A novel sensor for ocean electric field testing has been fabricated by polyacrylonitrile-based on carbon fibers with electro-chemical oxidation.The surface profile characteristics of the carbon fibers were characteriz...A novel sensor for ocean electric field testing has been fabricated by polyacrylonitrile-based on carbon fibers with electro-chemical oxidation.The surface profile characteristics of the carbon fibers were characterized by scanning electron microscope,Fourier transform infrared spectra and contact angle.Cyclic voltammetry and Tafel curves have been used to study its electro-chemical performances.Two identical electrodes in sea water as the electric field sensor will swiftly respond to applied electric field which causes positive and negative ions to move in opposite direction,resulting in a electric potential difference(ΔE).Test result indicates that the offset potential is typically below 1 m V with a drift of 60-170μVd^-1.Typical self noise level is 1.07 nV√Hz^(1/2)@1 Hz.The electric field response indicates that the modified electrode pair shows better response to AC sine signal of amplitude and frequency(5 mV and 1 mHz)respectively than its blank.The electric field response model of the modified electrodes is creatively presented according to its electric double layer capacitance and Faraday pseudo-capacitance.Many advantages of the carbon fiber electric field electrode will make it have potential application prospect.展开更多
Full concentration gradient lithium-rich layered oxides are catching lots of interest as the next generation cathode for lithium-ion batteries due to their high discharge voltage,reduced voltage decay and enhanced rat...Full concentration gradient lithium-rich layered oxides are catching lots of interest as the next generation cathode for lithium-ion batteries due to their high discharge voltage,reduced voltage decay and enhanced rate performance,whereas the high lithium residues on its surface impairs the structure stability and long-term cycle performance.Herein,a facile multifunctional surface modification method is implemented to eliminate surface lithium residues of full concentration gradient lithium-rich layered oxides by a wet chemistry reaction with tetrabutyl titanate and the post-annealing process.It realizes not only a stable Li_(2)TiO_(3)coating layer with 3D diffusion channels for fast Li^(+)ions transfer,but also dopes partial Ti^(4+)ions into the sub-surface region of full concentration gradient lithium-rich layered oxides to further strengthen its crystal structure.Consequently,the modified full concentration gradient lithium-rich layered oxides exhibit improved structure stability,elevated thermal stability with decomposition temperature from 289.57℃to 321.72℃,and enhanced cycle performance(205.1 mAh g^(-1)after 150 cycles)with slowed voltage drop(1.67 mV per cycle).This work proposes a facile and integrated modification method to enhance the comprehensive performance of full concentration gradient lithium-rich layered oxides,which can facilitate its practical application for developing higher energy density lithium-ion batteries.展开更多
The hot dipping process of pure aluminum on H13 steel substrates followed by plasma electrolytic oxidation(PEO) was studied to form alumina ceramic coatings for protective purpose.H13 steel bars were first dipped in p...The hot dipping process of pure aluminum on H13 steel substrates followed by plasma electrolytic oxidation(PEO) was studied to form alumina ceramic coatings for protective purpose.H13 steel bars were first dipped in pure aluminum melts,and then,a reactive iron-aluminum intermetallic layer grew at the interface between the melt and the steel substrate.The reactive layer was mainly composed of intermetallic Fe-Al(Fe_2Al_5);the thickness of aluminum layer and Fe-Al intermetallic layer were mainly influenced by dipping time(1.5~12.0 min) and dipping temperature(710~760 ℃).After PEO process,uniform Al_2O_3 ceramic coatings were deposited on the surface of aluminized steel.The element distribution,phase composition and morphology of the aluminized layer,and the ceramic coatings were characterized by SEM/EDS and XRD.The distribution of hardness across the composite coating is demonstrated,and the maximum value reaches 1864 HV.The thermal shock resistance of the coated sample is also well improved.展开更多
In this study, compounded surface modification technology-high current pulsed electron beam (HCPEB) + micro-plasma oxidation (MPO) was applied to treat ZK60 Mg alloys. The characteristics of the microstructure of...In this study, compounded surface modification technology-high current pulsed electron beam (HCPEB) + micro-plasma oxidation (MPO) was applied to treat ZK60 Mg alloys. The characteristics of the microstructure of ZK60 Mg alloy after single MPO and HCPEB+MPO compounded treatment were investigated by SEM. The results showed that the density of the ceramic layer of HCPEB+MPO-treated ZK60 Mg alloy was improved and defects were reduced compared to that under MPO treatment alone. Surface modified layer of ZK60 Mg alloys treated by HCPEB+MPO was divided into three zones, namely the top loose ceramic zone, middle compact zone and inside HCPEB-induced melted zone. Corrosion resistance of ZK60 Mg alloy before and after the compounded surface modification was measured in a solution of 3.5% NaCl by potentiodynamic polarization curves. It was found that the corrosion current density of ZK60 Mg alloys could be reduced by about three orders of magnitude, from 311μA/cm^2 of the original sample to 0.2μA/cm^2 of the HCPEB+MPO-treated sample. This indicates the great application potential of the HCPEB+MPO compounded surface modification technology in improving the corrosion resistance of ZK60 Mg alloys in the future.展开更多
