The effect of CC-chemokine receptor 7 (CCR7) and CC-chemokine ligand 19 (CCL19) on rheumatic mitral ste- nosis is unknown. This study aimed to explore the roles of CCR7 and CCL19 in rheumatic mitral stenosis by me...The effect of CC-chemokine receptor 7 (CCR7) and CC-chemokine ligand 19 (CCL19) on rheumatic mitral ste- nosis is unknown. This study aimed to explore the roles of CCR7 and CCL19 in rheumatic mitral stenosis by mea- suring the expression of CCR7 and CCL19 in human mitral valves from rheumatic mitral stenosis patients. Additionally, we examined their effects on human mitral valve interstitial cells (hMVICs) proliferation, apoptosis and wound repair. CCR7 and CCL19 expression was measured in the mitral valves from rheumatic mitral stenosis patients (n= 10) and compared to normal mitral valves (n=5). CCR7 was measured in cultured hMVICs from rheu- matic mitral stenosis patients and normal donors by RT-PCR and immunofluorescence. The cells were also treated with exogenous CCL19, and the effects on wound healing, proliferation and apoptosis were assayed. In the rheu- matic mitral valves, valve interstitial cells expressed CCR7, while mononuclear cells and the endothelium expressed CCL19. Healthy mitral valves did not stain positive for CCR7 or CCL19. CCR7 was also detected in cultured rheu- matic hMVICs or in normal hMVICs treated with CCL19. In a wound healing experiment, wound closure rates of both rheumatic and normal hMVICs were significantly accelerated by CCL19. These effects were abrogated by a CCR7 neutralizing antibody. The CCR7/CCL19 axis did not influence the proliferation or apoptosis of hMVICs, indicating that wound healing was due to increased migration rates rather than increased proliferation. In conclu- sion, CCR7 and CCL19 were expressed in rheumatic mitral valves. The CCR7/CCL19 axis may regulate remodel- ing of rheumatic valve injury through promoting migratory ability of hMVICs.展开更多
Bi_(2)O_(2)CO_(3)(BOC)/Bi_(4)O_5Br_(2)(BOB)/reduced graphene oxide(rGO)Z-scheme heterojunction with promising photocatalytic properties was synthesized via a facile one-pot room-temperature method.Ultra-thin nanosheet...Bi_(2)O_(2)CO_(3)(BOC)/Bi_(4)O_5Br_(2)(BOB)/reduced graphene oxide(rGO)Z-scheme heterojunction with promising photocatalytic properties was synthesized via a facile one-pot room-temperature method.Ultra-thin nanosheets of BOC and BOB were grown in situ on r GO.The formed 2D/2D direct Z-scheme heterojunction of BOC/BOB with oxygen vacancies(OVs)effectively leads to lower negative electron reduction potential of BOB as well as higher positive hole oxidation potential of BOC,showing improved reduction/oxidation ability.Particularly,rGO is an acceptor of the electrons from the conduction band of BOC.Its dual roles significantly improve the transfer performance of photo-induced charge carriers and accelerate their separation.With layered nanosheet structure,rich OVs,high specific surface area,and increased utilization efficiency of visible light,the multiple synergistic effects of BOC/BOB/rGO can achieve effective generation and separation of the electron-holes,thereby generating more·O_(2)^(-)and h^(+).The photocatalytic reduction efficiency of CO_(2)to CO(12.91μmol/(g·hr))is three times higher than that of BOC(4.18μmol/(g·hr)).Moreover,it also achieved almost 100%removal of Rhodamine B and cyanobacterial cells within 2 hours.展开更多
The rapidly advancing energy storage performance of dielectric ceramics capacitors has garnered significant interest for applications in fast charge/discharge and high-power electronic techniques.Exploring the excepti...The rapidly advancing energy storage performance of dielectric ceramics capacitors has garnered significant interest for applications in fast charge/discharge and high-power electronic techniques.Exploring the exceptional electrical properties in harsh environments can further promote their practical applications.Defect carriers can be excited under luminance irradiation,thereby leading to degradation of energy storage performance.Herein,a synergic optimization strategy is proposed