Pitch produced by the lique-faction of coal was divided into two frac-tions:soluble in toluene(TS)and insol-uble in toluene but soluble in pyridine(TI-PS),and their differences in molecu-lar structure and oxidation ac...Pitch produced by the lique-faction of coal was divided into two frac-tions:soluble in toluene(TS)and insol-uble in toluene but soluble in pyridine(TI-PS),and their differences in molecu-lar structure and oxidation activity were studied.Several different carbon materi-als were produced from them by oxida-tion in air(350℃,300 mL/min)fol-lowed by carbonization(1000℃ in Ar),and the effect of the cross-linked structure on their structure and sodium storage properties was investigated.The results showed that the two pitch fractions were obviously different after the air oxidation.The TS fraction with a low degree of condensation and abundant side chains had a stronger oxidation activity and thus introduced more cross-linked oxygen-containing functional groups C(O)―O which prevented carbon layer rearrangement during the carbonization.As a result,a disordered hard carbon with more defects was formed,which improved the electrochemical performance.Therefore,the carbon materials derived from TS(O-TS-1000)had an obvious disordered structure and a larger layer spacing,giving them better sodium storage perform-ance than those derived from the TI-PS fraction(O-TI-PS-1000).The specific capacity of O-TS-1000 was about 250 mAh/g at 20 mA/g,which was 1.67 times higher than that of O-TI-PS-1000(150 mAh/g).展开更多
The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation ...The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation and oxygen evolution competition,sluggish kinetics,low Faradaic efficiency,and limited nitrate yields.In this work,a novel two-dimensional(2D)layered MOF Mn-BCPPy(H_(2)BCPPy=3,5-di(4'-carboxyphenyl)pyridine)has been successfully synthesized.The framework is composed of a rod-manganese motifs and possesses abundant active sites including open metal sites(OMSs)and Lewis base sites(LBSs).The Mn-BCPPy is the first MOF catalyst applied in electrocatalytic NOR which NO_(3)^(-)exhibited relatively high activity with a yield of 99.75μg/(h·mg)and a Faraday efficiency(FE)of 32.09%.Furthermore,it can be used as fluorescent sensor for selectively and sensitively detect nitrofuran antibiotics(NFs).Therefore,this work explores the application of MOF materials in the field of electrocatalytic NOR,which reveals that manganese-based MOFs have great potential prospects.展开更多
To improve the oxidation resistance of HfB_(2)-SiC coatings on carbon/carbon composites at 1700°C in air,CeO_(2) was introduced to improve oxygen blocking and its mechanism was investigated.During the rapid oxida...To improve the oxidation resistance of HfB_(2)-SiC coatings on carbon/carbon composites at 1700°C in air,CeO_(2) was introduced to improve oxygen blocking and its mechanism was investigated.During the rapid oxidation stage,CeO_(2) accelerated the formation of a multiphase glass layer on the coating surface.The maximum oxidation rates of CeO_(2)-HfB2-SiC coatings with 1%,3%,and 5%CeO_(2) were 24.1%,20.3%,and 53.2%higher than that of the unmodified HfB2-SiC coating,respectively.In the stable oxidation stage,the maximum oxidation rates of coatings with 1%and 3%CeO_(2) decreased by 31.4%and 21.9%,respectively,demonstrating adequate inert protection.CeO_(2) is a“coagulant”and“stabilizer”in the composite glass layer.However,increasing the CeO_(2) content accelerates the reaction between the SiO_(2) glass phase and SiC,leading to a higher SiO_(2) consumption and reduced self-healing ability of the glass layer.The 1%CeO_(2)-60%HfB2-39%SiC coating showed improved glass layer viscosity and stability,moderate SiO_(2) consumption,and better self-healing ability,significantly boosting the oxidation protection of the coating.展开更多
Applying bio-oxidation waste solution(BOS)to chemical-biological two-stage oxidation process can significantly improve the bio-oxidation efficiency of arsenopyrite.This study aims to clarify the enhanced oxidation mec...Applying bio-oxidation waste solution(BOS)to chemical-biological two-stage oxidation process can significantly improve the bio-oxidation efficiency of arsenopyrite.This study aims to clarify the enhanced oxidation mechanism of arsenopyrite by evaluating the effects of physical and chemical changes of arsenopyrite in BOS chemical oxidation stage on mineral dissolution kinetics,as well as microbial growth activity and community structure composition in bio-oxidation stage.The results showed that the chemical oxidation contributed to destroying the physical and chemical structure of arsenopyrite surface and reducing the particle size,and led to the formation of nitrogenous substances on mineral surface.These chemical oxidation behaviors effectively promoted Fe^(3+)cycling in the bio-oxidation system and weakened the inhibitory effect of the sulfur film on ionic diffusion,thereby enhancing the dissolution kinetics of the arsenopyrite.Therefore,the bio-oxidation efficiency of arsenopyrite was significantly increased in the two-stage oxidation process.After 18 d,the two-stage oxidation process achieved total extraction rates of(88.8±2.0)%,(86.7±1.3)%,and(74.7±3.0)%for As,Fe,and S elements,respectively.These values represented a significant increase of(50.8±3.4)%,(47.1±2.7)%,and(46.0±0.7)%,respectively,compared to the one-stage bio-oxidation process.展开更多
Silicon-carbide-fiber-reinforced silicon-carbide-ceramic-based matrix(SiC/SiC)composites possess excellent properties such as low density,high strength and high temperature resistance,showing a potential application f...Silicon-carbide-fiber-reinforced silicon-carbide-ceramic-based matrix(SiC/SiC)composites possess excellent properties such as low density,high strength and high temperature resistance,showing a potential application for structural components in the aerospace field,but their oxidation behavior remains largely unknown.In this study,Yb_(2)Si_(2)O_(7)modified SiC/SiC(SiC/SiC-Yb_(2)Si_(2)O_(7))mini-composites were prepared by introducing Yb_(2)Si_(2)O_(7)as anti-oxidation phase into SiC fiber bundles via Sol-Gel and depositing SiC matrix by chemical vapor deposition(CVD).Influence of Yb_(2)Si_(2)O_(7)on microstructure,mechanical property and oxidation behavior of SiC/SiC mini-composites was investigated.The results showed that after oxidation in air at 1200 and 1400℃for 50 h,the tensile strength retentions of SiC/SiC mini-composites were 77%and 69%,respectively,and the fracture morphology exhibited flat.The Yb_(2)Si_(2)O_(7)introduced by Sol-Gel partially distributed in layers,contributing to the toughening of the material.On the fracture surface,there was interlayer debonding,which extended energy dissipation mechanism of SiC/SiC mini-composites.Tensile strength of SiC/SiC-Yb_(2)Si_(2)O_(7)mini-composites at room temperature was 484 MPa.After oxidation in air at 1200 and 1400℃for 50 h,the tensile strengths decreased to 425 and 374 MPa,resulting in retention rates of 88%and 77%,respectively.It displayed typical non-brittle fracture characteristics.The interface oxygen content of SiC/SiC mini-composites at the fracture surface was higher than that of SiC/SiC-Yb_(2)Si_(2)O_(7)mini-composites,indicating that introduction of Yb_(2)Si_(2)O_(7)could alleviate oxygen diffusion towards the interface,and therefore improve the oxidation resistance of SiC/SiC-Yb_(2)Si_(2)O_(7)mini-composites.展开更多