Glycerol(electrochemical) oxidation reaction(GOR) producing organic small molecule acid and coupling with hydrogen evolution reaction is a critical aspect of ensuring balanced glycerol capacity and promoting hydrogen ...Glycerol(electrochemical) oxidation reaction(GOR) producing organic small molecule acid and coupling with hydrogen evolution reaction is a critical aspect of ensuring balanced glycerol capacity and promoting hydrogen generation on a large scale. However, the development of highly efficient and selective non-noble metal-based GOR electrocatalysts is still a key problem. Here, an S-doped CuO nanorod array catalyst(S-CuO/CF) constructed by sulfur leaching and oxidative remodeling is used to drive GOR at low potentials: It requires potentials of only 1.23 and 1.33 V versus RHE to provide currents of 100 and 500 mA cm^(-2), respectively. Moreover, it shows satisfactory comprehensive performance(at 100 mA cm^(-2), V_(cell) = 1.37 V) when assembled as the anode in asymmetric coupled electrolytic cell. Furthermore, we propose a detailed cycle reaction pathway(in alkaline environment) of S-doped CuO surface promoting GOR to produce formic acid and glycolic acid. Among them, the C–C bond breaking and lattice oxygen deintercalation steps frequently involved in the reaction pathway are the key factors to determine the catalytic performance and product selectivity. This research provides valuable guidance for the development of transition metal-based electrocatalysts for GOR and valuable insights into the glycerol oxidation cycle reaction pathway.展开更多
Al2O3 ceramic powder was applied to modify the large pores defects on the surface of the porous metal Ti support,in situ oxidation method was a convenient method to prepare defect free ceramic/Ti composite membranes o...Al2O3 ceramic powder was applied to modify the large pores defects on the surface of the porous metal Ti support,in situ oxidation method was a convenient method to prepare defect free ceramic/Ti composite membranes on this basis.In situ oxidation conditions experimental results show that the best condition for preparing the TiO2-Al2O3/Ti composite membrane is under 800°C for 2 h,and the microstructure and pore sizes of the TiO2-Al2O3/Ti composite membranes are affected obviously.The thickness and composition of the TiO2/Ti composite membranes are determined by SEM and XRD completely.The pore size distribution of the composite membrane is measured by bubble pressure method,the most probable aperture is about 3.12μm,while the average pore size of defect free TiO2-Al2O3/Ti is about 3.23μm.After ultrasonic treatment,the slight weight change of membranes reveals no observable change,which indicates that TiO2-Al2O3/Ti composite membranes maintain a good stability.展开更多
The effects of mixed rare earth oxides and CaCO3 on the microstructure of an in-situ Mg2Si/Al-Si hypereutectic alloy composite were investigated by optical microscope,scanning electron microscope,and energy dispersive...The effects of mixed rare earth oxides and CaCO3 on the microstructure of an in-situ Mg2Si/Al-Si hypereutectic alloy composite were investigated by optical microscope,scanning electron microscope,and energy dispersive spectrum analysis. The results showed that the morphol-ogy of the primary Mg2Si phase particles changed from irregular or crosses to polygonal shape,their sizes decreased from 75 μm to about 25 μm,and the compound of both the oxide and CaCO3 was better than either the single mixed rare earth o...展开更多
Intracellular reactive oxygen species (ROS) are known to regulate apoptosis. Activation of caspase-9, the initial caspase in the mitochondrial apoptotic cascade, is closely associated with ROS, but it is unclear whe...Intracellular reactive oxygen species (ROS) are known to regulate apoptosis. Activation of caspase-9, the initial caspase in the mitochondrial apoptotic cascade, is closely associated with ROS, but it is unclear whether ROS regulate caspase-9 via direct oxidative modification. The present study aims to elucidate the molecular mechanisms by which ROS mediate caspase-9 activation. Our results show that the cellular oxidative state facilitates caspase-9 activation. Hydrogen peroxide treatment causes the activation of caspase-9 and apoptosis, and promotes an interac- tion between easpase-9 and apoptotic protease-activating factor 1 (Apaf-1) via disulfide formation. In addition, in an in vitro mitochondria-free system, the thiol-oxidant diamide promotes auto-cleavage of caspase-9 and the caspase-9/ Apaf-1 interaction by facilitating the formation of disulfide-linked complexes. Finally, a point mutation at C403 of caspase-9 impairs both H2O2-promoted caspase-9 activation and interaction with Apaf-1 through the abolition of disulfide formation. The association between cytochrome c and the C403S mutant is significantly weaker than that between cytochrome c and wild-type caspase-9, indicating that oxidative modification of caspase-9 contributes to apoptosome formation under oxidative stress. Taken together, oxidative modification of caspase-9 by ROS can medi- ate its interaction with Apaf-1, and can thus promote its auto-cleavage and activation. This mechanism may facilitate apoptosome formation and caspase-9 activation under oxidative stress.展开更多
The activity and thermal stability of Pd/Al2O3 and Pd/(Al2O3+MOx) (M=Ca, La, Ce) palladium catalysts in the reaction of complete oxidation of methane are presented in this study. The catalyst supports were prepar...The activity and thermal stability of Pd/Al2O3 and Pd/(Al2O3+MOx) (M=Ca, La, Ce) palladium catalysts in the reaction of complete oxidation of methane are presented in this study. The catalyst supports were prepared by sol-gel method and they were dried either conventionally or with supercritical carbon dioxide. Then they were impregnated with palladium nitrate solution. The catalysts with unmodified alumina had a high surface area. The activity and thermal stability of the aluminasupported catalyst was also very high. The introduction of calcium, lanthanum, or cerium oxide into alumina support caused a decrease of the surface area in the way dependent on the support precursor drying method. These modifiers decreased the activity of palladium catalysts, and they required higher temperatures for the complete oxidation of methane than unmodified Pd/Al2O3. The improvement of the palladium activity by lanthanum and cerium support modifier was observed only at low temperatures of the reaction.展开更多