to enhance energy storage properties and luminance resistance of(K_(0.5)Na_(0.5))NbO_(3)-base(KNN)ceramics.First,the introduction of Bi(Zn0.5Ti0.5)O_(3) solid solution and La3+ions disrupts the long-range polar orders and enhances super paraelectric relaxation characteristics.Additionally,doping La3+ions can increase the band gap and reduce oxygen vacancy concentration,resulting in excellent luminance resistance.Finally,the viscous polymer process is employed to suppress the grain growth and promote chemical homogeneity.As a result,ultrahigh recoverable energy storage density(Wrec)of 8.11 J/cm3 and high efficiency(η)of 80.98%are achieved under an electric field of 568 kV/cm.Moreover,the variations in Wrec andηare only 12.45%and 1.75%,respectively,under 500 W xenon lamp irradiation compared to the performance under a dark environment.These findings hold great potential in facilitating the practical application of dielectric ceramic capacitors in luminance irradiation environments.展开更多
With the increasing demand of high-power and pulsed power electronic devices,environmental-friendly potassium sodium niobate((Na_(0.5)K_(0.5))NbO_(3),KNN)ceramic-based capacitors have attracted much attention in recen...With the increasing demand of high-power and pulsed power electronic devices,environmental-friendly potassium sodium niobate((Na_(0.5)K_(0.5))NbO_(3),KNN)ceramic-based capacitors have attracted much attention in recent years owning to the boosted energy storage density(W_(rec)).Nevertheless,the dielectric loss also increases as the external electric field increases,which will generate much dissipated energy and raise the temperature of ceramic capacitors.Thus,an effective strategy is proposed to enhance the energy storage efficiency(η)via tailoring relaxor behavior and bad gap energy in the ferroelectric 0.9(Na_(0.5)K_(0.5))-NbO_(3)-0.1Bi(Zn_(2/3)(Nb_(x)Ta_(1−x))1/3)O_(3) ceramics.On the one hand,the more diverse ions in the B-sites owing to introducing the Ta could further disturb the long-range ferroelectric polar order to form the short−range polar nanoregions(PNRs),resulting in the highη.On the other hand,the introduction of Ta ions could boost the intrinsic band energy gap and thus improve the Eb.As a result,high Wrec of 3.29 J/cm^(3) and ultrahighηof 90.1%at the high external electric field of 310 kV/cm are achieved in x=0.5 sample.These results reveal that the KNN-based ceramics are promising lead-free candidate for high-power electronic devices.展开更多
Herein,a one-step co-pyrolysis protocol was adopted for the first time to prepare a novel pyrogenic carbon-Cu^(0)/Fe_(3)O_(4)heteroatoms (FCBC) in CO_(2)ambiance to discern the roles of each component in PDS activatio...Herein,a one-step co-pyrolysis protocol was adopted for the first time to prepare a novel pyrogenic carbon-Cu^(0)/Fe_(3)O_(4)heteroatoms (FCBC) in CO_(2)ambiance to discern the roles of each component in PDS activation.During co-pyrolysis,CO_(2)catalyzed formation of reducing gases by biomass which facilitated reductive transformation of Fe^(3+)and Cu^(2+)to Cu^(0)and Fe_(3)O_(4),respectively.According to the analysis,the resulting metal (oxide) catalyzed graphitization of biocharand decomposition of volatile substances resulting in an unprecedented surface area (1240 m^(2)/g).The resulting FCBC showed greater structural defects and less electrical impedance.Batch experiments indicated that Rhodamine B (RhB) degradation by FCBC (100%) was superior to Fe_(3)O_(4)(50%) and Cu^(0)/Fe_(3)O_(4)(76.4%) in persulfate (PDS) system,which maintained reasonable efficiency (75.6%-63.6%) within three cycles.The reactive oxygen species (ROS) associated with RhB degradation was identified by an electron paramagnetic resonance and confirmed by scavenging experiments.RhB degradation invoked both(sulfate and dominantly hydroxyl) radical and non-radical (singlet oxygen,^(1)O_(2)) pathways.Regarding FCBC,Cu^(0)can continuously react with Fe^(3+)in Fe_(3)O_(4)to generate larger quantities of Fe^(2+),and both Cu^(0)and Fe^(2+)activated PDS to yield sulfate radicals which was quickly converted to hydroxyl radical.Besides,Cu^(0)/Cu^(2+)could complex with PDS to form a metastable complex,which particularly contributed to1O_(2)generation.These cascade reactions by FCBC were reinforced by carbonyl group of biochar and favorable electron transfer ability.This work highlighted a new approach to prepare a magnetic and environment-benign heterogonous catalyst to remove organic pollutants in water.展开更多