Microarc oxidation is an effective surface treatment for improving certain properties of metals and their alloys.In this paper,TiO_(2)/Cu_(2)O and TiO_(2)/Cu_(2)O@CeO_(2)coatings were prepared on Ti-6Al-4V by microarc...Microarc oxidation is an effective surface treatment for improving certain properties of metals and their alloys.In this paper,TiO_(2)/Cu_(2)O and TiO_(2)/Cu_(2)O@CeO_(2)coatings were prepared on Ti-6Al-4V by microarc oxidation.Thecoatings exhibited good corrosion resistance and antimicrobial properties.X-ray diffraction(XRD),scanning electronmicroscopy(SEM),and 3D laser confocal were used to characterize the coatings.The properties of TiO_(2)/Cu_(2)O and TiO_(2)/Cu_(2)O@CeO_(2)coatings were analyzed,including microstructure,surface roughness,corrosion resistance,andantimicrobial properties.The electrochemical results showed that the coatings prepared by microarc oxidation hadenhanced corrosion resistance compared to the substrate.The antibacterial properties of TiO_(2)/Cu_(2)O and TiO_(2)/Cu_(2)O@CeO_(2)coating against Pseudomonas aeruginosa were evaluated by fluorescence microscopy and plate counting.The antibacterial rate of TiO_(2)/Cu_(2)O@CeO_(2)coating was up to 99.70%.In summary,the TiO_(2)/Cu_(2)O and TiO_(2)/Cu_(2)O@CeO_(2)coatings prepared by microarc oxidation have a potential application background in the field of marine corrosionprotection and biofouling.展开更多
The oxidation behavior of ferrovanadium spinel(FeV_(2)O_(4)),synthesized via high-temperature solid-state reaction,was investigated using thermogravimetry,X-ray diffractometry,and X-ray photoelectron spectroscopy over...The oxidation behavior of ferrovanadium spinel(FeV_(2)O_(4)),synthesized via high-temperature solid-state reaction,was investigated using thermogravimetry,X-ray diffractometry,and X-ray photoelectron spectroscopy over the temperature range of 450–700℃.The results revealed that the oxidation process of FeV_(2)O_(4)can be divided into three stages with the second stage being responsible for maximum weight gain due to oxidation.Three classical methods were employed to analyze the reaction mechanisms and model functions for distinct oxidation stages.The random nucleation and subsequent growth(A_(3))kinetic model was found to be applicable to both initial and secondary stage.The third stage of oxidation was consistent with the three-dimensional diffusion,spherical symmetry(D_(3))kinetic mode.Both the model-function method and the model-free method were utilized to investigate the apparent activation energy of the oxidation reaction at each stage.It was found that the intermediates including Fe_(3)O_(4),VO_(2),V_(2)O_(3),and Fe_(2.5)V_(7.11)O_(16),played significant roles in the oxidation process prior to the final formation of FeVO_(4)and V_(2)O_(5)through oxidation of FeV_(2)O_(4).展开更多
Micro-arc oxidation(MAO)technique is capable of producing dense oxide films on the aluminium alloy surface.This oxide film protects the aluminium alloy from the corrosion attack for longer duration.Empirical relations...Micro-arc oxidation(MAO)technique is capable of producing dense oxide films on the aluminium alloy surface.This oxide film protects the aluminium alloy from the corrosion attack for longer duration.Empirical relationships were derived to evaluate the MAO coating properties(porosity and hardness)by incorporating very important MAO parameters(current density,inter-electrode distance and oxidation time).MAO parameters were also optimized to achieve coatings with minimum porosity and maximum hardness.Further,the effect of MAO parameters on coating characteristics was analysed.From the results,it is found that the current density has greater influence on the responses than the other two parameters.展开更多
Electro-copolymerized film containing ruthenium complexes as electron-transfer(or redox)mediators and water-oxidation catalysts by an oxidative copolymerization method is presented.The addition of the redox mediator s...Electro-copolymerized film containing ruthenium complexes as electron-transfer(or redox)mediators and water-oxidation catalysts by an oxidative copolymerization method is presented.The addition of the redox mediator significantly improved the electrocatalytic water-oxidation activity and reduced the overpotential to 220 mV.The prepared electrode showed a water-oxidation catalytic rate constant kobs of 31.7 s^(-1)and an initial turnover frequency of 1.01 s^(-1)in 1000 s by potential electrolysis at 1.7 V applied bias vs NHE(normal hydrogen electrode).The kinetic isotope effect study suggests that the catalytic water oxidation reaction on the electrode surface occurs via a bimolecular coupling mechanism.展开更多
Biomass-derived platform molecules,such as furfural,are abundant and renewable feedstock for valuable chemical production.It is critical to synthesize highly efficient photocatalysts for selective oxidation under visi...Biomass-derived platform molecules,such as furfural,are abundant and renewable feedstock for valuable chemical production.It is critical to synthesize highly efficient photocatalysts for selective oxidation under visible light.The Er@K-C_(3)N_(4)/UiO-66-NH_(2) catalyst was synthesized using a straight-forward hydrothermal technique,and exhibited exceptional efficiency in the photocatalytic oxidation of furfural to furoic acid.The catalyst was thoroughly characterized,confirming the effective adjustment of the band gap energy of Er@K-C_(3)N_(4)/UiO-66-NH_(2).Upon the optimized reaction conditions,the conversion rate of furfural reached 89.3%,with a corresponding yield of furoic acid at 79.8%.The primary reactive oxygen species was identified as·O_(2)^(-) from ESR spectra and scavenger tests.The incorporation of Er and K into the catalyst enhanced the photogenerated carriers transfer rate,hence increasing the separating efficiency of photogenerated electron-hole pairs.This study expands the potential applications of rare earth element doped g-C_(3)N_(4) in the photocatalytic selective oxidation of furfurans.展开更多