A hollow-fiber-supported stable Au/FAU catalytic membrane was successfully synthesized through a polydopamine coating modification-removal strategy and used as a flow-through catalytic membrane reactor for preferentia...A hollow-fiber-supported stable Au/FAU catalytic membrane was successfully synthesized through a polydopamine coating modification-removal strategy and used as a flow-through catalytic membrane reactor for preferential oxidation of CO.Small Au nanoparticles can be efficiently isolated by dopamine and the dopamine-derived carbon shells.The interactions between Au nanoparticles and zeolite layer support are enhanced during annealing at high temperature under an inert atmosphere.A zeolite membrane supported Au nanoparticle catalyst was obtained after the removal of carbon shells,which showed high catalytic activity and stability for the removal of CO from hydrogen.展开更多
Y-Modified USY was prepared by ion exchange of USY slurry with 0.01 mol·L-1 Y(NO3)3. Phosphotungstic acid (HPW) catalyst supported on USY and Y-USY was prepared by an impregnation method. The materials were chara...Y-Modified USY was prepared by ion exchange of USY slurry with 0.01 mol·L-1 Y(NO3)3. Phosphotungstic acid (HPW) catalyst supported on USY and Y-USY was prepared by an impregnation method. The materials were characterized by NH3-TPD, XRD, and N2 adsorption. The activity for the removal of thiophene was examined in a three-necked flask. The sulfur content of model compound was tested on WK-2D microcoulometric detector. The effect of yttrium and HPW content, reaction temperature and catalysts, activation temperature on the activity of catalysts were investigated. It was shown that the oxidation activity of thiophene decreased with the increase of Y content except for the catalyst of Y 5%. HPW content had limit influence on activity of catalysts. The optimal reaction temperature and activation temperature were 40 and 320 ℃, respectively.展开更多
Study was made on the effect of surface modification on the behaviors of cerium oxide nanopowders.A surfactant-sodium dodecyl sulfate(C12H25SO4Na)was used to modify the surface of CeO2 powder particles.The unmodifie...Study was made on the effect of surface modification on the behaviors of cerium oxide nanopowders.A surfactant-sodium dodecyl sulfate(C12H25SO4Na)was used to modify the surface of CeO2 powder particles.The unmodified and modified CeO2 powders were characterized by using a powder comprehensive characteristic tester,laser particle size analyzer,specific surface area tester,X-ray diffraction tester,and a scanning electron microscope.The testing and analysis results showed that C12H25SO4Na surface modification might increase the flowability and dispersity,and decrease the specific surface area and agglomeration of CeO2 powders.The mechanism of the surface modification of CeO2 powder particles was also discussed.展开更多
Nickel-rich layered oxides have been identified as the most promising commercial cathode materials for lithium-ion batteries(LIBs)for their high theoretical specific capacity.However,the poor cycling stability of nick...Nickel-rich layered oxides have been identified as the most promising commercial cathode materials for lithium-ion batteries(LIBs)for their high theoretical specific capacity.However,the poor cycling stability of nickel-rich cathode materials is one of the major barriers for the large-scale usage of LIBs.The existing obstructions that suppress the capacity degradation of nickel-rich cathode materials are as a result of phase transition,mechanical instability,intergranular cracks,side reaction,oxygen loss,and thermal instability during cycling.Core–shell structures,oxidating precursors,electrolyte additives,doping/coating and synthesizing single crystals have been identified as effective methods to improve cycling stability of nickel-rich cathode materials.Herein,recent progress of surface modification,e.g.coating and doping,in nickel-rich cathode materials are summarized based on Periodic table to provide a clear understanding.Electrochemical performances and mechanisms of modified structure are discussed in detail.It is hoped that an overview of synthesis and surface modification can be presented and a perspective of nickel-rich materials in LIBs can be given.展开更多
Mn_2O_3-Na_2WO_4/SiO_2 is considered as the most promising catalyst for the oxidative coupling of methane(OCM) process; however, it only has a better catalytic performance over 800 °C. To improve its low-temper...Mn_2O_3-Na_2WO_4/SiO_2 is considered as the most promising catalyst for the oxidative coupling of methane(OCM) process; however, it only has a better catalytic performance over 800 °C. To improve its low-temperature performance, an attempt has been made to modify the Mn_2O_3-Na_2WO_4/SiO_2 catalyst using TiO_2, MgO, Ga_2O_3, and ZrO_2. Among the synthesized catalysts, the TiO_2-modified Mn_2O_3-Na_2WO_4/SiO_2 catalyst shows markedly improved low-temperature OCM performance,achieving a high CH_4 conversion of ~23% and a good C_2-C_3 selectivity of ~73% at 700 °C(the catalyst bed temperature), along with promising stability for at least 300 h without signs of deactivation.In comparison with the unmodified Mn_2O_3-Na_2WO_4/SiO_2 catalyst, the TiO_2 modification results in significant improvement in the low-temperature activity/selectivity, whereas the MgO modification has almost no impact and the Ga_2O_3 and ZrO_2 modifications have a negative effect. The X-ray diffraction(XRD) and Raman results reveal that the formation of a MnTiO_3 phase and a MnTiO_3-dominated catalyst surface is crucial for the improvement of the low-temperature activity/selectivity in the OCM process.展开更多
Carbon modified TiO_2 nanobelts(TiO_2-C) were synthesized using a hydrothermal growth method,as a support material for palladium(Pd) nanoparticles(Pd/TiO_2-C) to improve the electrocatalytic performance for methanol e...Carbon modified TiO_2 nanobelts(TiO_2-C) were synthesized using a hydrothermal growth method,as a support material for palladium(Pd) nanoparticles(Pd/TiO_2-C) to improve the electrocatalytic performance for methanol electrooxidation by comparison to Pd nanoparticles on bare TiO_2 nanobelts(Pd/TiO_2)and activated carbon(Pd/AC). Cyclic voltammetry characterization was conducted with respect to saturated calomel electrode(SCE) in an alkaline methanol solution, and the results indicate that the specific activity of Pd/TiO_2-C is 2.2 times that of Pd/AC and 1.5 times that of Pd/TiO_2. Chronoamperometry results revealed that the TiO_2-C support was comparable in stability to activated carbon, but possesses an enhanced current density for methanol oxidation at a potential of -0.2 V vs. SCE. The current study demonstrates the potential of Pd nanoparticle loaded on hierarchical TiO_2-C nanobelts for electrocatalytic applications such as fuel cells and batteries.展开更多