Herein,we report the synthesis of interconnected hierarchical pore biochar(HTB)via an ice-templating strategy using bio-waste(tofukasu).The abundance of N-and O-containing functional groups in tofukasu makes it easy t...Herein,we report the synthesis of interconnected hierarchical pore biochar(HTB)via an ice-templating strategy using bio-waste(tofukasu).The abundance of N-and O-containing functional groups in tofukasu makes it easy to form hydrogen bonds with water molecules and water clusters,resulting in nano-micro structures like ice clusters and snow crystals during freezing process.More importantly,tofukasu will be squeezed by micron-scale snow crystals to form coiled sheet-like structures,and its surface and interior will be affected by needle-like ice nanocrystals from several nanometers to tens of nanometers to form transverse groove needles and mesopores.The ice crystals are then removed by sublimation with tofukasu,leaving the interconnected pore structure intact.Therefore,the ice template synthesis strategy endowed the interconnected hierarchical pore structure of HTB with a large specific surface area(SBET,733 m^(2)⋅g^(−1))and hierarchical porosity(30.30%for mesopores/total pore volume ratio),which is significantly higher than the normal dry treated tofukasu biochar(TB),which had a SBET of 436 m^(2)⋅g^(−1) and contained 1.53%mesopores.In addition,the sheet-like structure with interconnected pores of HTB favors high exposure of active sites(N-and O-containing functional groups),and a fast electron transport rate.As a result,HTB had an excellent adsorption capacity of 159.65 mg⋅g^(−1),which is 4.7 times that of typical block biochar of TB(33.89 mg⋅g^(−1))according to Langmuir model.Electrochemical characterization,FTIR and XPS analysis showed that the mechanism of Cr(Ⅵ)removal by HTB included electrostatic attraction,pore filling,reduction and surface complexation.展开更多
In this work,taking NiSe_(2)as a prototype to be used as cocatalyst in photocatalytic hydrogen evolution,we demonstrate that the crystal phase of NiSe_(2)plays a vital role in determining the catalytic stability,rathe...In this work,taking NiSe_(2)as a prototype to be used as cocatalyst in photocatalytic hydrogen evolution,we demonstrate that the crystal phase of NiSe_(2)plays a vital role in determining the catalytic stability,rather than activity.Theoretical and experimental results indicate that the phase structure shows negligible influence to the charge transport and hydrogen adsorption capacity.When integrating with carbon nitride(CN)photocatalyst forming hybrids(m-NiSe_(2)/CN and p-NiSe_(2)/CN),the hybrids show comparable photocatalytic hydrogen evolution rates(3.26μmol/h and 3.75μmol/h).Unlike the comparable catalytic activity,we found that phase-engineered NiSe_(2)exhibits distinct stability,i.e.,m-NiSe_(2)can evolve H_(2) steadily,but p-NiSe_(2)shows a significant decrease in catalytic process(∼57.1%decrease in 25 h).The factor leading to different catalytic stability can be ascribed to the different surface conversion behavior during photocatalytic process,i.e.,chemical structure of m-NiSe_(2)can be well preserved in catalytic process,but partial p-NiSe_(2)tends to be converted to NiOOH.展开更多
