Laminated elastomeric bearings have been widely used for small-to-medium-span highway bridges in China, in which concrete shear keys are set transversely to prohibit large girder displacement. To evaluate bridge seism...Laminated elastomeric bearings have been widely used for small-to-medium-span highway bridges in China, in which concrete shear keys are set transversely to prohibit large girder displacement. To evaluate bridge seismic responses more accurately, proper analytical models of bearings and shear keys should be developed. Based on a series of cyclic loading experiments and analyses, rational analytical models of laminated elastomeric bearings and shear keys, which can consider mechanical degradation, were developed. The effect of the mechanical degradation was investigated by examining the seismic response of a small-to-medium-span bridge in the transverse direction under a wide range of peak ground accelerations(PGA). The damage mechanism for small-to-medium-span highway bridges was determined, which can explain the seismic damage investigation during earthquakes in recent years. The experimental results show that the mechanical properties of laminated elastomeric bearings will degrade due to friction sliding, but the degree of decrease is dependent upon the influencing parameters. It can be concluded that the mechanical degradation of laminated elastomeric bearings and shear keys play an important role in the seismic response of bridges. The degradation of mechanical properties of laminated elastomeric bearings and shear keys should be included to evaluate more precise bridge seismic performance.展开更多
Generation of large strains upon Na^(+) intercalation is one of the prime concerns of the mechanical degradation of Prussian blue(PB)and its analogs.Structural construction from the atomic level is imperative to maint...Generation of large strains upon Na^(+) intercalation is one of the prime concerns of the mechanical degradation of Prussian blue(PB)and its analogs.Structural construction from the atomic level is imperative to maintain structural stability and ameliorate the long-term stability of PB.Herein,an inter nickel hexacyanoferrate(NNiFCN)is successfully introduced at the out layer of iron hexacyanoferrate(NFFCN)through ion exchange to improve structural stability through compressive stress locking by forming NNiFCN shell.Furthermore,the kinetics of sodium ion diffusion is enhanced through the built-in electric pathway.The electrochemical performance is therefore significantly improved with a remarkable long-term cycling stability over 3,000 cycles at 500 mA·g^(–1) in the full sodium-ion batteries(SIBs)with a maximum energy density of 91.94 Wh·g^(–1),indicating that the core-shell structured NNiFCN/NFFCN could be the low-cost and high-performance cathode for full SIBs in large-scale EES applications.展开更多
LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries(LIBs)due to high discharge capacities and energy ...LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries(LIBs)due to high discharge capacities and energy densities at high operation voltage.However,the capacity fading under high operation voltage still restricts the practical application.Herein,the capacity degradation mechanism of NCM811 at atomic-scale is studied in detail under various cut-off voltages using aberration-corrected scanning transmission electron microscopy(STEM).It is observed that the crystal structure of NCM811 evolution from a layered structure to a rock-salt phase is directly accompanied by serious intergranular cracks under 4.9 V,which is distinguished from the generally accepted structure evolution of layered,disordered layered,defect rock salt and rock salt phases,also observed under 4.3 and 4.7 V.The electron energy loss spectroscopy analysis also confirms the reduction of Ni and Co from the surface to the bulk,not the previously reported only Li/Ni interlayer mixing.The degradation mechanism of NCM811 at a high cut-off voltage of4.9 V is attributed to the formation of intergranular cracks induced by defects,the direct formation of the rock salt phase,and the accompanied reduction of Ni^(2+)and Co^(2+)phases from the surface to the bulk.展开更多
The ever-increasing future demands of electrification and grid storage have spurred continued research to develop rechargeable battery chemistries for reliable energy storage[1].Beyond current lithium-ion batteries,li...The ever-increasing future demands of electrification and grid storage have spurred continued research to develop rechargeable battery chemistries for reliable energy storage[1].Beyond current lithium-ion batteries,lithium–sulfur battery represents a promising system due to its high energy density(2600 Wh kg^(-1))and low material cost[2].展开更多
Lignin is a natural polymer,second only to cellulose in natural reserves.Degradation is one of the ways to achieve the high-value transformation of lignin.Deep eutectic solvent(DES)thermal degradation of lignin can be...Lignin is a natural polymer,second only to cellulose in natural reserves.Degradation is one of the ways to achieve the high-value transformation of lignin.Deep eutectic solvent(DES)thermal degradation of lignin can be used as an excellent green degradation method.This paper introduces the degradation mechanism and effect of the lactic acid-choline chloride DES system in dissolving and degrading alkaline lignin,and the final solvent recovery.It can also be found from the scanning electron microscope(SEM)images that the surface of the degraded solid product is transformed from smooth to disordered.Fourier transform infrared(FTIR)spectroscopy and 1H-NMR spectroscopy were used to characterize the changes in lignin functional groups during DES treatment.The results showed that the content of phenolic hydroxyl groups increased after degradation,indicating that theβ-O-4 ether bond was broken.The molecular weight of the degraded lignin was observed by gel permeation chromatography(GPC),and the lignin residue with low molecular weight and narrow polydispersity index was obtained.The lowest average molecular weight(Mw)reached 2512 g/mol.The ratio of oxygen to carbon atoms in lignin increased substantially during degradation as measured by X-ray photoelectron spectroscopy(XPS),probably because DES treatment was accompanied by many oxidation reactions,which led to significant structural changes in lignin and a large number of ether bond breakage reactions during the reaction.The main final degradation products are aromatic monomers,vanillin,butyrovanillone,etc.展开更多