The properties of poly(3-hexylthiophene):(6,6)-phenyl C61 butyric acid methyl ester (P3HT:PCBM) organic pho- tovoltaic devices (OPVs) with an indium tin oxide (ITO) anode treated by a KMnO4 solution are in...The properties of poly(3-hexylthiophene):(6,6)-phenyl C61 butyric acid methyl ester (P3HT:PCBM) organic pho- tovoltaic devices (OPVs) with an indium tin oxide (ITO) anode treated by a KMnO4 solution are investigated. The optimized KMnO4 solution has a concentration of 50 rag/L, and ITO is treated for 15 min. The modification of ITO anode results in an enhancement of the power conversion efficiency (PCE) of the device, which is responsible for the increase of the photocurrent. The performance enhancement is attributed to the work function modification of the ITO substrate through the strong oxygenation of KMnO4, and then the charge collection efficiency is improved.展开更多
The surface modification of metal oxides using organic modifiers is a potential strategy for enhancing their catalytic performances.In this study,a hydrophobic surface amine-modified CoO catalyst with a water contact ...The surface modification of metal oxides using organic modifiers is a potential strategy for enhancing their catalytic performances.In this study,a hydrophobic surface amine-modified CoO catalyst with a water contact angle of 143°was fabricated.The catalyst was characterized by XRD,TGA,FT-IR,HR-TEM,and XPS.The results showed that the fabricated catalyst performed better than the hydrophilic commercial CoO nanoparticle in the process of aromatic hydrocarbon oxidation.After the amines modification,commercial CoO also became hydrophobic and improved conversion of ethylbenzene was achieved.The surface modification of CoO with amines induced the hydrophobicity property,which could serve as a reference for the design of other hydrophobic catalysts.展开更多
Asymmetrically modified Janus graphene oxide(JGO)has attracted great attention due to its unique physical chemistry properties and wide applications.The modification degree of Janus nanosheets inevitably affects their...Asymmetrically modified Janus graphene oxide(JGO)has attracted great attention due to its unique physical chemistry properties and wide applications.The modification degree of Janus nanosheets inevitably affects their interfacial activity,which is essential for their performances in enhanced oil recovery(EOR).In this study,the interfacial properties of Janus graphene oxide(JGO)with various modification degrees at liquid-liquid and liquid-solid interfaces were systematically evaluated via the measurements of interfacial tension(IFT),dilatational modulus,contact angle,and EOR efficiency was further assessed by core flooding tests.It is found that JGO-5 with higher modification degree exhibits the greater ability to reduce IFT(15.16 mN/m)and dilatational modulus(26 mN/m).Furthermore,JGO can construct interfacial and climbing film with the assistance of hydrodynamic power to effectively detach the oil from the rock surface and greatly enhance oil recovery.Moderately modified JGO-2 can highly improve recovery of residual crude oil(11.53%),which is regarded as the promising EOR agent in practical application.The present study firstly focuses on the effects of modification degrees on the JGO interfacial properties and proposes diverse EOR mechanisms for JGO with different modification degrees.展开更多
Mesoporous TiO2 (m-TiO2) nanoparticles were used to prepare the porous film electrodes for dye-sensitized solar cells, and a second metal oxide (MgO, ZnO, A1203, or NiO) modifi- cation was carried out by dipping t...Mesoporous TiO2 (m-TiO2) nanoparticles were used to prepare the porous film electrodes for dye-sensitized solar cells, and a second metal oxide (MgO, ZnO, A1203, or NiO) modifi- cation was carried out by dipping the m-TiO2 electrode into their respective nitrate solution followed by annealing at 500 ℃. Experimental results indicated that the above second metal oxide modifications on m-TiO2 electrode are shown in all cases to act as barrier layer for the interracial charge transfer processes, but film electron transport and interfacial charge recombination characteristics under applied bias voltage were dependent significantly on the existing states and kinds of these second metal oxides. Those changes based on sec- ond metal oxide modifications showed good correlation with the current-voltage analyses of dye-sensitized solar cell, and all modifications were found to increase the open-circuit photo- voltage in various degrees, while the MgO, ZnO, and NiO modifications result in 23%, 13%, and 6% improvement in cell conversion efficiency, respectively. The above observations indi- cate that controlling the charge transport and recombination is very important to improve the photovoltaic performance of TiO2-based solar cell.展开更多
In this paper, the superhydrophobic polyurethane sponge(SS-PU) was facilely fabricated by etching with Jones reagent to bind the nanoparticles of Ni-Co double layered oxides(LDOs) on the surface, and following modific...In this paper, the superhydrophobic polyurethane sponge(SS-PU) was facilely fabricated by etching with Jones reagent to bind the nanoparticles of Ni-Co double layered oxides(LDOs) on the surface, and following modification with n-dodecyl mercaptan(DDT). This method provides a new strategy to fabricate superhydrophobic PU sponge with a water contact angle of 157° for absorbing oil with low cost and in large scale. It exhibits the strong absorption capacity and highly selective characteristic for various kinds of oils which can be recycled by simple squeezing. Besides, the as-prepared sponge can deal with the floating and underwater oils, indicating its application value in handling oil spills and domestic oily wastewater. The good self-cleaning ability shows the potential to clear the pollutants due to the ultralow adhesion to water. Especially, the most important point is that the superhydrophobic sponge can continuously and effectively separate the oil/water mixture against the condition of turbulent disturbance by using our designed device system, which exhibit its good superhydrophobicity, strong stability.Furthermore, the SS-PU still maintained stable absorption performance after 150 cycle tests without losing capacity obviously, showing excellent durability in long-term operation and significant potential as an efficient absorbent in large-scale dispose of oily water.展开更多
