 100 mg/L phenol. The factors influencing phenol removal were investigated and the results showed that microwave-induced C102-CuOx/ml203 process could effectively degrade contaminants in a short reaction time with a low oxidant dosage, extensive pH range. Under a given condition (ClO2 concentration 80 mg/L, microwave power 50 W, contact time 5 latin, catalyst dosage 50 g/L, pH 9), phenol removal percentage approached 92.24%, corresponding to 79.13% of CODcr removal. The removal of phenol by microwave-induced ClO2-CuOx/Al2O3 catalytic oxidation process was a complicated non-homogeneous solid/water reaction, which fitted pseudo-first-order by kinetics. Compared with traditional ClO2 oxidation, ClO2 catalytic oxidation and microwave-induced ClO2 oxidation, microwave-induced ClO2 catalytic oxidation system could significantly enhance the degradation efficiency. It provides an effective technology for the removal of phenol wastewater.
基金Project supported by State Key Fundamental Research Project(G1999022400)
文摘Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction(XRD),BET areas,H2 temperature-programmed reduction(H2-TPR),and X-ray photoelectron spectroscopy(XPS).Through the test of catalytic partial oxidation of methane(CPOM),Ni/CeO2-ZrO2-Al2O3 displayed the highest activity,which resulted from its largest BET area and best NiO dispersion.Furthermore,Ni/CeO2-ZrO2-Al2O3 maintained a long-time stability in CPOM,which was attributed to its best coking resistance among all the prepared catalysts.
文摘CeO2-Co3O4 catalysts for low-temperature CO oxidation were prepared by a co-precipitation method. In combination with the characterization methods of N2 adsorption/desorption, XRD, temperature-programmed reduction (TPR), and FT-IR, the influence of the cerium content on the catalytic performance of CeO2-Co3O4 was investigated. The results indicate that the prepared CeO2-Co3O4 catalysts exhibit a better activity than that of pure CeO2 or pure Co3O4. The catalyst with the Ce/Co atomic ratio 1 : 16 exhibits the best activity, which converts 77% of CO at room temperature and completely oxidizes CO at 45 ℃.
文摘DBUH-Br_3 catalyzed selective conversion of sulfides to sulfoxides in the presence of H_2O_2 as oxidizing agent is described.The reaction was performed selectively at room temperature and relatively short reaction times.
基金supported by the National Natural Science Foundation of China (No. 20573089, 20976149)
文摘NF3 decomposition in the absence of water over Al2O3, Fe2O3, Co3O4 and NiO, and transition metal oxides (Fe203, CO3O4 and NiO) coated Al2O3 reagents was investigated. The results show that Al2O3 is an active reagent for NF3 decomposition with 100% conversion lasting for 8.5 h at 400 ℃. Fe203, Co3O4 and NiO coated Al2O3 reagents are superior to bare Al2O3, and 5%Co3O4/Al2O3 has a high reactivity with NF3 full conversion maintaining for 10.5 h. It is suggested that the presence of transition metal oxide is beneficial to the reactivity of Al2O3, and results in a significant enhancement in the fluorination of Al2O3.
基金Funded by the National Natural Science Foundation of China(No.51401155)the School Foundation(No.XAGDXJJ1012)The Open Fund of Shaanxi Key Laboratory of Photoelectric Functional Materials and Devices(No.ZSKJ201416)
文摘ZrO2-Y2O3 ceramic coating was produced by plasma electrolytic oxidation (PEO) on ZAlSil2Cu3Ni2 alloy. The microstructure and phase composition of the coating were investigated by SEM and XRD.: The results show that adding an appropriate amount of yttrium ion can improve the growing rate of ceramic coating at different oxidation stages and decrease arc voltage. The thickness of ZrO2-Y2O3 coating is 16 μn thicker than that of ZrO2 coating and the maximum oxidation rate improves by 0.6 μm/min. In addition, the arc voltage decreases from 227 to 172 V. It can be seen that the rate of oxidation firstly increases to some extent and then decreases with the content of yttrium ion increasing. The growth rate reaches the maximum while the content of yttrium ion is 0.05 g-L-1The maximum thickness is 90 μm.Compared to ZrO2 coating, the micropores of ZrO2-Y2O3 coating are less and the ceramic layer is repeatedly deposited by ZrO2 and Y2O3 ceramic particles. Meanwhile, the binding force between coating and substrate is better and the coating is uniform and compact. The ceramic layer is mainly composed of c-Y0.15Zr0.85O1.93□0.07, m-ZrO2, α-Al2O3, ,γ-Al2O3 and Y2O3. It is indicated that ZrO2 has beert fully stabilized by yttrium ion through the formation of solid solution.
文摘Ce x Ti 1- x O 2 mixed oxides of different mole ratios ( x =0, 0.1, 0.2~0.9, 1.0) were prepared by co precipitation of TiCl 4 with Ce(NO 3) 3 and then loaded with different amounts of CuO. The effects of CuO on NO+CO reaction were investigated, and the structure and reductive properties of various CuO/Ce x Ti 1- x O 2 were characterized by the methodologies of BET, TPR and XRD. The results show that different Ce/Ti mole ratios and calcination temperatures induce changes of structure and reductive properties of the Ce x Ti 1- x O 2 mixed oxides. When x =0.1~0.5, amorphous CeTi 2O 6 phase mainly forms at 650 ℃ compared to the formation of CeTi 2O 6 which crystallizes at 800 ℃. When x >0.6, some TiO 2 enters the CeO 2 lattice and a CeO 2 TiO 2 solid solution is formed. The activity of 6%CuO/Ce x Ti 1- x O 2 calcined at 650 ℃ is largely affected by the x values, which is the highest when x =0.3, 0.4 and 0.9. The NO conversion reaches 70% at a reaction temperature of 150 ℃. By comparison, the x values have little effect on the activity of 6%CuO/Ce x Ti 1- x O 2 calcined at 800 ℃ . There are strong interactions between CuO and CeTi 2O 6, i.e., formation of the CeTi 2O 6 phase shifts the CuO reduction peak temperature from 380 to 200 ℃, and CuO, in turn, shifts the CeTi 2O 6 reduction peak temperature from 600 to 300 ℃.
基金the National Natural Science Foundation of China (20571019)Scientific Research Foundation for the Returned Overseas Chinese Scholars, Heilongjiang (LC06C130)Program of Harbin Subject Chief Scientist
文摘Polycrystalline particles of Ca3-xErxCo2O6 (x=0.0, 0.15, 0.3, 0.45 and 0.6) were synthesized using sol-gel method combined with Low Temperature Sintering procedure (LTS) to evaluate the effect of Er substitution on the thermoelectric properties of Ca3Co2O6. The crystal structure and microstructure were investigated using X-ray diffraction, infrared spectroscopy and scanning electron microscope. The electrical conductivity and Seebeck coefficient of the complex oxides were measured from 300 to 1073 K. The results showed that all the sampies were p-type semiconductors. The electrical conductivity increased with the increase in temperature. Er substitutions at Ca site affected carrier concentrations and carder mobility, resulting an increase in Seebeck coefficient and decrease in electrical conductivity. The power factor of Ca2.85Er0.15Co2O6 reached 10.66 μw/mK^2 at 1073 K.