Layered transition metal hydroxides show distinct advantages in separately co-catalyzing CO_(2)reduction and H_(2)O oxidation at the electron-accumulating and hole-accumulating sites of wrapped heterojunction photocat...Layered transition metal hydroxides show distinct advantages in separately co-catalyzing CO_(2)reduction and H_(2)O oxidation at the electron-accumulating and hole-accumulating sites of wrapped heterojunction photocatalysts,while concurrently preventing side reactions and photocorrosion on the semiconductor surface.Herein,Ni-Co bimetallic hydroxides with varying Ni/Co molar ratios(Ni_(x)Co_(1-x)(OH)_(2),x=1,0.75,0.5,0.25,and 0)were grown in situ on a model 2D/2D S-scheme heterojunction composed of Cu_(2)O nanosheets and Fe_(2)O_(3)nanoplates to form a series of Cu_(2)O/Fe_(2)O_(3)@Ni_(x)Co_(1-x)(OH)_(2)(CF@NiCo)photocatalysts.The combined experimental and theoretical investigation demonstrates that incorporating an appropriate amount of Co into Ni(OH)_(2)not only modulates the energy band structure of Ni_(x)Co_(1-x)(OH)_(2),balances the electron-and hole-trapping abilities of the bifunctional cocatalyst and maximizes the charge separation efficiency of the heterojunction,but also regulates the d-band center of Ni_(x)Co_(1-x)(OH)_(2),reinforcing the adsorption and activation of CO_(2)and H_(2)O on the cocatalyst surface and lowering the rate-limiting barriers in the CO_(2)-to-CO and H_(2)O-to-O_(2)conversion.Benefiting from the Ni-Co synergy,the redox reactions proceed stoichiometrically.The optimized CF@Ni_(0.75)Co_(0.25)achieves CO and O_(2)yields of 552.7 and 313.0μmol gcat^(-1)h^(-1),respectively,11.3/9.9,1.6/1.7,and 4.5/5.9-fold higher than those of CF,CF@Ni,and CF@Co.This study offers valuable insights into the design of bifunctional noble-metal-free cocatalysts for high-performance artificial photosynthesis.展开更多
The expandable graphite(EG)modified TiO_(2) nanocomposites were prepared by the high shearmethod using the TiO_(2) nanoparticles(NPs)and EG as precursors,in which the amount of EG doped in TiO_(2) was 10 wt.%.Followed...The expandable graphite(EG)modified TiO_(2) nanocomposites were prepared by the high shearmethod using the TiO_(2) nanoparticles(NPs)and EG as precursors,in which the amount of EG doped in TiO_(2) was 10 wt.%.Followed by the impregnation method,adjusting the pH of the solution to 10,and using the electrostatic adsorption to achieve spatial confinement,the Pt elementswere mainly distributed on the exposed TiO_(2),thus generating the Pt/10EG-TiO_(2)-10 catalyst.The best CO oxidation activity with the excellent resistance to H_(2)O and SO_(2) was obtained over the Pt/10EG-TiO_(2)-10 catalyst:CO conversion after 36 hr of the reaction was ca.85%under the harsh condition of 10 vol.%H_(2)O and 100 ppm SO_(2) at a high gaseous hourly space velocity(GHSV)of 400,000 hr−1.Physicochemical properties of the catalystswere characterized by various techniques.The results showed that the electrostatic adsorption,which riveted the Pt elements mainly on the exposed TiO_(2) of the support surface,reduced the dispersion of Pt NPs on EG and achieved the effective dispersion of Pt NPs,hence significantly improving CO oxidation activity over the Pt/10EG-TiO_(2)-10 catalyst.The 10 wt.%EG doped in TiO_(2) caused the TiO_(2) support to form a more hydrophobic surface,which reduced the adsorption of H_(2)O and SO_(2) on the catalyst,greatly inhibited deposition of the TiOSO_(4) and formation of the PtSO4 species as well as suppressed the oxidation of SO_(2),thus resulting in an improvement in the resistance to H_(2)O and SO_(2) of the Pt/10EG-TiO_(2)-10 catalyst.展开更多
Two Al2O3/Cu composites containing 0.24 wt.% Al2O3 and 0.60 wt.% Al2O3 separately are prepared by internal oxidation. Effects of sliding speed and pressure on the frictional characteristics of the composites and coppe...Two Al2O3/Cu composites containing 0.24 wt.% Al2O3 and 0.60 wt.% Al2O3 separately are prepared by internal oxidation. Effects of sliding speed and pressure on the frictional characteristics of the composites and copper against brass are investigated and compared. The changes in morphology of the sliding surface and subsurface are examined with scanning electron microscope （SEM） and energy dispersive X-ray spectrum （EDS）. The results show that the wear resistance of the Al2O3/Cu composites is superior to that of copper under the same conditions, Under a given electrical current, the wear rate of Al2O3/Cu composites decreases as the Al2O3-content increases, However, the wear rates of the Al2O3/Cu composites and copper increase as the sliding speed and pressure increase under dry sliding condition. The main wear mechanisms for Al2O3/Cu composites are of abrasion and adhesion; for copper, it is adhesion, although wear by oxidation and electrical erosion can also be observed as the speed and pressure rise.展开更多