The photocatalytic degradation of Rhodamine B (RhB) was carried out using TiO2 supported on activated carbon (TiO2-AC) under microwave irradiation. Composite catalyst TiO2-AC was prepared and characterized using X...The photocatalytic degradation of Rhodamine B (RhB) was carried out using TiO2 supported on activated carbon (TiO2-AC) under microwave irradiation. Composite catalyst TiO2-AC was prepared and characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM) and Brunauer-Emmett-Teller (BET). In the process of microwave-enhanced photocatalysis (MPC), RhB (30 mg/L) was almost completely decoloured in 10 min, and the mineralization efficiency was 96.0% in 20 min. The reaction rate constant of RhB in MPC using TiO2-AC by pseudo first-order reaction kinetics was 4.16 times of that using Degussa P25. Additionally, according to gas chromatography/mass spectrometry (GC/MS) and liquid chromatography/mass spectrometry (LC/MS) identification, the major intermediates of RhB in MPC included two kinds of N-de-ethylation intermediates (N,N-diethyl-N'-ethyl-rhodamine (DER)), oxalic acid, malonic acid, snccinic acid, and phthalic acid, maleic acid, 3-nitrobenzoic acid, and so on. The degradation of RhB in MPC was mainly attributed to the destruction of the conjugated structure, and then the intermediates transformed to acid molecules which were mineralized to water and carbon dioxide.展开更多
The 2,4,6-trinitrotoluene (TNT) is a potential carcinogens and TNT contaminated wastewater, which could not be effectively disposed with conventional treatments. The supercritical water oxidation (SCWO) to treat T...The 2,4,6-trinitrotoluene (TNT) is a potential carcinogens and TNT contaminated wastewater, which could not be effectively disposed with conventional treatments. The supercritical water oxidation (SCWO) to treat TNT contaminated wastewater was studied in this article, The TNT concentration in wastewater was measured by high-performance liquid chromatograph (HPLC) and the degraded intermediates were analyzed using GC-MS. The results showed that SCWO could degrade TNT efficiently in the presence of oxygen. The reaction temperature, pressure, residence time and oxygen excess were the main contributing factors in the process. The decomposition of TNT was accelerated as the temperature or residence time increased. At 550℃, 24 MPa, 120 s and oxygen excess 300%, TNT removal rate could exceed 99.9%. Partial oxidation occured in SCWO without oxygen. It was concluded that supercritical water was a good solvent and had excellent oxidation capability in the existence of oxygen. The main intermediates of TNT during SCWO included toluene, 1,3,5-trinitrobenzene, nitrophenol, naphthalene, fluorenone, dibutyl phthalate, alkanes and several dimers based on the intermediate analysis. Some side reactions, such as coupled reaction, hydrolysis reaction and isomerization reaction may take place simultaneously when TNT was oxidized by SCWO.展开更多
The mechanism of carotenoid degradation and the changes in the activities of related enzymes in flue-cured tobacco at the leaf-drying stage during the bulk-curing process were studied in order to provide theoretical b...The mechanism of carotenoid degradation and the changes in the activities of related enzymes in flue-cured tobacco at the leaf-drying stage during the bulk-curing process were studied in order to provide theoretical basis for optimization of curing technology. The effect of different rising speeds of temperature on the carotenoid degradation and the related enzymes activities at the color-fixing stage during the bulk curing process was studied by using the electric-heated fluecuring barn designed by Henan Agricultural University, China, based on curing technology with yellowing at low temperature and moderate humidity and leaf drying at moderate humidity. The results showed that the carotenoid degradation components (β-carotene, lutein, neoxanthin, and violaxthin) decreased gradually at the color-fixing stage during the bulk curing process. The carotenoid degradation components viz.,β-carotene, lutein, neoxanthin, and violaxthin at the slow heating curing (T1) were relatively higher than the rapid heating curing (T2) accounting for 10, 2, 32 and 32% respectively, but there were no differences among treatments (P〉 0.05). The effect of different conditions of curing on the activities of enzymes related to carotenoids degradation were significant. The lipoxygenase, phenylalanine ammonialyase, peroxidase, and polyphenol oxidase enzymes had a bidirectional effect on the quality of tobacco leaves and it was beneficial to form more premise matter of aroma based on the higher enzyme activities at the early leaf-drying stage. The slow heating could regulate the change in various enzymes' activities reasonably, making cell redox reaction to reach the dynamic balance and make the degradation of carotenoids adequately. Meanwhile, it could avoid the occurrence of browning reaction and provide foundation for improving the quality of tobacco and optimization of technology for bulk curing and further enhancing aroma.展开更多
Tetracycline(TC)is an antibiotic mainly used in livestock production and respiratory infection.Traditional methods are not effective in removing TC from solution.In this study,TC was degraded by gas–liquid plasma in ...Tetracycline(TC)is an antibiotic mainly used in livestock production and respiratory infection.Traditional methods are not effective in removing TC from solution.In this study,TC was degraded by gas–liquid plasma in the presence of rGO-TiO_(2)in solution.The rGO-TiO_(2)was prepared by modified hummers and hydrothermal method.The electrical and optical properties of the gas–liquid discharge plasma were studied and the produced long-lived reactive species were analyzed by spectrophotometer.The degradation efficiency of TC was improved by 41.4%after plasma treatment for 12 min in presence of 30 mg l-1 r GO-TiO_(2)compared to that with plasma alone.The degradation efficiency increased with increasing discharge power,but as the initial concentration was increased from 20 to 80 mg l-1,the degradation efficiency of TC decreased.The initial p H had no significant effect on the degradation of TC.The intermediate products were determined by UV–vis spectrophotometry and ESI(+)–MS,and the degradation mechanism was analyzed.The reactive species,including O_(3),·OH,and H_(2)O_(2),etc.,produced in the plasma/catalyst system attracted electron-rich functional groups(amino group,aromatic ring,and double bond).Therefore,the gas–liquid plasma/catalyst system could be an effective and promising method for pharmaceutical wastewater treatment in future.展开更多
Step-stress experiments are performed in this paper to investigate the degradation mechanism of an AIGaN/GaN high electron mobility transistor (HEMT). It is found that the stress current shows a recoverable decrease...Step-stress experiments are performed in this paper to investigate the degradation mechanism of an AIGaN/GaN high electron mobility transistor (HEMT). It is found that the stress current shows a recoverable decrease during each voltage step and there is a critical voltage beyond which the stress current starts to increase sharply in our experiments. We postulate that defects may be randomly induced within the A1GaN barrier by the high electric field during each voltage step. But once the critical voltage is reached, the trap concentration will increase sharply due to the inverse piezoelectric effect. A leakage path may be introduced by excessive defect, and this may result in the permanent degradation of the A1GaN/GaN HEMT.展开更多