ZrB_(2)-based ceramics typically necessitate high temperature and pressure for sintering,whereas ZrB_(2)-SiC ceramics can be fabricated at 1500℃using the process of reactive melt infiltration with Si.In comparison to...ZrB_(2)-based ceramics typically necessitate high temperature and pressure for sintering,whereas ZrB_(2)-SiC ceramics can be fabricated at 1500℃using the process of reactive melt infiltration with Si.In comparison to the conventional preparation method,reactive synthesis allows for the more facile production of ultra-high temperature ceramics with fine particle size and homogeneous composition.In this work,ZrSi_(2),B4C,and C were used as raw materials to prepare ZrB_(2)-SiC via combination of tape casting and reactive melt infiltration herein referred to as ZBC ceramics.Control sample of ZrB_(2)-SiC was also prepared using ZrB_(2)and SiC as raw materials through an identical process designated as ZS ceramics.Microscopic analysis of both ceramic groups revealed smaller and more uniformly distributed particles of the ZrB_(2)phase in ZBC ceramics compared to the larger particles in ZS ceramics.Both sets of ceramics underwent cyclic oxidation testing in the air at 1600℃for a cumulative duration of 5 cycles,each cycle lasting 2 h.Analysis of the oxidation behavior showed that both ZBC ceramics and ZS ceramics developed a glassy SiO_(2)-ZrO_(2)oxide layer on their surfaces during the oxidation.This layer severed as a barrier against oxygen.In ZBC ceramics,ZrO_(2)is finely distributed in SiO_(2),whereas in ZS ceramics,larger ZrO_(2)particles coexist with glassy SiO_(2).The surface oxide layer of ZBC ceramics maintains a dense structure because the well-dispersed ZrO_(2)increases the viscosity of glassy SiO_(2),preventing its crystallization during the cooling.Conversely,some SiO_(2)in the oxide layer of ZS ceramics may crystallize and form a eutectic with ZrO_(2),leading to the formation of ZrSiO_(4).This leads to cracking of the oxide layer due to differences in thermal expansion coefficients,weakening its barrier effect.An analysis of the oxidation resistance shows that ZBC ceramics exhibit less increase in oxide layer thickness and mass compared to ZS ceramics,suggesting superior oxidation resistance of ZBC ceramics.展开更多
Reversible solid oxide cell(RSOC)is a new energy conversion device with significant applications,especially for power grid peaking shaving.However,the reversible conversion process of power generation/energy storage p...Reversible solid oxide cell(RSOC)is a new energy conversion device with significant applications,especially for power grid peaking shaving.However,the reversible conversion process of power generation/energy storage poses challenges for the performance and stability of air electrodes.In this work,a novel high-entropy perovskite oxide La_(0.2)Pr_(0.2)Gd_(0.2)Sm_(0.2)Sr_(0.2)Co_(0.8)Fe_(0.2)O_(3−δ)(HE-LSCF)is proposed and investigated as an air electrode in RSOC.The electrochemical behavior of HE-LSCF was studied as an air electrode in both fuel cell and electrolysis modes.The polarization impedance(Rp)of the HE-LSCF electrode is only 0.25Ω·cm^(2) at 800℃ in an air atmosphere.Notably,at an electrolytic voltage of 2 V and a temperature of 800℃,the current density reaches up to 1.68 A/cm^(2).The HE-LSCF air electrode exhibited excellent reversibility and stability,and its electrochemical performance remains stable after 100 h of reversible operation.With these advantages,HE-LSCF is shown to be an excellent air electrode for RSOC.展开更多
Formic acid oxidation reaction(FAOR),as the anodic reaction in direct formic acid fuel cells,has attracted much attention but increasing the mass activity and stability of catalysts still face a bottleneck to meet the...Formic acid oxidation reaction(FAOR),as the anodic reaction in direct formic acid fuel cells,has attracted much attention but increasing the mass activity and stability of catalysts still face a bottleneck to meet the requirements of practical applications.In the past decades,researchers developed many strategies to fix these issues by improving the structure of catalysts and the newly raised single atom catalysts(SACs)show the high mass activity and stability in FAOR.This review first summarized the reaction mechanism involved in FAOR.The mass activity as well as stability of catalysts reported in the past five years have been outlined.Moreover,the synthetic strategies to improve the catalytic performance of catalysts are also reviewed in this work.Finally,we proposed the research directions to guide the rational design of new FAOR catalysts in the future.展开更多
Inducing the classic strong metal-support interaction(SMSI)is an effective approach to enhance the performance of supported metal catalysts by encapsulating the metal nanoparticles(NPs)with supports.Conventional therm...Inducing the classic strong metal-support interaction(SMSI)is an effective approach to enhance the performance of supported metal catalysts by encapsulating the metal nanoparticles(NPs)with supports.Conventional thermal reduction method for inducing SMSI processes is often accompanied by undesirable structural evolution of metal NPs.In this study,a mild electrochemical method has been developed as a new approach to induce SMSI,using the cable structured core@shell CNT@SnO_(2) loaded Pt NPs as a proof of concept.The induced SnO_(x) encapsulation layer on the surface of Pt NPs can protect Pt NPs from the poisoned of CO impurity in hydrogen oxidation reaction(HOR),and the HOR current density could still maintain 85% for 2000 s with 10,000 ppm CO in H_(2),while the commercial Pt/C is completely inactivated.In addition,the electrons transfer from SnO_(x) to Pt NPs improved the HOR activity of the E-Pt-CNT@SnO_(2),achieving the excellent exchange current density of 1.55 A·mgPt^(-1).In situ Raman spectra and theoretical calculations show that the key to the electrochemical-method-induced SMSI is the formation of defects and the migration of SnO_(x) caused by the electrochemical redox operation,and the weakening the SneO bond strength by Pt NPs.展开更多