α-Bi2O3 powders were prepared from nanometer Bi powders through low-temperature oxidation at less than 873.15 K. XRD, SEM, TEM and HRTEM were used to characterize the structure and morphology of Bi powders and Bi2O3 ...α-Bi2O3 powders were prepared from nanometer Bi powders through low-temperature oxidation at less than 873.15 K. XRD, SEM, TEM and HRTEM were used to characterize the structure and morphology of Bi powders and Bi2O3 particles. Kinetic studies on the bismuth oxidation at low-temperatures were carried out by TGA method. The results show that bismuth beads should be reunited and oxidized to become irregular Bi2O3 powders. The bismuth oxidation follows shrinking core model, and its controlling mechanism varies at different reaction time. Within 0-10 min, the kinetics is controlled by chemical reaction, after that it is controlled by O2 diffusion in the solid α-Bi2O3 layer. The apparent activation energy is determined as 55.19 kJ/mol in liquid-phase oxidation.展开更多
Layered transition metal oxides have emerged as promising cathode materials for sodium ion batteries.However,irreversible phase transitions cause structural distortion and cation rearrangement,leading to sluggish Na+d...Layered transition metal oxides have emerged as promising cathode materials for sodium ion batteries.However,irreversible phase transitions cause structural distortion and cation rearrangement,leading to sluggish Na+dynamics and rapid capacity decay.In this study,we propose a medium-entropy cathode by simultaneously introducing Fe,Mg,and Li dopants into a typical P2-type Na_(0.75)Ni_(0.25)Mn_(0.75)O_(2)cathode.The modified Na_(0.75)Ni_(0.2125)Mn_(0.6375)Fe_(0.05)Mg_(0.05)Li_(0.05)O_(2)cathode predominantly exhibits a main P2 phase(93.5%)with a minor O3 phase(6.5%).Through spectroscopy techniques and electrochemical investigations,we elucidate the redox mechanisms of Ni^(2+/3+/4+),Mn^(3+/4+),Fe^(3+/4+),and O_(2)-/O_(2)^(n-)during charging/discharging.The medium-entropy doping mitigates the detrimental P2-O_(2)phase transition at high-voltage,replacing it with a moderate and reversible structural evolution(P2-OP4),thereby enhancing structural stability.Consequently,the modified cathode exhibits a remarkable rate capacity of 108.4 mAh·g^(-1)at 10C,with a capacity retention of 99.0%after 200 cycles at 1C,82.5%after 500 cycles at 5C,and 76.7%after 600 cycles at 10C.Furthermore,it also demonstrates superior electrochemical performance at high cutoff voltage of 4.5 V and extreme temperature(55 and 0℃).This work offers solutions to critical challenges in sodium ion batteries cathode materials.展开更多
Ni-La2O3/CeO2 composite films were prepared by electrodeposition from a nickel sulfate bath containing certain content of micrometer and nanometer La2O3/CeO2 particles. The effect of La2O3 or CeO2 particle size on the...Ni-La2O3/CeO2 composite films were prepared by electrodeposition from a nickel sulfate bath containing certain content of micrometer and nanometer La2O3/CeO2 particles. The effect of La2O3 or CeO2 particle size on the oxidation resistance of the electrodeposited Ni-La2O3/CeO2 composites in air at 1000 °C was studied. The results indicate that, compared with the electrodeposited Ni-film, Ni-La2O3/CeO2 composites exhibit a superior oxidation resistance due to the codeposited La2O3 or CeO2 particles blocking the outward diffusion of nickel. Moreover, compared with nanoparticles, La2O3 or CeO2 microparticles have stronger effect because La2O3 or CeO2 microparticles also act as a diffusion barrier layer at the onset of oxidation.展开更多