Phenolic compounds are widely present in domestic and industrial sewage and have serious environmental hazards.Electrochemical oxidation(EO)is one of the most promising methods for sewage degradation because of its hi...Phenolic compounds are widely present in domestic and industrial sewage and have serious environmental hazards.Electrochemical oxidation(EO)is one of the most promising methods for sewage degradation because of its high efficiency,environmental compatibility,and safety.In this work,we present an in-depth overview of the mechanism and factors affecting the degradation of phenolic compounds by EO.In particular,the effects of treatment of phenolic compounds with different anode materials are discussed in detail.The non-active anode shows higher degradation efficiency,less intermediate accumulation,and lower energy consumption than the active anode.EO combined with other treatment methods(biological,photo,and Fenton)presents advantages,such as low energy consumption and high degradation rate.Mean-while,the remaining drawbacks of the EO process in the phenolic compound treatment system have been discussed.Furthermore,future re-search directions are put forward to improve the feasibility of the practical application of EO technology.展开更多
The accelerated degradation in the front ceils of a polymer electrolyte membrane fuel cell(PEMFC) stack seriously reduces the reliability and durability of the whole stack. Most researches only focus on the size and...The accelerated degradation in the front ceils of a polymer electrolyte membrane fuel cell(PEMFC) stack seriously reduces the reliability and durability of the whole stack. Most researches only focus on the size and configuration of the gas intake manifold, which may lead to the maldistribution of flow and pressure. In order to find out the mechanisms of the accelerated degradation in the front cells, an extensive program of experimental and simulation work is initiated and the results are reported. It is found that after long-term lifetime tests the accelerated degradation in the front cells occurs in all three fuel cell stacks with different flow-fields under the U-type feed configuration. Compared with the rear cells of the stack, the voltage of the front cells is much lower at the same current densities and the membrane electrode assembly(MEA) has smaller active area, more catalyst particle agglomeration and higher ohmic impedance. For further investigation, a series of three dimensional isothermal numerical models are built to investigate the degradation mechanisms based on the experimental data. The simulation results reveal that the dry working condition of the membrane and the effect of high-speed gas scouting the MEA are the main causes of the accelerated degradation in the front cells of a PEM fuel cell stack under the U-type feed configuration. Several mitigation strategies that would mitigate these phenomena are presented: removing cells that have failed and replacing them with those of the same aging condition as the average of the stack; choosing a Z-type feed pattern instead of a U-type one; putting several air flow-field plates without MEA in the front of the stack; or exchanging the gas inlet and outlet alternately at a certain interval. This paper specifies the causes of the accelerated degradation in the front cells and provides the mitigation strategies.展开更多
Organic Light Emitting Devices (OLED) have attracted much attention recently, for their applications in futureFlat Panel Displays and lighting products. However, their fast degradation remained a major obstacle to the...Organic Light Emitting Devices (OLED) have attracted much attention recently, for their applications in futureFlat Panel Displays and lighting products. However, their fast degradation remained a major obstacle to theircommercialization. Here we present a brief summary of our studies on both extrinsic and intrinsic causes for the fastdegradation of OLEDs. In particular, we focus on the origin of the dark spots by 'rebuilding' cathodes, which confirms thatthe growth of dark spots occurs primarily due to cathode delamination. In the meantime, we recapture the findings from thesearch for suitable OLED packaging materials, in particular polymer composites, which provide both heat dissipation andmoisture resistance, in addition to electrical insulation.展开更多
Recently,a plasma catalyst was employed to efflciently degrade antibiotic residues in the environment.In this study,the plasma generated in a packed bed dielectric barrier reactor combined with TiO_(2)catalyst is used...Recently,a plasma catalyst was employed to efflciently degrade antibiotic residues in the environment.In this study,the plasma generated in a packed bed dielectric barrier reactor combined with TiO_(2)catalyst is used to degrade the antibiotic tiamulin(TIA)loaded on the surface of simulated soil particles.The effects of applied voltage,composition of the working gas,gas flow rate and presence or absence of catalyst on the degradation effect were studied.It was found that plasma and catalyst can produce a synergistic effect under optimal conditions(applied voltage 25 k V,oxygen ratio 1%,gas flow rate 0.6 l min^(-1),treatment time 5 min).The degradation efflciency of the plasma combined with catalyst can reach 78.6%,which is 18.4%higher than that of plasma without catalyst.When the applied voltage is 30 k V,the gas flow rate is 1 l min^(-1),the oxygen ratio is 1%and the plasma combined with TiO_(2)catalyst treats the sample for 5 min the degradation efflciency of TIA reached 97%.It can be concluded that a higher applied voltage and longer processing times not only lead to more degradation but also result in a lower energy efflciency.Decreasing the oxygen ratio and gas flow rate could improve the degradation efflciency.The relative distribution and identity of the major TIA degradation product generated was determined by high-performance liquid chromatography–mass spectrometry analysis.The mechanism of TIA removal by plasma and TiO_(2)catalyst was analyzed,and the possible degradation path is discussed.展开更多
This paper finds that the two-dimensional electron gas density in high Al-content A1GaN/GaN heterostructures exhibits an obvious time-dependent degradation after the epitaxial growth. The degradation mechanism was inv...This paper finds that the two-dimensional electron gas density in high Al-content A1GaN/GaN heterostructures exhibits an obvious time-dependent degradation after the epitaxial growth. The degradation mechanism was investigated in depth using Hall effect measurements,high resolution x-ray diffraction,scanning electron microscopy,x-ray photoelectron spectroscopy and energy dispersive x-ray spectroscopy.The results reveal that the formation of surface oxide is the main reason for the degradation,and the surface oxidation always occurs within the surface hexagonal defects for high Al-content AlGaN/GaN heterostructures.展开更多
Degradation reaction of doxycycline or methacycline was carried out in KOH solution and intense fluorescence was obtained.A degradation mechanism of doxycycline or methacycline was suggested.