基金supported by the National Defense Science and Technology Innovation Zone Project(No.18-H863-05-ZT-001-018-09)
文摘A novel sensor for ocean electric field testing has been fabricated by polyacrylonitrile-based on carbon fibers with electro-chemical oxidation.The surface profile characteristics of the carbon fibers were characterized by scanning electron microscope,Fourier transform infrared spectra and contact angle.Cyclic voltammetry and Tafel curves have been used to study its electro-chemical performances.Two identical electrodes in sea water as the electric field sensor will swiftly respond to applied electric field which causes positive and negative ions to move in opposite direction,resulting in a electric potential difference(ΔE).Test result indicates that the offset potential is typically below 1 m V with a drift of 60-170μVd^-1.Typical self noise level is 1.07 nV√Hz^(1/2)@1 Hz.The electric field response indicates that the modified electrode pair shows better response to AC sine signal of amplitude and frequency(5 mV and 1 mHz)respectively than its blank.The electric field response model of the modified electrodes is creatively presented according to its electric double layer capacitance and Faraday pseudo-capacitance.Many advantages of the carbon fiber electric field electrode will make it have potential application prospect.
基金financially supported by the Natural Science Foundation of Shandong Province(ZR2022QB166,ZR2020KE032)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA22010600)+3 种基金the Youth Innovation Promotion Association of CAS(2021210)the Foundation of Qingdao Postdoctoral Application Program(Y63302190F)the Natural Science Foundation of Qingdao Institute ofBioenergy and Bioprocess Technology(QIBEBT SZ202101)support from the Max Planck-POSTECH-Hsinchu Center for Complex Phase Materials
文摘Full concentration gradient lithium-rich layered oxides are catching lots of interest as the next generation cathode for lithium-ion batteries due to their high discharge voltage,reduced voltage decay and enhanced rate performance,whereas the high lithium residues on its surface impairs the structure stability and long-term cycle performance.Herein,a facile multifunctional surface modification method is implemented to eliminate surface lithium residues of full concentration gradient lithium-rich layered oxides by a wet chemistry reaction with tetrabutyl titanate and the post-annealing process.It realizes not only a stable Li_(2)TiO_(3)coating layer with 3D diffusion channels for fast Li^(+)ions transfer,but also dopes partial Ti^(4+)ions into the sub-surface region of full concentration gradient lithium-rich layered oxides to further strengthen its crystal structure.Consequently,the modified full concentration gradient lithium-rich layered oxides exhibit improved structure stability,elevated thermal stability with decomposition temperature from 289.57℃to 321.72℃,and enhanced cycle performance(205.1 mAh g^(-1)after 150 cycles)with slowed voltage drop(1.67 mV per cycle).This work proposes a facile and integrated modification method to enhance the comprehensive performance of full concentration gradient lithium-rich layered oxides,which can facilitate its practical application for developing higher energy density lithium-ion batteries.
基金supported by Natural Science Foundation of Chongqing (No. 2008AA4029)Scientific Research Training Program of Chongqing University
文摘The hot dipping process of pure aluminum on H13 steel substrates followed by plasma electrolytic oxidation(PEO) was studied to form alumina ceramic coatings for protective purpose.H13 steel bars were first dipped in pure aluminum melts,and then,a reactive iron-aluminum intermetallic layer grew at the interface between the melt and the steel substrate.The reactive layer was mainly composed of intermetallic Fe-Al(Fe_2Al_5);the thickness of aluminum layer and Fe-Al intermetallic layer were mainly influenced by dipping time(1.5~12.0 min) and dipping temperature(710~760 ℃).After PEO process,uniform Al_2O_3 ceramic coatings were deposited on the surface of aluminized steel.The element distribution,phase composition and morphology of the aluminized layer,and the ceramic coatings were characterized by SEM/EDS and XRD.The distribution of hardness across the composite coating is demonstrated,and the maximum value reaches 1864 HV.The thermal shock resistance of the coated sample is also well improved.
基金supported by Liaoning BaiQianWan Talents Program of China (No. 2008921028)Doctoral Fund of Ministry of Education of China (No. 200801451082)
文摘In this study, compounded surface modification technology-high current pulsed electron beam (HCPEB) + micro-plasma oxidation (MPO) was applied to treat ZK60 Mg alloys. The characteristics of the microstructure of ZK60 Mg alloy after single MPO and HCPEB+MPO compounded treatment were investigated by SEM. The results showed that the density of the ceramic layer of HCPEB+MPO-treated ZK60 Mg alloy was improved and defects were reduced compared to that under MPO treatment alone. Surface modified layer of ZK60 Mg alloys treated by HCPEB+MPO was divided into three zones, namely the top loose ceramic zone, middle compact zone and inside HCPEB-induced melted zone. Corrosion resistance of ZK60 Mg alloy before and after the compounded surface modification was measured in a solution of 3.5% NaCl by potentiodynamic polarization curves. It was found that the corrosion current density of ZK60 Mg alloys could be reduced by about three orders of magnitude, from 311μA/cm^2 of the original sample to 0.2μA/cm^2 of the HCPEB+MPO-treated sample. This indicates the great application potential of the HCPEB+MPO compounded surface modification technology in improving the corrosion resistance of ZK60 Mg alloys in the future.