In pursuit of more efficient and stable electrochemical energy storage materials,composite materials consisting of metal oxides and graphene oxide have garnered significant attention due to their unique structures and...In pursuit of more efficient and stable electrochemical energy storage materials,composite materials consisting of metal oxides and graphene oxide have garnered significant attention due to their unique structures and exceptional properties.Graphene oxide(GO),a two-dimensional material with an extremely high specific surface area and excellent conductivity,offers new possibilities for enhancing the electrochemical performance of metal oxides.In this work,we synthesized met-al-organic framework(MOF)and GO composites by regulating the amount of GO,and successfully prepared composites of metal oxides supported by nitrogen-doped carbon frameworks and GO through a simple one-step calcination process.Based on the electrochemical tests,the optimal amount of GO was determined.This research will provide new insights into and directions for designing and synthesizing metal oxide and graphene oxide composite materials with an ideal electro-chemical performance.展开更多
Graphene oxide nanomaterials are increasingly used in various fields due to their superior properties.In order to study the influence of graphene oxide additives on the performance of modified asphalt,in this study,gr...Graphene oxide nanomaterials are increasingly used in various fields due to their superior properties.In order to study the influence of graphene oxide additives on the performance of modified asphalt,in this study,graphene oxide modified asphalt was prepared and characteristics was studied including the high deformation resistance performance and the self-healing property of modified asphalt.Functional groups and morphology of graphene oxide modified asphalt were described by Fourier transform infrared spectroscopy.The high deformation resistance performance and self-healing effect of asphalt samples were obtained through dynamic slear rheometer(DSR)test.Results shows that graphene oxide dispersions improve the performance of asphalt relatively well compared to graphene oxide powder.There is no chemical reaction between graphene oxide and asphalt,but physical connection.The addition of graphene oxide improved the high deformation resistance of modified asphalt and expedited the self-healing ability of asphalt under fatigue load.展开更多
With the aim to effectively depolymerize polyethylene terephthalate(PET)under mild reaction conditions,PET methanolysis and dimethyl terephthalate(DMT)hydrolysis are integrated in a catalyst system.Firstly,methanolysi...With the aim to effectively depolymerize polyethylene terephthalate(PET)under mild reaction conditions,PET methanolysis and dimethyl terephthalate(DMT)hydrolysis are integrated in a catalyst system.Firstly,methanolysis of PET to DMT is achieved over Cu-Mg-Al oxide catalyst.Next,terephthalic acid(TPA)is prepared by DMT hydrolysis.It is found that hydrolysis of DMT to TPA can be promoted by introducing trace amount of water in this catalyst system.CuO-MgO-4.5Al_2O_(3)catalyst demonstrates the excellent catalytic performance for the depolymerization of PET with high conversion rate and TPA yield(100%and 99.5%,respectively)after reaction at 160℃for 6 h,which provides a new idea for the depolymerization of PET.展开更多
ZnO thin films with varying Ta concentrations were fabricated through magnetron sputtering.The crystallinity and surface morphology of the ZnO films are significantly influenced by the incorporation of Ta,as evidenced...ZnO thin films with varying Ta concentrations were fabricated through magnetron sputtering.The crystallinity and surface morphology of the ZnO films are significantly influenced by the incorporation of Ta,as evidenced by the X-ray diffraction and scanning electron microscopy results.The lattice constants,as determined by X-ray diffraction,contradict the disparity in Ta and Zn ion radii,which is attributed to the impact of interstitial defects.This inconsistency introduces variations in carrier concentration in this experiment compared with prior studies.Subsequent exploration of the luminescent characteristics and emission mechanism of defect levels in Ta-doped ZnO films was conducted through photoluminescence.Furthermore,the factors influencing the bandgap are discussed.展开更多
Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-p...Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-phase method as the cathode for CO_(2)electrolysis by SOECs.XRD confirms that SFMSc exhibits a stable cubic phase crystal structure.The experimental results of TPD,TG,EPR,CO_(2)-TPD further demonstrate that Sc-doping increases the concentration of oxygen vacancy in the material and the chemical adsorption capacity of CO_(2)molecules.Electrochemical tests reveal that SFMSc single cell achieves a current density of 2.26 A/cm^(2) and a lower polarization impedance of 0.32Ω·cm^(2) at 800°C under the applied voltage of 1.8 V.And no significant performance attenuation or carbon deposition is observed after 80 h continuous long-term stability test.This study provides a favorable support for the development of SOEC cathode materials with good electro-catalytic performance and stability.展开更多
文摘Pitch produced by the lique-faction of coal was divided into two frac-tions:soluble in toluene(TS)and insol-uble in toluene but soluble in pyridine(TI-PS),and their differences in molecu-lar structure and oxidation activity were studied.Several different carbon materi-als were produced from them by oxida-tion in air(350℃,300 mL/min)fol-lowed by carbonization(1000℃ in Ar),and the effect of the cross-linked structure on their structure and sodium storage properties was investigated.The results showed that the two pitch fractions were obviously different after the air oxidation.The TS fraction with a low degree of condensation and abundant side chains had a stronger oxidation activity and thus introduced more cross-linked oxygen-containing functional groups C(O)―O which prevented carbon layer rearrangement during the carbonization.As a result,a disordered hard carbon with more defects was formed,which improved the electrochemical performance.Therefore,the carbon materials derived from TS(O-TS-1000)had an obvious disordered structure and a larger layer spacing,giving them better sodium storage perform-ance than those derived from the TI-PS fraction(O-TI-PS-1000).The specific capacity of O-TS-1000 was about 250 mAh/g at 20 mA/g,which was 1.67 times higher than that of O-TI-PS-1000(150 mAh/g).