3Gd2O3-3Yb2O3-4Y2O3 （mole fraction, %） co-doped ZrO2 （GY-YSZ） thermal barrier coatings （TBCs） were produced by electron beam physical vapor deposition （EB-PVD）. The oxidation behavior of GY-YSZ at 1 050 ℃ was...3Gd2O3-3Yb2O3-4Y2O3 （mole fraction, %） co-doped ZrO2 （GY-YSZ） thermal barrier coatings （TBCs） were produced by electron beam physical vapor deposition （EB-PVD）. The oxidation behavior of GY-YSZ at 1 050 ℃ was investigated using impedance spectroscopy （IS） combined with scanning electron microscopy （SEM）, Raman spectroscopy and X-ray diffractometry （XRD）. Various electrical responses observed in the impedance spectra corresponding to GY-YSZ grains and grain boundaries were explained using circuit modeling. The change in the conduction mechanism of GY-YSZ was found to be related to the O^2- vacancy and lattice distortion due to the stabilizer diffusion during the oxidation. The results also suggested that the specific oxidation information about the GY-YSZ grains and grain boundaries should be acquired at a moderate measurement temperature, which was related to the resistance value in the impedance spectra. The resistance values of the GY-YSZ grains and grain boundaries should be measured at 200 ℃ and 300 ℃, respectively.展开更多
Al2O3/Au nano-laminated composite coatings were prepared by means of magnetron sputtering. The coating was compact and comprised of nano-laminated Al2O3 and Au layers. High temperature cyclic oxidation test was employ...Al2O3/Au nano-laminated composite coatings were prepared by means of magnetron sputtering. The coating was compact and comprised of nano-laminated Al2O3 and Au layers. High temperature cyclic oxidation test was employed to investigate the oxidation resistance of the composite coatings. The results revealed that the applied Al2O3/Au nano-laminated composite coatings improved the oxidation and spallation resistance of the stainless steel substrate significantly. The mechanism accounting for oxidation resistance was related with the suppression of inward oxygen diffusion and selective oxidation of Cr in the substrate. The mechanism accounting for spallation resistance was attributed to the relaxation of thermal stress by the nano-laminated structure.展开更多
A series of K-promoted Pt/Al2O3 catalysts were tested for CO oxidation. It was found that the addition of K significantly enhanced the activity. A detailed kinetic study showed that the activation energies of the K-co...A series of K-promoted Pt/Al2O3 catalysts were tested for CO oxidation. It was found that the addition of K significantly enhanced the activity. A detailed kinetic study showed that the activation energies of the K-containing catalysts were lower than those of the K-free ones, particularly for catalysts with high Pt contents （51.6 k）/mol for 0.42K-2.0Pt/Al2O3 and 6：3.6 kJ/mol for 2.0Pt/Al2O3 ）. The CO reaction orders were higher for the K-containing catalysts （about -0.2） than for the K-free ones （about -0.5）, with the former having much lower equilibrium constants for CO adsorption than the latter. In situ Fourier-transform infrared spectroscopy showed that surface CO desorption from the 0.42K-2.0Pt/Al2O3 catalyst was easier than from 2.0Pt/Al2O3. The promoting effect of K was therefore caused by weakening of the interactions between CO and surface Pt atoms. This decreased coverage of the catalyst with CO and facilitated competitive O2 chemisorption on the Pt surface, and significantly lowered the reaction barrier between chemisorbed CO and O2 species.展开更多
Heterogeneous oxidation of gas-phase Hg 0 by nano-Fe 2 O 3 was investigated on a fixed bed reactor, and the effects of oxygen concentration, bed temperature, water vapour concentration and particle size have been disc...Heterogeneous oxidation of gas-phase Hg 0 by nano-Fe 2 O 3 was investigated on a fixed bed reactor, and the effects of oxygen concentration, bed temperature, water vapour concentration and particle size have been discussed. The results showed that Hg 0 could be oxidized by active oxygen atom on the surface of nano-Fe 2 O 3 as well as lattice oxygen in nano-Fe 2 O 3 . Among the factors that affect Hg 0 oxidation by nano-Fe 2 O 3 , bed temperature plays an important role. More than 40% of total mercury was oxidized at 300°C, however, the test temperature at 400°C could cause sintering of nano-catalyst, which led to a lower efficiency of Hg 0 oxidation. The increase of oxygen concentration could promote mercury oxidation and led to higher Hg 0 oxidation efficiency. No obvious mercury oxidation was detected in the pure N 2 atmosphere, which indicates that oxygen is required in the gas stream for mercury oxidation. The presence of water vapour showed different effects on mercury oxidation depending on its concentration. The lower content of water vapour could promote mercury oxidation, while the higher content of water vapour inhibits mercury oxidation.展开更多