Systemic measurements show that there is no 3D to 2D crossover in the reduction of the superconducting transition temperature Tc in Nb thin films. This result is consistent with all previous measurements while it is c...Systemic measurements show that there is no 3D to 2D crossover in the reduction of the superconducting transition temperature Tc in Nb thin films. This result is consistent with all previous measurements while it is contrary to the prevailing understanding based on the interplay between proximity, localization, and lifetime broadening. Our study indicates that the decrease of Tc can be interpreted by the combined effects of electron-phonon coupling parameter λ and the defect scattering rate pw, being uniquely determined by their ratio λ/ρw. Other factors such as film thickness and irradiation do not produce additional effects beyond these two parameters.展开更多
SF_(6)degradation mechanism in non-thermal plasma(NTP)systems is not fully understood due to the formation of a complex physico-chemical reaction network,especially when reactive gases and packing materials are involv...SF_(6)degradation mechanism in non-thermal plasma(NTP)systems is not fully understood due to the formation of a complex physico-chemical reaction network,especially when reactive gases and packing materials are involved.In this work,we conduct a combined experimental and theoretical study to unravel the SF_(6)degradation path in a-Al_(2)O_(3)packed plasma in the presence of H_(2)O or O_(2).Our experimental results show that both H_(2)O and O_(2)have a synergetic effect with-Al_(2)O_(3)packing on promoting SF_(6)degradation,leading to higher stable gas yields than typical spark or corona discharges.H_(2)O or O_(2)addition promotes SO_(2)or SO_(2)F_(2)selectivity,respectively.Density functional theory(DFT)calculations reveal that SO_(2)generation corresponding with the highest activation barrier is the most critical step toward SF_(6)degradation.Radicals like H and O generated from H_(2)O or O_(2)discharge can significantly promote the degradation process via Eley-Rideal mechanism,affecting key reactions of stable product generation,advancing degradation efficiency.The results of this work could provide insights on further understanding SF_(6)degradation mechanism especially in packed-bed plasma systems.展开更多
High-temperature proton exchange membrane fuel cells(HT-PEMFCs)are pursued worldwide as efficient energy conversion devices.Great efforts have been made in the area of designing and developing phosphoric acid(PA)-base...High-temperature proton exchange membrane fuel cells(HT-PEMFCs)are pursued worldwide as efficient energy conversion devices.Great efforts have been made in the area of designing and developing phosphoric acid(PA)-based proton exchange membrane(PEM)of HT-PEMFCs.This review focuses on recent advances in the limitations of acid-based PEM(acid leaching,oxidative degradation,and mechanical degradation)and the approaches mitigating the membrane degradation.Preparing multilayer or polymers with continuous network,adding hygroscopic inorganic materials,and introducing PA doping sites or covalent interactions with PA can effectively reduce acid leaching.Membrane oxidative degradation can be alleviated by synthesizing crosslinked or branched polymers,and introducing antioxidative groups or highly oxidative stable materials.Crosslinking to get a compact structure,blending with stable polymers and inorganic materials,preparing polymer with high molecular weight,and fabricating the polymer with PA doping sites away from backbones,are recommended to improve the membrane mechanical strength.Also,by comparing the running hours and decay rate,three current approaches,1.crosslinking via thermally curing or polymeric crosslinker,2.incorporating hygroscopic inorganic materials,3.increasing membrane layers or introducing strong basic groups and electron-withdrawing groups,have been concluded to be promising approaches to improve the durability of HT-PEMFCs.The overall aim of this review is to explore the existing degradation challenges and opportunities to serve as a solid basis for the deployment in the fuel cell market.展开更多
In spite of their extraordinary performance, AlGaN/GaN high electron mobility transistors (HEMTs) still lack solid reliability. Devices under accelerated DC stress tests (off-state, VDS = 0 state, and on-state step...In spite of their extraordinary performance, AlGaN/GaN high electron mobility transistors (HEMTs) still lack solid reliability. Devices under accelerated DC stress tests (off-state, VDS = 0 state, and on-state step-stress) are investigated to help us identify the degradation mechanisms of the AlGaN/GaN HEMTs. All our findings are consistent with the degradation mechanism based on crystallographic-defect formation due to the inverse piezoelectric effects in Ref. [1] (Joh J and del Alamo J A 2006 IEEE IDEM Tech. Digest p. 415). However, under the on-state condition, the devices are suffering from both inverse piezoelectric effects and hot electron effects, and so to improve the reliability of the devices both effects should be taken into consideration.展开更多
基金Project of China International Science and Technology Cooperation under Grant No.2009DFA82480Science and Technology Project of Communications’ Construction in Western China,MOC under Grant No.2009318223094
文摘Laminated elastomeric bearings have been widely used for small-to-medium-span highway bridges in China, in which concrete shear keys are set transversely to prohibit large girder displacement. To evaluate bridge seismic responses more accurately, proper analytical models of bearings and shear keys should be developed. Based on a series of cyclic loading experiments and analyses, rational analytical models of laminated elastomeric bearings and shear keys, which can consider mechanical degradation, were developed. The effect of the mechanical degradation was investigated by examining the seismic response of a small-to-medium-span bridge in the transverse direction under a wide range of peak ground accelerations(PGA). The damage mechanism for small-to-medium-span highway bridges was determined, which can explain the seismic damage investigation during earthquakes in recent years. The experimental results show that the mechanical properties of laminated elastomeric bearings will degrade due to friction sliding, but the degree of decrease is dependent upon the influencing parameters. It can be concluded that the mechanical degradation of laminated elastomeric bearings and shear keys play an important role in the seismic response of bridges. The degradation of mechanical properties of laminated elastomeric bearings and shear keys should be included to evaluate more precise bridge seismic performance.