Reactive oxygen species(ROS)have a significant part in the elimination of recalcitrant organic pollutants and commonly coexist in one advanced oxidation system.It is difficult for us to make clear the effect of the co...Reactive oxygen species(ROS)have a significant part in the elimination of recalcitrant organic pollutants and commonly coexist in one advanced oxidation system.It is difficult for us to make clear the effect of the co-instantaneous generation of radicals and nonradicals,which would cover and obscure the transformation pathway.Herein,a coordinate welding process is presented for fabricating accessible Mn1 site catalysts(Mn SSCs)in order to clarify the nonradical(singlet oxygen/^(1)O_(2))generated pathway and transformation in oxidative removal of contaminants.The Mn SSCs achieve nearly 100%^(1)O_(2) fabrication by activating peroxymonosulfate,which displays an excellent sulfamethoxazole elimination performance,super anti-anion interference,and extraordinary stability.As revealed by density functional theory calculations,the Mn SSCs with a special welded three-dimensional nanostructure could significantly boost the activation process by oxidizing the peroxymonosulfate at the interlayer of Mn SSCs and reducing dissolved oxygen on the surface of Mn SSCs.This design of Mn SSCs with a three-dimensional welded nanostructure might offer a potential approach for employing single site catalysts for environmental remediation.展开更多
Relaxor dielectric ceramic capacitors are very attractive for high-power energy storage.However,the low breakdown strength severely restricts improvements to the energy storage density and practical application.Here,a...Relaxor dielectric ceramic capacitors are very attractive for high-power energy storage.However,the low breakdown strength severely restricts improvements to the energy storage density and practical application.Here,a strategy of designing small grain sizes and abundant amorphous grain boundaries is proposed to improve the energy storage properties under the guidance of phase field theory.0.925(K_(0.5)Na_(0.5))NbO_(3)-e0.075Bi(Zn_(2/3)(Ta_(0.5)Nb_(0.5))1/3)O_(3)(KNNe-BZTN)relaxor ferroelectric ceramic is taken as an example to verify our strategy.The grain sizes and grain boundaries of the KNNeBZTN ceramics are carefully controlled by the high-energy ball milling method and twoestep sintering strategy.Impedance analysis and diffusion reflectance spectra demonstrate that KNNeBZTN ceramics with a small grain size and abundant amorphous grain boundary exhibit a lower charge carrier concentration and higher band gap.As a consequence,the breakdown electric field of KNNeBZTN ceramics increases from 222 kV/cm to 317 kV/cm when the grain size is decreased from 410 nm to 200 nm,accompanied by a slightly degraded maximum polarization.KNNeBZTN ceramics with an average grain size of~250 nm and abundant amorphous grain boundaries exhibit optimum energy storage properties with a high recoverable energy density of 4.02 J/cm^(3) and a high energy efficiency of 87.4%.This successful local structural design opens up a new paradigm to improve the energy storage performance of other dielectric ceramic capacitors for electrical energy storage.展开更多
In this work,a high-efficiency photocatalytic BiOCl material with a visible light absorption range was successfully prepared by one-pot molecular self-assembly and particle recrystallization method at room temperature...In this work,a high-efficiency photocatalytic BiOCl material with a visible light absorption range was successfully prepared by one-pot molecular self-assembly and particle recrystallization method at room temperature.In the process of crystal growth,tartaric acid,as a structure control agent,gradually transforms the stacked two-dimensional nano-sheet-like BiOCl into a hierarchical structure composed of petallike nano-sheets through hydrogen bonding.Besides,the acid etching of organic carboxylic acid on the crystal surface increases the number of micropores and mesopores,thereby the reaction interface.The thiourea(TU)molecules adsorbed on the BiOCl surface with a strong electronic effect introduce oxygen vacancies(OVs)under the condition of low oxygen content.The synergistic effect of hierarchical structure and OVs reduces the recombination of photogenerated carriers,but absorbs more O_(2)and OH−to generate a large number of superoxide radicals(·O_(2)−)and hydroxyl radicals(·OH)effectively.The photocatalytic performance of the synthesized BiOCl material has been significantly improved,and it can effectively degrade 94.15%of rhodamine B(RhB)within 20 min.Furthermore,90.95%of tetracycline(TC),93.76%of ciprofloxacin(CIP),and 85.53%of methyl orange(MO)can be removed in 80 min.Therefore,our work provides an effective method for preparing BiOCl with visible light catalytic activity,which,of course,can be used to treat and repair actual environmental problems under mild conditions.展开更多