Large amounts of cyanide tailings are produced during the cyanidation process in gold extraction,which are hazardous solid wastes due to the toxic cyanide.Pyrite is one of the main minerals in cyanide tailings.The rem...Large amounts of cyanide tailings are produced during the cyanidation process in gold extraction,which are hazardous solid wastes due to the toxic cyanide.Pyrite is one of the main minerals in cyanide tailings.The removal of cyanide adsorbed on pyrite by H_2O_2 oxidation under alkaline conditions was investigated in this study.It was found that the removal efficiency was positively correlated with pH from 5 to 12,but remained almost constant when pH was higher than 12.The highest cyanide removal efficiency of 91.10% was achieved by adding no less than 0.6 wt.% of H_2O_2.Cyanide removal was positively correlated with the CN^-adsorption amount between 1.06 and 8.5 mg/g,and temperature between 25 and 85°C.The removal of cyanide adsorbed on pyrite by H_2O_2 oxidation under alkaline conditions was due to the oxidation of pyrite.Hexacyanoferrate,thiocyanate and sulfate were generated with mole ratios of about 2.03:1.12:3.17 during the cyanide removal.?2018 The Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences.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
The BiOCl/Bi12O17Cl2@MoS2(BOC-MS)composites were successfully synthesized by a facile method at room temperature.The physicochemical properties of the as-obtained samples were characterized by X-ray diffractometer(XRD...The BiOCl/Bi12O17Cl2@MoS2(BOC-MS)composites were successfully synthesized by a facile method at room temperature.The physicochemical properties of the as-obtained samples were characterized by X-ray diffractometer(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),ultraviolet–visible diffuse reflection spectra(UV–Vis DRS),photoluminescence(PL),Brunauer–Emmett–Teller–Barrett–Joyner–Halenda(BET–BJH),and electron spin resonance(ESR)in detail.Moreover,the in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)was applied to elucidate the adsorption and photocatalytic reaction mechanism.The optimized BOC-MS-1.0 composites exhibited excellent visible light photocatalytic capability(51.1%)and photochemical stability for removal of NO.Based on the DMPOESR spin trapping,the·O2-radicals andáOH radicals were identified as the main active species generated from BOCMS-1.0 under visible light irradiation.The enhanced photocatalytic performance can be ascribed to the positive synergetic effect of the MoS2 and the effective carrier separation ability.展开更多
A wet catalytic oxidation at room temperature was investigated with solution containing ferric, ferrous and cupric ions for H2S removal. The experiments were carried out in a two step process, and the results obtained...A wet catalytic oxidation at room temperature was investigated with solution containing ferric, ferrous and cupric ions for H2S removal. The experiments were carried out in a two step process, and the results obtained show that the removal efficiency of H2S can always reach 100% in a 300 mm scrubbing column with four sieve plates, and the regeneration of ferric ions in 200 mm bubble column can match the consumed ferric species in absorption. Removal of H2S, production of elemental sulfur and regeneration of ferric, cupric ions can all be accomplished at the same time. No raw material is consumed except O2 in flue gas or air, the process has no secondary pollution and no problem of catalyst degradation and congestion.展开更多
A series of Ce1-xFexO2 （x=0, 0.2, 0.4, 0.6, 0.8, 1） complex oxide catalysts were prepared using the coprecipitation method. The catalysts were characterized by means of XRD and H2-TPR. The reactions between methane ...A series of Ce1-xFexO2 （x=0, 0.2, 0.4, 0.6, 0.8, 1） complex oxide catalysts were prepared using the coprecipitation method. The catalysts were characterized by means of XRD and H2-TPR. The reactions between methane and lattice oxygen from the complex oxides were investigated. The characteristic results revealed that the combination of Ce and Fe oxide in the catalysts could lower the temperature necessary to reduce the cerium oxide. The catalytic activity for selective CH4 oxidation was strongly influenced by dropped Fe species. Adding the appropriate amount of Fe2O3 to CeO2 could promote the action between CH4 and CeO2. Dispersed Fe2O3 first returned to the original state and would then virtually form the Fe species on the catalyst, which could be considered as the active site for selective CH4 oxidation. The appearance of carbon formation was significant and the oxidation of carbon appeared to be the rate-determining step; the amounts of surface reducible oxygen species in CeO2 were also relevant to the activity. Among all the catalysts, Ce0.6Fe0.402 exhibited the best activity, which converted 94.52% of CH4 at 900 ℃.展开更多