基金supported by Natural Science Foundation of Shandong Province(ZR2021MB075)Fundamental Research Funds for the Central Universities,Ocean University of China(202461021).
文摘The electrocatalytic nitrogen oxidation reaction(NOR)is a sustainable approach for converting N_(2)to NO_(3)^(-)under mild conditions.However,it still faces challenges including inefficient N_(2)absorption/activation and oxygen evolution competition,sluggish kinetics,low Faradaic efficiency,and limited nitrate yields.In this work,a novel two-dimensional(2D)layered MOF Mn-BCPPy(H_(2)BCPPy=3,5-di(4'-carboxyphenyl)pyridine)has been successfully synthesized.The framework is composed of a rod-manganese motifs and possesses abundant active sites including open metal sites(OMSs)and Lewis base sites(LBSs).The Mn-BCPPy is the first MOF catalyst applied in electrocatalytic NOR which NO_(3)^(-)exhibited relatively high activity with a yield of 99.75μg/(h·mg)and a Faraday efficiency(FE)of 32.09%.Furthermore,it can be used as fluorescent sensor for selectively and sensitively detect nitrofuran antibiotics(NFs).Therefore,this work explores the application of MOF materials in the field of electrocatalytic NOR,which reveals that manganese-based MOFs have great potential prospects.
文摘To improve the oxidation resistance of HfB_(2)-SiC coatings on carbon/carbon composites at 1700°C in air,CeO_(2) was introduced to improve oxygen blocking and its mechanism was investigated.During the rapid oxidation stage,CeO_(2) accelerated the formation of a multiphase glass layer on the coating surface.The maximum oxidation rates of CeO_(2)-HfB2-SiC coatings with 1%,3%,and 5%CeO_(2) were 24.1%,20.3%,and 53.2%higher than that of the unmodified HfB2-SiC coating,respectively.In the stable oxidation stage,the maximum oxidation rates of coatings with 1%and 3%CeO_(2) decreased by 31.4%and 21.9%,respectively,demonstrating adequate inert protection.CeO_(2) is a“coagulant”and“stabilizer”in the composite glass layer.However,increasing the CeO_(2) content accelerates the reaction between the SiO_(2) glass phase and SiC,leading to a higher SiO_(2) consumption and reduced self-healing ability of the glass layer.The 1%CeO_(2)-60%HfB2-39%SiC coating showed improved glass layer viscosity and stability,moderate SiO_(2) consumption,and better self-healing ability,significantly boosting the oxidation protection of the coating.
基金Project(52274348)supported by the National Natural Science Foundation of ChinaProject(2022JH1/10400024)supported by the Major Projects for the“Revealed Top”Science and Technology of Liaoning Province,China。
文摘Applying bio-oxidation waste solution(BOS)to chemical-biological two-stage oxidation process can significantly improve the bio-oxidation efficiency of arsenopyrite.This study aims to clarify the enhanced oxidation mechanism of arsenopyrite by evaluating the effects of physical and chemical changes of arsenopyrite in BOS chemical oxidation stage on mineral dissolution kinetics,as well as microbial growth activity and community structure composition in bio-oxidation stage.The results showed that the chemical oxidation contributed to destroying the physical and chemical structure of arsenopyrite surface and reducing the particle size,and led to the formation of nitrogenous substances on mineral surface.These chemical oxidation behaviors effectively promoted Fe^(3+)cycling in the bio-oxidation system and weakened the inhibitory effect of the sulfur film on ionic diffusion,thereby enhancing the dissolution kinetics of the arsenopyrite.Therefore,the bio-oxidation efficiency of arsenopyrite was significantly increased in the two-stage oxidation process.After 18 d,the two-stage oxidation process achieved total extraction rates of(88.8±2.0)%,(86.7±1.3)%,and(74.7±3.0)%for As,Fe,and S elements,respectively.These values represented a significant increase of(50.8±3.4)%,(47.1±2.7)%,and(46.0±0.7)%,respectively,compared to the one-stage bio-oxidation process.
基金National Natural Science Foundation of China(52222202)National Key R&D Program of China(2022YFB3707700)+2 种基金Project of Shanghai Science and Technology Innovation Action Plan(21511104800)Shanghai Pilot Program for Basic Research-Chinese Academy of Science,Shanghai Branch(JCYJ-SHFY-2021-001)Science Center for Gas Turbine Project(P2022-B-Ⅳ-001-001)。
文摘Silicon-carbide-fiber-reinforced silicon-carbide-ceramic-based matrix(SiC/SiC)composites possess excellent properties such as low density,high strength and high temperature resistance,showing a potential application for structural components in the aerospace field,but their oxidation behavior remains largely unknown.In this study,Yb_(2)Si_(2)O_(7)modified SiC/SiC(SiC/SiC-Yb_(2)Si_(2)O_(7))mini-composites were prepared by introducing Yb_(2)Si_(2)O_(7)as anti-oxidation phase into SiC fiber bundles via Sol-Gel and depositing SiC matrix by chemical vapor deposition(CVD).Influence of Yb_(2)Si_(2)O_(7)on microstructure,mechanical property and oxidation behavior of SiC/SiC mini-composites was investigated.The results showed that after oxidation in air at 1200 and 1400℃for 50 h,the tensile strength retentions of SiC/SiC mini-composites were 77%and 69%,respectively,and the fracture morphology exhibited flat.The Yb_(2)Si_(2)O_(7)introduced by Sol-Gel partially distributed in layers,contributing to the toughening of the material.On the fracture surface,there was interlayer debonding,which extended energy dissipation mechanism of SiC/SiC mini-composites.Tensile strength of SiC/SiC-Yb_(2)Si_(2)O_(7)mini-composites at room temperature was 484 MPa.After oxidation in air at 1200 and 1400℃for 50 h,the tensile strengths decreased to 425 and 374 MPa,resulting in retention rates of 88%and 77%,respectively.It displayed typical non-brittle fracture characteristics.The interface oxygen content of SiC/SiC mini-composites at the fracture surface was higher than that of SiC/SiC-Yb_(2)Si_(2)O_(7)mini-composites,indicating that introduction of Yb_(2)Si_(2)O_(7)could alleviate oxygen diffusion towards the interface,and therefore improve the oxidation resistance of SiC/SiC-Yb_(2)Si_(2)O_(7)mini-composites.