基金financially supported by National Natural Science Foundation of China (52174283 and 52274308)。
文摘Glycerol(electrochemical) oxidation reaction(GOR) producing organic small molecule acid and coupling with hydrogen evolution reaction is a critical aspect of ensuring balanced glycerol capacity and promoting hydrogen generation on a large scale. However, the development of highly efficient and selective non-noble metal-based GOR electrocatalysts is still a key problem. Here, an S-doped CuO nanorod array catalyst(S-CuO/CF) constructed by sulfur leaching and oxidative remodeling is used to drive GOR at low potentials: It requires potentials of only 1.23 and 1.33 V versus RHE to provide currents of 100 and 500 mA cm^(-2), respectively. Moreover, it shows satisfactory comprehensive performance(at 100 mA cm^(-2), V_(cell) = 1.37 V) when assembled as the anode in asymmetric coupled electrolytic cell. Furthermore, we propose a detailed cycle reaction pathway(in alkaline environment) of S-doped CuO surface promoting GOR to produce formic acid and glycolic acid. Among them, the C–C bond breaking and lattice oxygen deintercalation steps frequently involved in the reaction pathway are the key factors to determine the catalytic performance and product selectivity. This research provides valuable guidance for the development of transition metal-based electrocatalysts for GOR and valuable insights into the glycerol oxidation cycle reaction pathway.
基金Projects(212006065,21666018)supported by the National Natural Science Foundation of China
文摘Al2O3 ceramic powder was applied to modify the large pores defects on the surface of the porous metal Ti support,in situ oxidation method was a convenient method to prepare defect free ceramic/Ti composite membranes on this basis.In situ oxidation conditions experimental results show that the best condition for preparing the TiO2-Al2O3/Ti composite membrane is under 800°C for 2 h,and the microstructure and pore sizes of the TiO2-Al2O3/Ti composite membranes are affected obviously.The thickness and composition of the TiO2/Ti composite membranes are determined by SEM and XRD completely.The pore size distribution of the composite membrane is measured by bubble pressure method,the most probable aperture is about 3.12μm,while the average pore size of defect free TiO2-Al2O3/Ti is about 3.23μm.After ultrasonic treatment,the slight weight change of membranes reveals no observable change,which indicates that TiO2-Al2O3/Ti composite membranes maintain a good stability.
基金the Natural Science Foundation of Jiangxi Province (No. 0650047)the Science and Technology Program of the Education Department of Jiangxi Province,China(No.GJJ08268).
文摘The effects of mixed rare earth oxides and CaCO3 on the microstructure of an in-situ Mg2Si/Al-Si hypereutectic alloy composite were investigated by optical microscope,scanning electron microscope,and energy dispersive spectrum analysis. The results showed that the morphol-ogy of the primary Mg2Si phase particles changed from irregular or crosses to polygonal shape,their sizes decreased from 75 μm to about 25 μm,and the compound of both the oxide and CaCO3 was better than either the single mixed rare earth o...
文摘Intracellular reactive oxygen species (ROS) are known to regulate apoptosis. Activation of caspase-9, the initial caspase in the mitochondrial apoptotic cascade, is closely associated with ROS, but it is unclear whether ROS regulate caspase-9 via direct oxidative modification. The present study aims to elucidate the molecular mechanisms by which ROS mediate caspase-9 activation. Our results show that the cellular oxidative state facilitates caspase-9 activation. Hydrogen peroxide treatment causes the activation of caspase-9 and apoptosis, and promotes an interac- tion between easpase-9 and apoptotic protease-activating factor 1 (Apaf-1) via disulfide formation. In addition, in an in vitro mitochondria-free system, the thiol-oxidant diamide promotes auto-cleavage of caspase-9 and the caspase-9/ Apaf-1 interaction by facilitating the formation of disulfide-linked complexes. Finally, a point mutation at C403 of caspase-9 impairs both H2O2-promoted caspase-9 activation and interaction with Apaf-1 through the abolition of disulfide formation. The association between cytochrome c and the C403S mutant is significantly weaker than that between cytochrome c and wild-type caspase-9, indicating that oxidative modification of caspase-9 contributes to apoptosome formation under oxidative stress. Taken together, oxidative modification of caspase-9 by ROS can medi- ate its interaction with Apaf-1, and can thus promote its auto-cleavage and activation. This mechanism may facilitate apoptosome formation and caspase-9 activation under oxidative stress.
文摘The activity and thermal stability of Pd/Al2O3 and Pd/(Al2O3+MOx) (M=Ca, La, Ce) palladium catalysts in the reaction of complete oxidation of methane are presented in this study. The catalyst supports were prepared by sol-gel method and they were dried either conventionally or with supercritical carbon dioxide. Then they were impregnated with palladium nitrate solution. The catalysts with unmodified alumina had a high surface area. The activity and thermal stability of the aluminasupported catalyst was also very high. The introduction of calcium, lanthanum, or cerium oxide into alumina support caused a decrease of the surface area in the way dependent on the support precursor drying method. These modifiers decreased the activity of palladium catalysts, and they required higher temperatures for the complete oxidation of methane than unmodified Pd/Al2O3. The improvement of the palladium activity by lanthanum and cerium support modifier was observed only at low temperatures of the reaction.
基金Supported by the National Natural Science Foundation of China(21490585,21606126,21176117)National High-tech Research and Development Program of China(2015AA03A602)+2 种基金the Outstanding Young Fund of Jiangsu Province(BK2012040)the“Six Top Talents”and“333 Talent Project”of Jiangsu Province,State Key Laboratory of Materials-Oriented Chemical Engineering(ZK201719)the State Key Laboratory of Inorganic Synthesis and Preparative Chemistry,Jilin University(2018-19).