The attractive utilization route for one-step catalytic oxidation of dimethyl ether to dimethoxymethane was successfully carried out over the H3PW12O40（40%）/SiO2 catalyst, modified by Cs, K, Ni, and V. The Cs modifi...The attractive utilization route for one-step catalytic oxidation of dimethyl ether to dimethoxymethane was successfully carried out over the H3PW12O40（40%）/SiO2 catalyst, modified by Cs, K, Ni, and V. The Cs modification of H3PW12O40（40%）/SiO2 gave the most promising result of 20% dimethyl ether conversion and 34.8% dimethoxymethane selectivity. Dimethoxymethane could be synthe- sized via methoxy groups decomposed from dimethyl ether through the synergistic effect between the acid sites and the redox sites of Cs modified H3PW12O40（40%）/SiO2.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
文摘Layered transition metal hydroxides show distinct advantages in separately co-catalyzing CO_(2)reduction and H_(2)O oxidation at the electron-accumulating and hole-accumulating sites of wrapped heterojunction photocatalysts,while concurrently preventing side reactions and photocorrosion on the semiconductor surface.Herein,Ni-Co bimetallic hydroxides with varying Ni/Co molar ratios(Ni_(x)Co_(1-x)(OH)_(2),x=1,0.75,0.5,0.25,and 0)were grown in situ on a model 2D/2D S-scheme heterojunction composed of Cu_(2)O nanosheets and Fe_(2)O_(3)nanoplates to form a series of Cu_(2)O/Fe_(2)O_(3)@Ni_(x)Co_(1-x)(OH)_(2)(CF@NiCo)photocatalysts.The combined experimental and theoretical investigation demonstrates that incorporating an appropriate amount of Co into Ni(OH)_(2)not only modulates the energy band structure of Ni_(x)Co_(1-x)(OH)_(2),balances the electron-and hole-trapping abilities of the bifunctional cocatalyst and maximizes the charge separation efficiency of the heterojunction,but also regulates the d-band center of Ni_(x)Co_(1-x)(OH)_(2),reinforcing the adsorption and activation of CO_(2)and H_(2)O on the cocatalyst surface and lowering the rate-limiting barriers in the CO_(2)-to-CO and H_(2)O-to-O_(2)conversion.Benefiting from the Ni-Co synergy,the redox reactions proceed stoichiometrically.The optimized CF@Ni_(0.75)Co_(0.25)achieves CO and O_(2)yields of 552.7 and 313.0μmol gcat^(-1)h^(-1),respectively,11.3/9.9,1.6/1.7,and 4.5/5.9-fold higher than those of CF,CF@Ni,and CF@Co.This study offers valuable insights into the design of bifunctional noble-metal-free cocatalysts for high-performance artificial photosynthesis.
基金supported by the National Key R&D Program of China (No.2017YFC0210303).
文摘The expandable graphite(EG)modified TiO_(2) nanocomposites were prepared by the high shearmethod using the TiO_(2) nanoparticles(NPs)and EG as precursors,in which the amount of EG doped in TiO_(2) was 10 wt.%.Followed by the impregnation method,adjusting the pH of the solution to 10,and using the electrostatic adsorption to achieve spatial confinement,the Pt elementswere mainly distributed on the exposed TiO_(2),thus generating the Pt/10EG-TiO_(2)-10 catalyst.The best CO oxidation activity with the excellent resistance to H_(2)O and SO_(2) was obtained over the Pt/10EG-TiO_(2)-10 catalyst:CO conversion after 36 hr of the reaction was ca.85%under the harsh condition of 10 vol.%H_(2)O and 100 ppm SO_(2) at a high gaseous hourly space velocity(GHSV)of 400,000 hr−1.Physicochemical properties of the catalystswere characterized by various techniques.The results showed that the electrostatic adsorption,which riveted the Pt elements mainly on the exposed TiO_(2) of the support surface,reduced the dispersion of Pt NPs on EG and achieved the effective dispersion of Pt NPs,hence significantly improving CO oxidation activity over the Pt/10EG-TiO_(2)-10 catalyst.The 10 wt.%EG doped in TiO_(2) caused the TiO_(2) support to form a more hydrophobic surface,which reduced the adsorption of H_(2)O and SO_(2) on the catalyst,greatly inhibited deposition of the TiOSO_(4) and formation of the PtSO4 species as well as suppressed the oxidation of SO_(2),thus resulting in an improvement in the resistance to H_(2)O and SO_(2) of the Pt/10EG-TiO_(2)-10 catalyst.