基金Projects(41827805,41976044)supported by the National Natural Science Foundation of ChinaProject(ZDYF2021GXJS210)supported by the Hainan Provincial Science and Technology Special Fund,China+2 种基金Project(2021CXLH0005)supported by the Hainan Provincial Joint Project of Sanya Yazhou Bay Science and Technology City,ChinaProject(2021WHZZB2301)supported by the Wenhai Program of the S&T Fund of Shandong Province for Pilot National Laboratory for Marine Science and Technology,ChinaProject(121311KYSB20210005)supported by the Overseas Science and Education Centers of Bureau of International Cooperation Chinese Academy of Sciences。
文摘Microarc oxidation is an effective surface treatment for improving certain properties of metals and their alloys.In this paper,TiO_(2)/Cu_(2)O and TiO_(2)/Cu_(2)O@CeO_(2)coatings were prepared on Ti-6Al-4V by microarc oxidation.Thecoatings exhibited good corrosion resistance and antimicrobial properties.X-ray diffraction(XRD),scanning electronmicroscopy(SEM),and 3D laser confocal were used to characterize the coatings.The properties of TiO_(2)/Cu_(2)O and TiO_(2)/Cu_(2)O@CeO_(2)coatings were analyzed,including microstructure,surface roughness,corrosion resistance,andantimicrobial properties.The electrochemical results showed that the coatings prepared by microarc oxidation hadenhanced corrosion resistance compared to the substrate.The antibacterial properties of TiO_(2)/Cu_(2)O and TiO_(2)/Cu_(2)O@CeO_(2)coating against Pseudomonas aeruginosa were evaluated by fluorescence microscopy and plate counting.The antibacterial rate of TiO_(2)/Cu_(2)O@CeO_(2)coating was up to 99.70%.In summary,the TiO_(2)/Cu_(2)O and TiO_(2)/Cu_(2)O@CeO_(2)coatings prepared by microarc oxidation have a potential application background in the field of marine corrosionprotection and biofouling.
基金Project(cstb2022nscq-msx0801)supported by the Natural Science Foundation of Chongqing,ChinaProject(52004044)supported by the National Natural Science Foundation of China+2 种基金Project(ckrc2022030)supported by the Foundation of Chongqing University of Science and Technology,ChinaProject(YKJCX2220216)supported by the Graduate Research Innovation Project of Chongqing University of Science and Technology,ChinaProject(202311551007)supported by the National Undergraduate Training Program for Innovation and Entrepreneurship,China。
文摘The oxidation behavior of ferrovanadium spinel(FeV_(2)O_(4)),synthesized via high-temperature solid-state reaction,was investigated using thermogravimetry,X-ray diffractometry,and X-ray photoelectron spectroscopy over the temperature range of 450–700℃.The results revealed that the oxidation process of FeV_(2)O_(4)can be divided into three stages with the second stage being responsible for maximum weight gain due to oxidation.Three classical methods were employed to analyze the reaction mechanisms and model functions for distinct oxidation stages.The random nucleation and subsequent growth(A_(3))kinetic model was found to be applicable to both initial and secondary stage.The third stage of oxidation was consistent with the three-dimensional diffusion,spherical symmetry(D_(3))kinetic mode.Both the model-function method and the model-free method were utilized to investigate the apparent activation energy of the oxidation reaction at each stage.It was found that the intermediates including Fe_(3)O_(4),VO_(2),V_(2)O_(3),and Fe_(2.5)V_(7.11)O_(16),played significant roles in the oxidation process prior to the final formation of FeVO_(4)and V_(2)O_(5)through oxidation of FeV_(2)O_(4).
基金Council of Scientific and Industrial Research(G8/19901/2013)New Delhi for the financial support provided to conduct this investigation through sponsored project No.22(0615)/13/EMR-II dated 26.02.2013
文摘Micro-arc oxidation(MAO)technique is capable of producing dense oxide films on the aluminium alloy surface.This oxide film protects the aluminium alloy from the corrosion attack for longer duration.Empirical relationships were derived to evaluate the MAO coating properties(porosity and hardness)by incorporating very important MAO parameters(current density,inter-electrode distance and oxidation time).MAO parameters were also optimized to achieve coatings with minimum porosity and maximum hardness.Further,the effect of MAO parameters on coating characteristics was analysed.From the results,it is found that the current density has greater influence on the responses than the other two parameters.
文摘Electro-copolymerized film containing ruthenium complexes as electron-transfer(or redox)mediators and water-oxidation catalysts by an oxidative copolymerization method is presented.The addition of the redox mediator significantly improved the electrocatalytic water-oxidation activity and reduced the overpotential to 220 mV.The prepared electrode showed a water-oxidation catalytic rate constant kobs of 31.7 s^(-1)and an initial turnover frequency of 1.01 s^(-1)in 1000 s by potential electrolysis at 1.7 V applied bias vs NHE(normal hydrogen electrode).The kinetic isotope effect study suggests that the catalytic water oxidation reaction on the electrode surface occurs via a bimolecular coupling mechanism.