基金J.G.S.wants to thanks China Scholarship Council(CSC)for the scholarship support(No.201706050153)。
文摘Generation of large strains upon Na^(+) intercalation is one of the prime concerns of the mechanical degradation of Prussian blue(PB)and its analogs.Structural construction from the atomic level is imperative to maintain structural stability and ameliorate the long-term stability of PB.Herein,an inter nickel hexacyanoferrate(NNiFCN)is successfully introduced at the out layer of iron hexacyanoferrate(NFFCN)through ion exchange to improve structural stability through compressive stress locking by forming NNiFCN shell.Furthermore,the kinetics of sodium ion diffusion is enhanced through the built-in electric pathway.The electrochemical performance is therefore significantly improved with a remarkable long-term cycling stability over 3,000 cycles at 500 mA·g^(–1) in the full sodium-ion batteries(SIBs)with a maximum energy density of 91.94 Wh·g^(–1),indicating that the core-shell structured NNiFCN/NFFCN could be the low-cost and high-performance cathode for full SIBs in large-scale EES applications.
基金supported by the National Natural Science Foundation of China(U2032131)the Key R&D Program of Shaanxi Province(2021GY-118)the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(2022SX-TD012 and 2021SXTD012)。
文摘LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries(LIBs)due to high discharge capacities and energy densities at high operation voltage.However,the capacity fading under high operation voltage still restricts the practical application.Herein,the capacity degradation mechanism of NCM811 at atomic-scale is studied in detail under various cut-off voltages using aberration-corrected scanning transmission electron microscopy(STEM).It is observed that the crystal structure of NCM811 evolution from a layered structure to a rock-salt phase is directly accompanied by serious intergranular cracks under 4.9 V,which is distinguished from the generally accepted structure evolution of layered,disordered layered,defect rock salt and rock salt phases,also observed under 4.3 and 4.7 V.The electron energy loss spectroscopy analysis also confirms the reduction of Ni and Co from the surface to the bulk,not the previously reported only Li/Ni interlayer mixing.The degradation mechanism of NCM811 at a high cut-off voltage of4.9 V is attributed to the formation of intergranular cracks induced by defects,the direct formation of the rock salt phase,and the accompanied reduction of Ni^(2+)and Co^(2+)phases from the surface to the bulk.
基金supported by the Agency for Science,Technology and Research(Central Research Fund Award)。
文摘The ever-increasing future demands of electrification and grid storage have spurred continued research to develop rechargeable battery chemistries for reliable energy storage[1].Beyond current lithium-ion batteries,lithium–sulfur battery represents a promising system due to its high energy density(2600 Wh kg^(-1))and low material cost[2].
基金This work was financially supported by the National Natural Science Foundation of China(31730106).
文摘Lignin is a natural polymer,second only to cellulose in natural reserves.Degradation is one of the ways to achieve the high-value transformation of lignin.Deep eutectic solvent(DES)thermal degradation of lignin can be used as an excellent green degradation method.This paper introduces the degradation mechanism and effect of the lactic acid-choline chloride DES system in dissolving and degrading alkaline lignin,and the final solvent recovery.It can also be found from the scanning electron microscope(SEM)images that the surface of the degraded solid product is transformed from smooth to disordered.Fourier transform infrared(FTIR)spectroscopy and 1H-NMR spectroscopy were used to characterize the changes in lignin functional groups during DES treatment.The results showed that the content of phenolic hydroxyl groups increased after degradation,indicating that theβ-O-4 ether bond was broken.The molecular weight of the degraded lignin was observed by gel permeation chromatography(GPC),and the lignin residue with low molecular weight and narrow polydispersity index was obtained.The lowest average molecular weight(Mw)reached 2512 g/mol.The ratio of oxygen to carbon atoms in lignin increased substantially during degradation as measured by X-ray photoelectron spectroscopy(XPS),probably because DES treatment was accompanied by many oxidation reactions,which led to significant structural changes in lignin and a large number of ether bond breakage reactions during the reaction.The main final degradation products are aromatic monomers,vanillin,butyrovanillone,etc.
基金supported by the National Natural Science Foundation of China (No. 20707009)the Jiangsu Province Social Development Foundation (No.BS2007051)+1 种基金the Opening Foundation (WTWER0713) of Engineering Research Center for Water Treatment and Water Remediation of the Ministry of Education of Chinathe State Key Laboratory of Pollution Control and Resource Reuse Opening Foundation (No. PCRRCF07003).