基金National Natural Science Foundation of China (50432020)Henan Innovation Project for University Prominent Re- search Talents (2007KYCX008)+3 种基金Henan Education Department Science and Technology Project (2007430004)Henan Plan Project for College Youth Backbone TeacherHenan University of Science and Technology Major Pre-research Foundation (2005ZD003)Henan University of Science and Technology Personnel Scientific Research Foundation (of023)
文摘Two Al2O3/Cu composites containing 0.24 wt.% Al2O3 and 0.60 wt.% Al2O3 separately are prepared by internal oxidation. Effects of sliding speed and pressure on the frictional characteristics of the composites and copper against brass are investigated and compared. The changes in morphology of the sliding surface and subsurface are examined with scanning electron microscope （SEM） and energy dispersive X-ray spectrum （EDS）. The results show that the wear resistance of the Al2O3/Cu composites is superior to that of copper under the same conditions, Under a given electrical current, the wear rate of Al2O3/Cu composites decreases as the Al2O3-content increases, However, the wear rates of the Al2O3/Cu composites and copper increase as the sliding speed and pressure increase under dry sliding condition. The main wear mechanisms for Al2O3/Cu composites are of abrasion and adhesion; for copper, it is adhesion, although wear by oxidation and electrical erosion can also be observed as the speed and pressure rise.
基金Project (2006BAB02B05-04- 01/02) supported by the National Key Technologies R&D Program of China
文摘α-Bi2O3 powders were prepared from nanometer Bi powders through low-temperature oxidation at less than 873.15 K. XRD, SEM, TEM and HRTEM were used to characterize the structure and morphology of Bi powders and Bi2O3 particles. Kinetic studies on the bismuth oxidation at low-temperatures were carried out by TGA method. The results show that bismuth beads should be reunited and oxidized to become irregular Bi2O3 powders. The bismuth oxidation follows shrinking core model, and its controlling mechanism varies at different reaction time. Within 0-10 min, the kinetics is controlled by chemical reaction, after that it is controlled by O2 diffusion in the solid α-Bi2O3 layer. The apparent activation energy is determined as 55.19 kJ/mol in liquid-phase oxidation.
基金supported by the National Natural Science Foundation of China(No.21805018)by Sichuan Science and Technology Program(Nos.2022ZHCG0018,2023NSFSC0117 and 2023ZHCG0060)Yibin Science and Technology Program(No.2022JB005)and China Postdoctoral Science Foundation(No.2022M722704).
文摘Layered transition metal oxides have emerged as promising cathode materials for sodium ion batteries.However,irreversible phase transitions cause structural distortion and cation rearrangement,leading to sluggish Na+dynamics and rapid capacity decay.In this study,we propose a medium-entropy cathode by simultaneously introducing Fe,Mg,and Li dopants into a typical P2-type Na_(0.75)Ni_(0.25)Mn_(0.75)O_(2)cathode.The modified Na_(0.75)Ni_(0.2125)Mn_(0.6375)Fe_(0.05)Mg_(0.05)Li_(0.05)O_(2)cathode predominantly exhibits a main P2 phase(93.5%)with a minor O3 phase(6.5%).Through spectroscopy techniques and electrochemical investigations,we elucidate the redox mechanisms of Ni^(2+/3+/4+),Mn^(3+/4+),Fe^(3+/4+),and O_(2)-/O_(2)^(n-)during charging/discharging.The medium-entropy doping mitigates the detrimental P2-O_(2)phase transition at high-voltage,replacing it with a moderate and reversible structural evolution(P2-OP4),thereby enhancing structural stability.Consequently,the modified cathode exhibits a remarkable rate capacity of 108.4 mAh·g^(-1)at 10C,with a capacity retention of 99.0%after 200 cycles at 1C,82.5%after 500 cycles at 5C,and 76.7%after 600 cycles at 10C.Furthermore,it also demonstrates superior electrochemical performance at high cutoff voltage of 4.5 V and extreme temperature(55 and 0℃).This work offers solutions to critical challenges in sodium ion batteries cathode materials.
基金Project(GC13A113)supported by the Technology Research and Development Program of Heilongjiang Provincial Science and Technology DepartmentProject(12511469)supported by Heilongjiang Provincial Science and Technology Department
文摘Ni-La2O3/CeO2 composite films were prepared by electrodeposition from a nickel sulfate bath containing certain content of micrometer and nanometer La2O3/CeO2 particles. The effect of La2O3 or CeO2 particle size on the oxidation resistance of the electrodeposited Ni-La2O3/CeO2 composites in air at 1000 °C was studied. The results indicate that, compared with the electrodeposited Ni-film, Ni-La2O3/CeO2 composites exhibit a superior oxidation resistance due to the codeposited La2O3 or CeO2 particles blocking the outward diffusion of nickel. Moreover, compared with nanoparticles, La2O3 or CeO2 microparticles have stronger effect because La2O3 or CeO2 microparticles also act as a diffusion barrier layer at the onset of oxidation.