基金supported by Natural Science Foundation of Shandong Province(ZR2022MB049)National Natural Science Foundation of China(22078174)。
文摘Biomass-derived platform molecules,such as furfural,are abundant and renewable feedstock for valuable chemical production.It is critical to synthesize highly efficient photocatalysts for selective oxidation under visible light.The Er@K-C_(3)N_(4)/UiO-66-NH_(2) catalyst was synthesized using a straight-forward hydrothermal technique,and exhibited exceptional efficiency in the photocatalytic oxidation of furfural to furoic acid.The catalyst was thoroughly characterized,confirming the effective adjustment of the band gap energy of Er@K-C_(3)N_(4)/UiO-66-NH_(2).Upon the optimized reaction conditions,the conversion rate of furfural reached 89.3%,with a corresponding yield of furoic acid at 79.8%.The primary reactive oxygen species was identified as·O_(2)^(-) from ESR spectra and scavenger tests.The incorporation of Er and K into the catalyst enhanced the photogenerated carriers transfer rate,hence increasing the separating efficiency of photogenerated electron-hole pairs.This study expands the potential applications of rare earth element doped g-C_(3)N_(4) in the photocatalytic selective oxidation of furfurans.
基金National Key R&D Program of China(2022YFB3707700)Shanghai Science and Technology Innovation Action Plan(21511104800)+3 种基金National Natural Science Foundation of China(52172111)National Science and Technology Major Project(2017-IV-0005-0042)Key Research Program of the Chinese Academy of Sciences(ZDRW-CN-2021-2-2)Science Center for Gas Turbine Project(P2022-B-IV-001-001)。
文摘ZrB_(2)-based ceramics typically necessitate high temperature and pressure for sintering,whereas ZrB_(2)-SiC ceramics can be fabricated at 1500℃using the process of reactive melt infiltration with Si.In comparison to the conventional preparation method,reactive synthesis allows for the more facile production of ultra-high temperature ceramics with fine particle size and homogeneous composition.In this work,ZrSi_(2),B4C,and C were used as raw materials to prepare ZrB_(2)-SiC via combination of tape casting and reactive melt infiltration herein referred to as ZBC ceramics.Control sample of ZrB_(2)-SiC was also prepared using ZrB_(2)and SiC as raw materials through an identical process designated as ZS ceramics.Microscopic analysis of both ceramic groups revealed smaller and more uniformly distributed particles of the ZrB_(2)phase in ZBC ceramics compared to the larger particles in ZS ceramics.Both sets of ceramics underwent cyclic oxidation testing in the air at 1600℃for a cumulative duration of 5 cycles,each cycle lasting 2 h.Analysis of the oxidation behavior showed that both ZBC ceramics and ZS ceramics developed a glassy SiO_(2)-ZrO_(2)oxide layer on their surfaces during the oxidation.This layer severed as a barrier against oxygen.In ZBC ceramics,ZrO_(2)is finely distributed in SiO_(2),whereas in ZS ceramics,larger ZrO_(2)particles coexist with glassy SiO_(2).The surface oxide layer of ZBC ceramics maintains a dense structure because the well-dispersed ZrO_(2)increases the viscosity of glassy SiO_(2),preventing its crystallization during the cooling.Conversely,some SiO_(2)in the oxide layer of ZS ceramics may crystallize and form a eutectic with ZrO_(2),leading to the formation of ZrSiO_(4).This leads to cracking of the oxide layer due to differences in thermal expansion coefficients,weakening its barrier effect.An analysis of the oxidation resistance shows that ZBC ceramics exhibit less increase in oxide layer thickness and mass compared to ZS ceramics,suggesting superior oxidation resistance of ZBC ceramics.
基金supported by Fundamental Research Funds for the Central Universities(2023KYJD1008)the Science Research Projects of the Anhui Higher Education Institutions of China(2022AH051582).
文摘Reversible solid oxide cell(RSOC)is a new energy conversion device with significant applications,especially for power grid peaking shaving.However,the reversible conversion process of power generation/energy storage poses challenges for the performance and stability of air electrodes.In this work,a novel high-entropy perovskite oxide La_(0.2)Pr_(0.2)Gd_(0.2)Sm_(0.2)Sr_(0.2)Co_(0.8)Fe_(0.2)O_(3−δ)(HE-LSCF)is proposed and investigated as an air electrode in RSOC.The electrochemical behavior of HE-LSCF was studied as an air electrode in both fuel cell and electrolysis modes.The polarization impedance(Rp)of the HE-LSCF electrode is only 0.25Ω·cm^(2) at 800℃ in an air atmosphere.Notably,at an electrolytic voltage of 2 V and a temperature of 800℃,the current density reaches up to 1.68 A/cm^(2).The HE-LSCF air electrode exhibited excellent reversibility and stability,and its electrochemical performance remains stable after 100 h of reversible operation.With these advantages,HE-LSCF is shown to be an excellent air electrode for RSOC.
基金Project(22102218)supported by the National Natural Science Foundation of ChinaProject(2022RC1110)supported by the Science and Technology Innovation Program of Hunan Province,ChinaProject(2022QNRC001)supported by the Young Elite Scientists Sponsorship Program by CAST,China。
文摘Formic acid oxidation reaction(FAOR),as the anodic reaction in direct formic acid fuel cells,has attracted much attention but increasing the mass activity and stability of catalysts still face a bottleneck to meet the requirements of practical applications.In the past decades,researchers developed many strategies to fix these issues by improving the structure of catalysts and the newly raised single atom catalysts(SACs)show the high mass activity and stability in FAOR.This review first summarized the reaction mechanism involved in FAOR.The mass activity as well as stability of catalysts reported in the past five years have been outlined.Moreover,the synthetic strategies to improve the catalytic performance of catalysts are also reviewed in this work.Finally,we proposed the research directions to guide the rational design of new FAOR catalysts in the future.