文摘The photocatalytic degradation of Rhodamine B (RhB) was carried out using TiO2 supported on activated carbon (TiO2-AC) under microwave irradiation. Composite catalyst TiO2-AC was prepared and characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM) and Brunauer-Emmett-Teller (BET). In the process of microwave-enhanced photocatalysis (MPC), RhB (30 mg/L) was almost completely decoloured in 10 min, and the mineralization efficiency was 96.0% in 20 min. The reaction rate constant of RhB in MPC using TiO2-AC by pseudo first-order reaction kinetics was 4.16 times of that using Degussa P25. Additionally, according to gas chromatography/mass spectrometry (GC/MS) and liquid chromatography/mass spectrometry (LC/MS) identification, the major intermediates of RhB in MPC included two kinds of N-de-ethylation intermediates (N,N-diethyl-N'-ethyl-rhodamine (DER)), oxalic acid, malonic acid, snccinic acid, and phthalic acid, maleic acid, 3-nitrobenzoic acid, and so on. The degradation of RhB in MPC was mainly attributed to the destruction of the conjugated structure, and then the intermediates transformed to acid molecules which were mineralized to water and carbon dioxide.
基金Project supported by the Science Technology Foundation of Educational Department(No.204020).
文摘The 2,4,6-trinitrotoluene (TNT) is a potential carcinogens and TNT contaminated wastewater, which could not be effectively disposed with conventional treatments. The supercritical water oxidation (SCWO) to treat TNT contaminated wastewater was studied in this article, The TNT concentration in wastewater was measured by high-performance liquid chromatograph (HPLC) and the degraded intermediates were analyzed using GC-MS. The results showed that SCWO could degrade TNT efficiently in the presence of oxygen. The reaction temperature, pressure, residence time and oxygen excess were the main contributing factors in the process. The decomposition of TNT was accelerated as the temperature or residence time increased. At 550℃, 24 MPa, 120 s and oxygen excess 300%, TNT removal rate could exceed 99.9%. Partial oxidation occured in SCWO without oxygen. It was concluded that supercritical water was a good solvent and had excellent oxidation capability in the existence of oxygen. The main intermediates of TNT during SCWO included toluene, 1,3,5-trinitrobenzene, nitrophenol, naphthalene, fluorenone, dibutyl phthalate, alkanes and several dimers based on the intermediate analysis. Some side reactions, such as coupled reaction, hydrolysis reaction and isomerization reaction may take place simultaneously when TNT was oxidized by SCWO.
基金supported by the Key Project of State Tobacco Monoply Administration of China(3300806156)
文摘The mechanism of carotenoid degradation and the changes in the activities of related enzymes in flue-cured tobacco at the leaf-drying stage during the bulk-curing process were studied in order to provide theoretical basis for optimization of curing technology. The effect of different rising speeds of temperature on the carotenoid degradation and the related enzymes activities at the color-fixing stage during the bulk curing process was studied by using the electric-heated fluecuring barn designed by Henan Agricultural University, China, based on curing technology with yellowing at low temperature and moderate humidity and leaf drying at moderate humidity. The results showed that the carotenoid degradation components (β-carotene, lutein, neoxanthin, and violaxthin) decreased gradually at the color-fixing stage during the bulk curing process. The carotenoid degradation components viz.,β-carotene, lutein, neoxanthin, and violaxthin at the slow heating curing (T1) were relatively higher than the rapid heating curing (T2) accounting for 10, 2, 32 and 32% respectively, but there were no differences among treatments (P〉 0.05). The effect of different conditions of curing on the activities of enzymes related to carotenoids degradation were significant. The lipoxygenase, phenylalanine ammonialyase, peroxidase, and polyphenol oxidase enzymes had a bidirectional effect on the quality of tobacco leaves and it was beneficial to form more premise matter of aroma based on the higher enzyme activities at the early leaf-drying stage. The slow heating could regulate the change in various enzymes' activities reasonably, making cell redox reaction to reach the dynamic balance and make the degradation of carotenoids adequately. Meanwhile, it could avoid the occurrence of browning reaction and provide foundation for improving the quality of tobacco and optimization of technology for bulk curing and further enhancing aroma.
基金financially supported by National Natural Science Foundation of China(Nos.51777206 and 51541807)Natural Science Foundation of Anhui Province(Nos.1908085MA29,1708085MB47 and 1708085MA13)+4 种基金Doctoral Fund of Ministry of Education of China(No.2017M612058)Specialized Research Fund for the Doctoral Program of Hefei University of Technology(No.JZ2016HGBZ0769)Chinese Academy of Sciences under Grant No.DSJJ-14-YY02Science and Technology Cooperation Program between China and Finland(No.2017YFE0115200)Hong Kong Research Grants Council(RGC)General Research Funds(GRF)(No.City U 11205617)。
文摘Tetracycline(TC)is an antibiotic mainly used in livestock production and respiratory infection.Traditional methods are not effective in removing TC from solution.In this study,TC was degraded by gas–liquid plasma in the presence of rGO-TiO_(2)in solution.The rGO-TiO_(2)was prepared by modified hummers and hydrothermal method.The electrical and optical properties of the gas–liquid discharge plasma were studied and the produced long-lived reactive species were analyzed by spectrophotometer.The degradation efficiency of TC was improved by 41.4%after plasma treatment for 12 min in presence of 30 mg l-1 r GO-TiO_(2)compared to that with plasma alone.The degradation efficiency increased with increasing discharge power,but as the initial concentration was increased from 20 to 80 mg l-1,the degradation efficiency of TC decreased.The initial p H had no significant effect on the degradation of TC.The intermediate products were determined by UV–vis spectrophotometry and ESI(+)–MS,and the degradation mechanism was analyzed.The reactive species,including O_(3),·OH,and H_(2)O_(2),etc.,produced in the plasma/catalyst system attracted electron-rich functional groups(amino group,aromatic ring,and double bond).Therefore,the gas–liquid plasma/catalyst system could be an effective and promising method for pharmaceutical wastewater treatment in future.