基金Projects (50771009, 50731001 and 51071013) supported by the National Natural Science Foundations of China Project (2010CB631200) supported by the National Basic Research Program of China
文摘3Gd2O3-3Yb2O3-4Y2O3 （mole fraction, %） co-doped ZrO2 （GY-YSZ） thermal barrier coatings （TBCs） were produced by electron beam physical vapor deposition （EB-PVD）. The oxidation behavior of GY-YSZ at 1 050 ℃ was investigated using impedance spectroscopy （IS） combined with scanning electron microscopy （SEM）, Raman spectroscopy and X-ray diffractometry （XRD）. Various electrical responses observed in the impedance spectra corresponding to GY-YSZ grains and grain boundaries were explained using circuit modeling. The change in the conduction mechanism of GY-YSZ was found to be related to the O^2- vacancy and lattice distortion due to the stabilizer diffusion during the oxidation. The results also suggested that the specific oxidation information about the GY-YSZ grains and grain boundaries should be acquired at a moderate measurement temperature, which was related to the resistance value in the impedance spectra. The resistance values of the GY-YSZ grains and grain boundaries should be measured at 200 ℃ and 300 ℃, respectively.
基金Project (50771021) supported by the National Natural Science Foundation of China
文摘Al2O3/Au nano-laminated composite coatings were prepared by means of magnetron sputtering. The coating was compact and comprised of nano-laminated Al2O3 and Au layers. High temperature cyclic oxidation test was employed to investigate the oxidation resistance of the composite coatings. The results revealed that the applied Al2O3/Au nano-laminated composite coatings improved the oxidation and spallation resistance of the stainless steel substrate significantly. The mechanism accounting for oxidation resistance was related with the suppression of inward oxygen diffusion and selective oxidation of Cr in the substrate. The mechanism accounting for spallation resistance was attributed to the relaxation of thermal stress by the nano-laminated structure.
基金financially supported by the National Natural Science Foundation of China(21173195)~~
文摘A series of K-promoted Pt/Al2O3 catalysts were tested for CO oxidation. It was found that the addition of K significantly enhanced the activity. A detailed kinetic study showed that the activation energies of the K-containing catalysts were lower than those of the K-free ones, particularly for catalysts with high Pt contents （51.6 k）/mol for 0.42K-2.0Pt/Al2O3 and 6：3.6 kJ/mol for 2.0Pt/Al2O3 ）. The CO reaction orders were higher for the K-containing catalysts （about -0.2） than for the K-free ones （about -0.5）, with the former having much lower equilibrium constants for CO adsorption than the latter. In situ Fourier-transform infrared spectroscopy showed that surface CO desorption from the 0.42K-2.0Pt/Al2O3 catalyst was easier than from 2.0Pt/Al2O3. The promoting effect of K was therefore caused by weakening of the interactions between CO and surface Pt atoms. This decreased coverage of the catalyst with CO and facilitated competitive O2 chemisorption on the Pt surface, and significantly lowered the reaction barrier between chemisorbed CO and O2 species.
基金supported by the Scientific Funds for Outstanding Young Scientists of China(No.50525619)the National Natural Science Foundation of China(No.51078163,50706014)the National High Technology Research and Development Program(863)of China(No.2006AA05Z304)
文摘Heterogeneous oxidation of gas-phase Hg 0 by nano-Fe 2 O 3 was investigated on a fixed bed reactor, and the effects of oxygen concentration, bed temperature, water vapour concentration and particle size have been discussed. The results showed that Hg 0 could be oxidized by active oxygen atom on the surface of nano-Fe 2 O 3 as well as lattice oxygen in nano-Fe 2 O 3 . Among the factors that affect Hg 0 oxidation by nano-Fe 2 O 3 , bed temperature plays an important role. More than 40% of total mercury was oxidized at 300°C, however, the test temperature at 400°C could cause sintering of nano-catalyst, which led to a lower efficiency of Hg 0 oxidation. The increase of oxygen concentration could promote mercury oxidation and led to higher Hg 0 oxidation efficiency. No obvious mercury oxidation was detected in the pure N 2 atmosphere, which indicates that oxygen is required in the gas stream for mercury oxidation. The presence of water vapour showed different effects on mercury oxidation depending on its concentration. The lower content of water vapour could promote mercury oxidation, while the higher content of water vapour inhibits mercury oxidation.