文摘A hollow-fiber-supported stable Au/FAU catalytic membrane was successfully synthesized through a polydopamine coating modification-removal strategy and used as a flow-through catalytic membrane reactor for preferential oxidation of CO.Small Au nanoparticles can be efficiently isolated by dopamine and the dopamine-derived carbon shells.The interactions between Au nanoparticles and zeolite layer support are enhanced during annealing at high temperature under an inert atmosphere.A zeolite membrane supported Au nanoparticle catalyst was obtained after the removal of carbon shells,which showed high catalytic activity and stability for the removal of CO from hydrogen.
基金Project supported bythe National Nature Science Foundation of China (20276015)
文摘Y-Modified USY was prepared by ion exchange of USY slurry with 0.01 mol·L-1 Y(NO3)3. Phosphotungstic acid (HPW) catalyst supported on USY and Y-USY was prepared by an impregnation method. The materials were characterized by NH3-TPD, XRD, and N2 adsorption. The activity for the removal of thiophene was examined in a three-necked flask. The sulfur content of model compound was tested on WK-2D microcoulometric detector. The effect of yttrium and HPW content, reaction temperature and catalysts, activation temperature on the activity of catalysts were investigated. It was shown that the oxidation activity of thiophene decreased with the increase of Y content except for the catalyst of Y 5%. HPW content had limit influence on activity of catalysts. The optimal reaction temperature and activation temperature were 40 and 320 ℃, respectively.
基金Project supported by the National Key Basic Research Program(NKBRP20047CCA03900)National Natural Science Foundation of China(2056601)
文摘Study was made on the effect of surface modification on the behaviors of cerium oxide nanopowders.A surfactant-sodium dodecyl sulfate(C12H25SO4Na)was used to modify the surface of CeO2 powder particles.The unmodified and modified CeO2 powders were characterized by using a powder comprehensive characteristic tester,laser particle size analyzer,specific surface area tester,X-ray diffraction tester,and a scanning electron microscope.The testing and analysis results showed that C12H25SO4Na surface modification might increase the flowability and dispersity,and decrease the specific surface area and agglomeration of CeO2 powders.The mechanism of the surface modification of CeO2 powder particles was also discussed.
文摘Nickel-rich layered oxides have been identified as the most promising commercial cathode materials for lithium-ion batteries(LIBs)for their high theoretical specific capacity.However,the poor cycling stability of nickel-rich cathode materials is one of the major barriers for the large-scale usage of LIBs.The existing obstructions that suppress the capacity degradation of nickel-rich cathode materials are as a result of phase transition,mechanical instability,intergranular cracks,side reaction,oxygen loss,and thermal instability during cycling.Core–shell structures,oxidating precursors,electrolyte additives,doping/coating and synthesizing single crystals have been identified as effective methods to improve cycling stability of nickel-rich cathode materials.Herein,recent progress of surface modification,e.g.coating and doping,in nickel-rich cathode materials are summarized based on Periodic table to provide a clear understanding.Electrochemical performances and mechanisms of modified structure are discussed in detail.It is hoped that an overview of synthesis and surface modification can be presented and a perspective of nickel-rich materials in LIBs can be given.
文摘Mn_2O_3-Na_2WO_4/SiO_2 is considered as the most promising catalyst for the oxidative coupling of methane(OCM) process; however, it only has a better catalytic performance over 800 °C. To improve its low-temperature performance, an attempt has been made to modify the Mn_2O_3-Na_2WO_4/SiO_2 catalyst using TiO_2, MgO, Ga_2O_3, and ZrO_2. Among the synthesized catalysts, the TiO_2-modified Mn_2O_3-Na_2WO_4/SiO_2 catalyst shows markedly improved low-temperature OCM performance,achieving a high CH_4 conversion of ~23% and a good C_2-C_3 selectivity of ~73% at 700 °C(the catalyst bed temperature), along with promising stability for at least 300 h without signs of deactivation.In comparison with the unmodified Mn_2O_3-Na_2WO_4/SiO_2 catalyst, the TiO_2 modification results in significant improvement in the low-temperature activity/selectivity, whereas the MgO modification has almost no impact and the Ga_2O_3 and ZrO_2 modifications have a negative effect. The X-ray diffraction(XRD) and Raman results reveal that the formation of a MnTiO_3 phase and a MnTiO_3-dominated catalyst surface is crucial for the improvement of the low-temperature activity/selectivity in the OCM process.