基金Project supported by the Program for New Century Excellent Talents in University (Grant No.NCET-12-0915)
文摘Step-stress experiments are performed in this paper to investigate the degradation mechanism of an AIGaN/GaN high electron mobility transistor (HEMT). It is found that the stress current shows a recoverable decrease during each voltage step and there is a critical voltage beyond which the stress current starts to increase sharply in our experiments. We postulate that defects may be randomly induced within the A1GaN barrier by the high electric field during each voltage step. But once the critical voltage is reached, the trap concentration will increase sharply due to the inverse piezoelectric effect. A leakage path may be introduced by excessive defect, and this may result in the permanent degradation of the A1GaN/GaN HEMT.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.52025041 and 51974021)the Fundamental Research Funds for the Central Universities(No.FRF-TP-19-004B2Z),and the Beijing Excellent Talents Foundation.
文摘Phenolic compounds are widely present in domestic and industrial sewage and have serious environmental hazards.Electrochemical oxidation(EO)is one of the most promising methods for sewage degradation because of its high efficiency,environmental compatibility,and safety.In this work,we present an in-depth overview of the mechanism and factors affecting the degradation of phenolic compounds by EO.In particular,the effects of treatment of phenolic compounds with different anode materials are discussed in detail.The non-active anode shows higher degradation efficiency,less intermediate accumulation,and lower energy consumption than the active anode.EO combined with other treatment methods(biological,photo,and Fenton)presents advantages,such as low energy consumption and high degradation rate.Mean-while,the remaining drawbacks of the EO process in the phenolic compound treatment system have been discussed.Furthermore,future re-search directions are put forward to improve the feasibility of the practical application of EO technology.
基金supported by National Basic Research Program of China(973 Program,Grant No.2012CB215500)National Hi-tech Research and Development Program of China(863 Program,Grant Nos.2012AA1106012,2012AA053402)+1 种基金National Natural Science Foundation of China(Grant No.20976095)the Specialized Research Fund for the Doctoral Program of Higher Education,China(Grant No.20090002110074)
文摘The accelerated degradation in the front ceils of a polymer electrolyte membrane fuel cell(PEMFC) stack seriously reduces the reliability and durability of the whole stack. Most researches only focus on the size and configuration of the gas intake manifold, which may lead to the maldistribution of flow and pressure. In order to find out the mechanisms of the accelerated degradation in the front cells, an extensive program of experimental and simulation work is initiated and the results are reported. It is found that after long-term lifetime tests the accelerated degradation in the front cells occurs in all three fuel cell stacks with different flow-fields under the U-type feed configuration. Compared with the rear cells of the stack, the voltage of the front cells is much lower at the same current densities and the membrane electrode assembly(MEA) has smaller active area, more catalyst particle agglomeration and higher ohmic impedance. For further investigation, a series of three dimensional isothermal numerical models are built to investigate the degradation mechanisms based on the experimental data. The simulation results reveal that the dry working condition of the membrane and the effect of high-speed gas scouting the MEA are the main causes of the accelerated degradation in the front cells of a PEM fuel cell stack under the U-type feed configuration. Several mitigation strategies that would mitigate these phenomena are presented: removing cells that have failed and replacing them with those of the same aging condition as the average of the stack; choosing a Z-type feed pattern instead of a U-type one; putting several air flow-field plates without MEA in the front of the stack; or exchanging the gas inlet and outlet alternately at a certain interval. This paper specifies the causes of the accelerated degradation in the front cells and provides the mitigation strategies.
文摘Organic Light Emitting Devices (OLED) have attracted much attention recently, for their applications in futureFlat Panel Displays and lighting products. However, their fast degradation remained a major obstacle to theircommercialization. Here we present a brief summary of our studies on both extrinsic and intrinsic causes for the fastdegradation of OLEDs. In particular, we focus on the origin of the dark spots by 'rebuilding' cathodes, which confirms thatthe growth of dark spots occurs primarily due to cathode delamination. In the meantime, we recapture the findings from thesearch for suitable OLED packaging materials, in particular polymer composites, which provide both heat dissipation andmoisture resistance, in addition to electrical insulation.
基金supported by National Natural Science Foundation of China(Nos.51967018,11965018 and 51967017)the Science and Technology Development Fund of Xinjiang Production and Construction(No.2019BC009)the Innovation and Development Special Project of Shihezi University(No.CXFZ202105)。
文摘Recently,a plasma catalyst was employed to efflciently degrade antibiotic residues in the environment.In this study,the plasma generated in a packed bed dielectric barrier reactor combined with TiO_(2)catalyst is used to degrade the antibiotic tiamulin(TIA)loaded on the surface of simulated soil particles.The effects of applied voltage,composition of the working gas,gas flow rate and presence or absence of catalyst on the degradation effect were studied.It was found that plasma and catalyst can produce a synergistic effect under optimal conditions(applied voltage 25 k V,oxygen ratio 1%,gas flow rate 0.6 l min^(-1),treatment time 5 min).The degradation efflciency of the plasma combined with catalyst can reach 78.6%,which is 18.4%higher than that of plasma without catalyst.When the applied voltage is 30 k V,the gas flow rate is 1 l min^(-1),the oxygen ratio is 1%and the plasma combined with TiO_(2)catalyst treats the sample for 5 min the degradation efflciency of TIA reached 97%.It can be concluded that a higher applied voltage and longer processing times not only lead to more degradation but also result in a lower energy efflciency.Decreasing the oxygen ratio and gas flow rate could improve the degradation efflciency.The relative distribution and identity of the major TIA degradation product generated was determined by high-performance liquid chromatography–mass spectrometry analysis.The mechanism of TIA removal by plasma and TiO_(2)catalyst was analyzed,and the possible degradation path is discussed.