基金supported by the National Key Research and Development Program of China (No. 2017YFC0703200)
文摘Large amounts of cyanide tailings are produced during the cyanidation process in gold extraction,which are hazardous solid wastes due to the toxic cyanide.Pyrite is one of the main minerals in cyanide tailings.The removal of cyanide adsorbed on pyrite by H_2O_2 oxidation under alkaline conditions was investigated in this study.It was found that the removal efficiency was positively correlated with pH from 5 to 12,but remained almost constant when pH was higher than 12.The highest cyanide removal efficiency of 91.10% was achieved by adding no less than 0.6 wt.% of H_2O_2.Cyanide removal was positively correlated with the CN^-adsorption amount between 1.06 and 8.5 mg/g,and temperature between 25 and 85°C.The removal of cyanide adsorbed on pyrite by H_2O_2 oxidation under alkaline conditions was due to the oxidation of pyrite.Hexacyanoferrate,thiocyanate and sulfate were generated with mole ratios of about 2.03:1.12:3.17 during the cyanide removal.?2018 The Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences.
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financially supported by the National Natural Science Foundation of China (Nos. 51708078 and 41801063)the Natural Science Foundation of Chongqing (No. 2018jcyjA1040)
文摘The BiOCl/Bi12O17Cl2@MoS2(BOC-MS)composites were successfully synthesized by a facile method at room temperature.The physicochemical properties of the as-obtained samples were characterized by X-ray diffractometer(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray photoelectron spectroscopy(XPS),ultraviolet–visible diffuse reflection spectra(UV–Vis DRS),photoluminescence(PL),Brunauer–Emmett–Teller–Barrett–Joyner–Halenda(BET–BJH),and electron spin resonance(ESR)in detail.Moreover,the in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)was applied to elucidate the adsorption and photocatalytic reaction mechanism.The optimized BOC-MS-1.0 composites exhibited excellent visible light photocatalytic capability(51.1%)and photochemical stability for removal of NO.Based on the DMPOESR spin trapping,the·O2-radicals andáOH radicals were identified as the main active species generated from BOCMS-1.0 under visible light irradiation.The enhanced photocatalytic performance can be ascribed to the positive synergetic effect of the MoS2 and the effective carrier separation ability.
文摘A wet catalytic oxidation at room temperature was investigated with solution containing ferric, ferrous and cupric ions for H2S removal. The experiments were carried out in a two step process, and the results obtained show that the removal efficiency of H2S can always reach 100% in a 300 mm scrubbing column with four sieve plates, and the regeneration of ferric ions in 200 mm bubble column can match the consumed ferric species in absorption. Removal of H2S, production of elemental sulfur and regeneration of ferric, cupric ions can all be accomplished at the same time. No raw material is consumed except O2 in flue gas or air, the process has no secondary pollution and no problem of catalyst degradation and congestion.
基金the National Natural Science Foundation of China (50574046)National Natural Science Foundation of Major Research Projects (90610035)+1 种基金Natural Science Foundation of Yunnan Province (2004E0058Q)High School Doctoral Subject Special Science and Re- search Foundation of Ministry of Education (20040674005)
文摘A series of Ce1-xFexO2 （x=0, 0.2, 0.4, 0.6, 0.8, 1） complex oxide catalysts were prepared using the coprecipitation method. The catalysts were characterized by means of XRD and H2-TPR. The reactions between methane and lattice oxygen from the complex oxides were investigated. The characteristic results revealed that the combination of Ce and Fe oxide in the catalysts could lower the temperature necessary to reduce the cerium oxide. The catalytic activity for selective CH4 oxidation was strongly influenced by dropped Fe species. Adding the appropriate amount of Fe2O3 to CeO2 could promote the action between CH4 and CeO2. Dispersed Fe2O3 first returned to the original state and would then virtually form the Fe species on the catalyst, which could be considered as the active site for selective CH4 oxidation. The appearance of carbon formation was significant and the oxidation of carbon appeared to be the rate-determining step; the amounts of surface reducible oxygen species in CeO2 were also relevant to the activity. Among all the catalysts, Ce0.6Fe0.402 exhibited the best activity, which converted 94.52% of CH4 at 900 ℃.
基金Foundation items:the National Natural Science Foundation of China(No.20373085)the Natural Science Foundation of Shanxi Province(No.20051023)
文摘The attractive utilization route for one-step catalytic oxidation of dimethyl ether to dimethoxymethane was successfully carried out over the H3PW12O40（40%）/SiO2 catalyst, modified by Cs, K, Ni, and V. The Cs modification of H3PW12O40（40%）/SiO2 gave the most promising result of 20% dimethyl ether conversion and 34.8% dimethoxymethane selectivity. Dimethoxymethane could be synthe- sized via methoxy groups decomposed from dimethyl ether through the synergistic effect between the acid sites and the redox sites of Cs modified H3PW12O40（40%）/SiO2.
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.