基金the“National Natural Science Foundation of China(No.22122202)”.
文摘Inducing the classic strong metal-support interaction(SMSI)is an effective approach to enhance the performance of supported metal catalysts by encapsulating the metal nanoparticles(NPs)with supports.Conventional thermal reduction method for inducing SMSI processes is often accompanied by undesirable structural evolution of metal NPs.In this study,a mild electrochemical method has been developed as a new approach to induce SMSI,using the cable structured core@shell CNT@SnO_(2) loaded Pt NPs as a proof of concept.The induced SnO_(x) encapsulation layer on the surface of Pt NPs can protect Pt NPs from the poisoned of CO impurity in hydrogen oxidation reaction(HOR),and the HOR current density could still maintain 85% for 2000 s with 10,000 ppm CO in H_(2),while the commercial Pt/C is completely inactivated.In addition,the electrons transfer from SnO_(x) to Pt NPs improved the HOR activity of the E-Pt-CNT@SnO_(2),achieving the excellent exchange current density of 1.55 A·mgPt^(-1).In situ Raman spectra and theoretical calculations show that the key to the electrochemical-method-induced SMSI is the formation of defects and the migration of SnO_(x) caused by the electrochemical redox operation,and the weakening the SneO bond strength by Pt NPs.
基金supported by the National Natural Science Foundation of China(51971157)Shenzhen Science and Technology Program(JCYJ20210324115412035,JCYJ202103-24123202008,JCYJ20210324122803009 and ZDS-YS20210813095534001)Guangdong Foundation for Basic and Applied Basic Research Program(2021A1515110880).
文摘In pursuit of more efficient and stable electrochemical energy storage materials,composite materials consisting of metal oxides and graphene oxide have garnered significant attention due to their unique structures and exceptional properties.Graphene oxide(GO),a two-dimensional material with an extremely high specific surface area and excellent conductivity,offers new possibilities for enhancing the electrochemical performance of metal oxides.In this work,we synthesized met-al-organic framework(MOF)and GO composites by regulating the amount of GO,and successfully prepared composites of metal oxides supported by nitrogen-doped carbon frameworks and GO through a simple one-step calcination process.Based on the electrochemical tests,the optimal amount of GO was determined.This research will provide new insights into and directions for designing and synthesizing metal oxide and graphene oxide composite materials with an ideal electro-chemical performance.
基金supported by Gansu Provincial Science and Technology Plan(23CXGA0195)Longnan Science and Technology Plan(2024CX03)。
文摘Graphene oxide nanomaterials are increasingly used in various fields due to their superior properties.In order to study the influence of graphene oxide additives on the performance of modified asphalt,in this study,graphene oxide modified asphalt was prepared and characteristics was studied including the high deformation resistance performance and the self-healing property of modified asphalt.Functional groups and morphology of graphene oxide modified asphalt were described by Fourier transform infrared spectroscopy.The high deformation resistance performance and self-healing effect of asphalt samples were obtained through dynamic slear rheometer(DSR)test.Results shows that graphene oxide dispersions improve the performance of asphalt relatively well compared to graphene oxide powder.There is no chemical reaction between graphene oxide and asphalt,but physical connection.The addition of graphene oxide improved the high deformation resistance of modified asphalt and expedited the self-healing ability of asphalt under fatigue load.
文摘With the aim to effectively depolymerize polyethylene terephthalate(PET)under mild reaction conditions,PET methanolysis and dimethyl terephthalate(DMT)hydrolysis are integrated in a catalyst system.Firstly,methanolysis of PET to DMT is achieved over Cu-Mg-Al oxide catalyst.Next,terephthalic acid(TPA)is prepared by DMT hydrolysis.It is found that hydrolysis of DMT to TPA can be promoted by introducing trace amount of water in this catalyst system.CuO-MgO-4.5Al_2O_(3)catalyst demonstrates the excellent catalytic performance for the depolymerization of PET with high conversion rate and TPA yield(100%and 99.5%,respectively)after reaction at 160℃for 6 h,which provides a new idea for the depolymerization of PET.
基金supported by the National Natural Science Foundation of China(61774140).
文摘ZnO thin films with varying Ta concentrations were fabricated through magnetron sputtering.The crystallinity and surface morphology of the ZnO films are significantly influenced by the incorporation of Ta,as evidenced by the X-ray diffraction and scanning electron microscopy results.The lattice constants,as determined by X-ray diffraction,contradict the disparity in Ta and Zn ion radii,which is attributed to the impact of interstitial defects.This inconsistency introduces variations in carrier concentration in this experiment compared with prior studies.Subsequent exploration of the luminescent characteristics and emission mechanism of defect levels in Ta-doped ZnO films was conducted through photoluminescence.Furthermore,the factors influencing the bandgap are discussed.
基金supported by National Key R&D Program of China(2021YFB4001401)National Natural Science Foundation of China(52272190,22178023).
文摘Solid oxide electrolysis cells(SOECs)can effectively convert CO_(2)into high value-added CO fuel.In this paper,Sc-doped Sr_(2)Fe_(1.5)Mo_(0.3)Sc_(0.2)O_(6−δ)(SFMSc)perovskite oxide material is synthesized via solid-phase method as the cathode for CO_(2)electrolysis by SOECs.XRD confirms that SFMSc exhibits a stable cubic phase crystal structure.The experimental results of TPD,TG,EPR,CO_(2)-TPD further demonstrate that Sc-doping increases the concentration of oxygen vacancy in the material and the chemical adsorption capacity of CO_(2)molecules.Electrochemical tests reveal that SFMSc single cell achieves a current density of 2.26 A/cm^(2) and a lower polarization impedance of 0.32Ω·cm^(2) at 800°C under the applied voltage of 1.8 V.And no significant performance attenuation or carbon deposition is observed after 80 h continuous long-term stability test.This study provides a favorable support for the development of SOEC cathode materials with good electro-catalytic performance and stability.