基金Project supported by the Major Program and State Key Program of National Natural Science of China (Grant Nos 60890191 and 60736033)the National Key Science & Technology Special Project (Grant No 2008ZX 01002)
文摘This paper finds that the two-dimensional electron gas density in high Al-content A1GaN/GaN heterostructures exhibits an obvious time-dependent degradation after the epitaxial growth. The degradation mechanism was investigated in depth using Hall effect measurements,high resolution x-ray diffraction,scanning electron microscopy,x-ray photoelectron spectroscopy and energy dispersive x-ray spectroscopy.The results reveal that the formation of surface oxide is the main reason for the degradation,and the surface oxidation always occurs within the surface hexagonal defects for high Al-content AlGaN/GaN heterostructures.
文摘Degradation reaction of doxycycline or methacycline was carried out in KOH solution and intense fluorescence was obtained.A degradation mechanism of doxycycline or methacycline was suggested.
基金Supported by the National Natural Science Foundation of China under Grant No 11104331the National Basic Research Program of China under Grant No 2011CB921702
文摘Systemic measurements show that there is no 3D to 2D crossover in the reduction of the superconducting transition temperature Tc in Nb thin films. This result is consistent with all previous measurements while it is contrary to the prevailing understanding based on the interplay between proximity, localization, and lifetime broadening. Our study indicates that the decrease of Tc can be interpreted by the combined effects of electron-phonon coupling parameter λ and the defect scattering rate pw, being uniquely determined by their ratio λ/ρw. Other factors such as film thickness and irradiation do not produce additional effects beyond these two parameters.
基金supported by National Natural Science Foundation of China(Grant No.52207155).
文摘SF_(6)degradation mechanism in non-thermal plasma(NTP)systems is not fully understood due to the formation of a complex physico-chemical reaction network,especially when reactive gases and packing materials are involved.In this work,we conduct a combined experimental and theoretical study to unravel the SF_(6)degradation path in a-Al_(2)O_(3)packed plasma in the presence of H_(2)O or O_(2).Our experimental results show that both H_(2)O and O_(2)have a synergetic effect with-Al_(2)O_(3)packing on promoting SF_(6)degradation,leading to higher stable gas yields than typical spark or corona discharges.H_(2)O or O_(2)addition promotes SO_(2)or SO_(2)F_(2)selectivity,respectively.Density functional theory(DFT)calculations reveal that SO_(2)generation corresponding with the highest activation barrier is the most critical step toward SF_(6)degradation.Radicals like H and O generated from H_(2)O or O_(2)discharge can significantly promote the degradation process via Eley-Rideal mechanism,affecting key reactions of stable product generation,advancing degradation efficiency.The results of this work could provide insights on further understanding SF_(6)degradation mechanism especially in packed-bed plasma systems.
基金funded by the UK Research Council EPSRC EP/009050/1。
文摘High-temperature proton exchange membrane fuel cells(HT-PEMFCs)are pursued worldwide as efficient energy conversion devices.Great efforts have been made in the area of designing and developing phosphoric acid(PA)-based proton exchange membrane(PEM)of HT-PEMFCs.This review focuses on recent advances in the limitations of acid-based PEM(acid leaching,oxidative degradation,and mechanical degradation)and the approaches mitigating the membrane degradation.Preparing multilayer or polymers with continuous network,adding hygroscopic inorganic materials,and introducing PA doping sites or covalent interactions with PA can effectively reduce acid leaching.Membrane oxidative degradation can be alleviated by synthesizing crosslinked or branched polymers,and introducing antioxidative groups or highly oxidative stable materials.Crosslinking to get a compact structure,blending with stable polymers and inorganic materials,preparing polymer with high molecular weight,and fabricating the polymer with PA doping sites away from backbones,are recommended to improve the membrane mechanical strength.Also,by comparing the running hours and decay rate,three current approaches,1.crosslinking via thermally curing or polymeric crosslinker,2.incorporating hygroscopic inorganic materials,3.increasing membrane layers or introducing strong basic groups and electron-withdrawing groups,have been concluded to be promising approaches to improve the durability of HT-PEMFCs.The overall aim of this review is to explore the existing degradation challenges and opportunities to serve as a solid basis for the deployment in the fuel cell market.
基金Project supported by the National Basic Research Program of China (Grant No. 2011CBA00600)the National Natural Science Foundation of China (Grant No. 61106106)the Fundamental Research Funds for the Central Universities (Grant No. K50510250006)
文摘In spite of their extraordinary performance, AlGaN/GaN high electron mobility transistors (HEMTs) still lack solid reliability. Devices under accelerated DC stress tests (off-state, VDS = 0 state, and on-state step-stress) are investigated to help us identify the degradation mechanisms of the AlGaN/GaN HEMTs. All our findings are consistent with the degradation mechanism based on crystallographic-defect formation due to the inverse piezoelectric effects in Ref. [1] (Joh J and del Alamo J A 2006 IEEE IDEM Tech. Digest p. 415). However, under the on-state condition, the devices are suffering from both inverse piezoelectric effects and hot electron effects, and so to improve the reliability of the devices both effects should be taken into consideration.