基金supported by FedDev Ontario through the Applied Research and Commercialization (ARC) Initiative and the Natural Sciences and Engineering Research Council of Canada (NSERC) programMicrobonds, Inc. for additional financial support
文摘Carbon modified TiO_2 nanobelts(TiO_2-C) were synthesized using a hydrothermal growth method,as a support material for palladium(Pd) nanoparticles(Pd/TiO_2-C) to improve the electrocatalytic performance for methanol electrooxidation by comparison to Pd nanoparticles on bare TiO_2 nanobelts(Pd/TiO_2)and activated carbon(Pd/AC). Cyclic voltammetry characterization was conducted with respect to saturated calomel electrode(SCE) in an alkaline methanol solution, and the results indicate that the specific activity of Pd/TiO_2-C is 2.2 times that of Pd/AC and 1.5 times that of Pd/TiO_2. Chronoamperometry results revealed that the TiO_2-C support was comparable in stability to activated carbon, but possesses an enhanced current density for methanol oxidation at a potential of -0.2 V vs. SCE. The current study demonstrates the potential of Pd nanoparticle loaded on hierarchical TiO_2-C nanobelts for electrocatalytic applications such as fuel cells and batteries.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.10974013 and 60978060)the Research Fund for the Doctoral Program of Higher Education,China(Grant No.20090009110027)+3 种基金the Beijing Municipal Natural Science Foundation,China(Grant No.1102028)the New Century Excellent Talents in University,China(Grant No.NCET-10-0220)the Fundamental Research Funds for the Central Universities,China(Grant No.2012JBZ001)the Technology Innovation Fund for Outstanding Ph.D.Students of Beijing Jiaotong University,China(Grant No.48034)
文摘The properties of poly(3-hexylthiophene):(6,6)-phenyl C61 butyric acid methyl ester (P3HT:PCBM) organic pho- tovoltaic devices (OPVs) with an indium tin oxide (ITO) anode treated by a KMnO4 solution are investigated. The optimized KMnO4 solution has a concentration of 50 rag/L, and ITO is treated for 15 min. The modification of ITO anode results in an enhancement of the power conversion efficiency (PCE) of the device, which is responsible for the increase of the photocurrent. The performance enhancement is attributed to the work function modification of the ITO substrate through the strong oxygenation of KMnO4, and then the charge collection efficiency is improved.
基金supported by the National Natural Science Foundation of China (21790331,21603218)the Strategic Priority Research Program of Chinese Academy of Sciences (XDA21030400,XDB17020300)~~
文摘The surface modification of metal oxides using organic modifiers is a potential strategy for enhancing their catalytic performances.In this study,a hydrophobic surface amine-modified CoO catalyst with a water contact angle of 143°was fabricated.The catalyst was characterized by XRD,TGA,FT-IR,HR-TEM,and XPS.The results showed that the fabricated catalyst performed better than the hydrophilic commercial CoO nanoparticle in the process of aromatic hydrocarbon oxidation.After the amines modification,commercial CoO also became hydrophobic and improved conversion of ethylbenzene was achieved.The surface modification of CoO with amines induced the hydrophobicity property,which could serve as a reference for the design of other hydrophobic catalysts.
基金grateful for funding from the National Natural Science Foundation of China(Grant No.52174053,52130401 and 51974344)Natural Science Foundation of Shandong Provincial(ZR2019MEE077).
文摘Asymmetrically modified Janus graphene oxide(JGO)has attracted great attention due to its unique physical chemistry properties and wide applications.The modification degree of Janus nanosheets inevitably affects their interfacial activity,which is essential for their performances in enhanced oil recovery(EOR).In this study,the interfacial properties of Janus graphene oxide(JGO)with various modification degrees at liquid-liquid and liquid-solid interfaces were systematically evaluated via the measurements of interfacial tension(IFT),dilatational modulus,contact angle,and EOR efficiency was further assessed by core flooding tests.It is found that JGO-5 with higher modification degree exhibits the greater ability to reduce IFT(15.16 mN/m)and dilatational modulus(26 mN/m).Furthermore,JGO can construct interfacial and climbing film with the assistance of hydrodynamic power to effectively detach the oil from the rock surface and greatly enhance oil recovery.Moderately modified JGO-2 can highly improve recovery of residual crude oil(11.53%),which is regarded as the promising EOR agent in practical application.The present study firstly focuses on the effects of modification degrees on the JGO interfacial properties and proposes diverse EOR mechanisms for JGO with different modification degrees.
文摘Mesoporous TiO2 (m-TiO2) nanoparticles were used to prepare the porous film electrodes for dye-sensitized solar cells, and a second metal oxide (MgO, ZnO, A1203, or NiO) modifi- cation was carried out by dipping the m-TiO2 electrode into their respective nitrate solution followed by annealing at 500 ℃. Experimental results indicated that the above second metal oxide modifications on m-TiO2 electrode are shown in all cases to act as barrier layer for the interracial charge transfer processes, but film electron transport and interfacial charge recombination characteristics under applied bias voltage were dependent significantly on the existing states and kinds of these second metal oxides. Those changes based on sec- ond metal oxide modifications showed good correlation with the current-voltage analyses of dye-sensitized solar cell, and all modifications were found to increase the open-circuit photo- voltage in various degrees, while the MgO, ZnO, and NiO modifications result in 23%, 13%, and 6% improvement in cell conversion efficiency, respectively. The above observations indi- cate that controlling the charge transport and recombination is very important to improve the photovoltaic performance of TiO2-based solar cell.
基金the financial support from National Key Research & Development Program of China (2017B0602702)。
文摘In this paper, the superhydrophobic polyurethane sponge(SS-PU) was facilely fabricated by etching with Jones reagent to bind the nanoparticles of Ni-Co double layered oxides(LDOs) on the surface, and following modification with n-dodecyl mercaptan(DDT). This method provides a new strategy to fabricate superhydrophobic PU sponge with a water contact angle of 157° for absorbing oil with low cost and in large scale. It exhibits the strong absorption capacity and highly selective characteristic for various kinds of oils which can be recycled by simple squeezing. Besides, the as-prepared sponge can deal with the floating and underwater oils, indicating its application value in handling oil spills and domestic oily wastewater. The good self-cleaning ability shows the potential to clear the pollutants due to the ultralow adhesion to water. Especially, the most important point is that the superhydrophobic sponge can continuously and effectively separate the oil/water mixture against the condition of turbulent disturbance by using our designed device system, which exhibit its good superhydrophobicity, strong stability.Furthermore, the SS-PU still maintained stable absorption performance after 150 cycle tests without losing capacity obviously, showing excellent durability in long-term operation and significant potential as an efficient absorbent in large-scale dispose of oily water.