Although dielectric ceramic capacitors possess attractive properties for high-power energy storage,their pronounced electrostriction effect and high brittleness are conducive to easy initiation and propagation of crac...Although dielectric ceramic capacitors possess attractive properties for high-power energy storage,their pronounced electrostriction effect and high brittleness are conducive to easy initiation and propagation of cracks that significantly deteriorate electrical reliability and lifetime of capacitors in practical applications.Herein,a new strategy for designing relaxor ferroelectric ceramics with K_(0.5)Na_(0.5)NbO_(3)-core/SiO_(2)-shell structured grains was proposed to simultaneously reduce the electric-field-induced strain and enhance the mechanical strength of the ceramics.The simulation and experiment declared that the bending strength and compression strength of the core-shell structured ceramic were shown to increase by more than 50% over those of the uncoated sample.Meanwhile,the electric-field-induced strain was reduced by almost half after adding the SiO_(2) coating.The suppressed electrical deformation and enhanced mechanical strength could alleviate the probability of generation of cracks and prevent their propagation,thus remarkably improving breakdown strength and fatigue endurance of the ceramics.As a result,an ultra-high breakdown strength of 425 kV cm^(-1) and excellent recoverable energy storage density(Wrec~4.64 J cm^(-3))were achieved in the core-shell structured sample.More importantly,the unique structure could enhance the cycling stability of the ceramic(Wrec variation<±2% after 105 cycles).Thus,mechanical performance optimization via grain structure engineering offers a new paradigm for improving electrical breakdown strength and fatigue endurance of dielectric ceramic capacitors.展开更多
基金supported by grants from the National Natural Science Foundation of China(No.81100162)the Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD2010-2013)
文摘The effect of CC-chemokine receptor 7 (CCR7) and CC-chemokine ligand 19 (CCL19) on rheumatic mitral ste- nosis is unknown. This study aimed to explore the roles of CCR7 and CCL19 in rheumatic mitral stenosis by mea- suring the expression of CCR7 and CCL19 in human mitral valves from rheumatic mitral stenosis patients. Additionally, we examined their effects on human mitral valve interstitial cells (hMVICs) proliferation, apoptosis and wound repair. CCR7 and CCL19 expression was measured in the mitral valves from rheumatic mitral stenosis patients (n= 10) and compared to normal mitral valves (n=5). CCR7 was measured in cultured hMVICs from rheu- matic mitral stenosis patients and normal donors by RT-PCR and immunofluorescence. The cells were also treated with exogenous CCL19, and the effects on wound healing, proliferation and apoptosis were assayed. In the rheu- matic mitral valves, valve interstitial cells expressed CCR7, while mononuclear cells and the endothelium expressed CCL19. Healthy mitral valves did not stain positive for CCR7 or CCL19. CCR7 was also detected in cultured rheu- matic hMVICs or in normal hMVICs treated with CCL19. In a wound healing experiment, wound closure rates of both rheumatic and normal hMVICs were significantly accelerated by CCL19. These effects were abrogated by a CCR7 neutralizing antibody. The CCR7/CCL19 axis did not influence the proliferation or apoptosis of hMVICs, indicating that wound healing was due to increased migration rates rather than increased proliferation. In conclu- sion, CCR7 and CCL19 were expressed in rheumatic mitral valves. The CCR7/CCL19 axis may regulate remodel- ing of rheumatic valve injury through promoting migratory ability of hMVICs.
基金supported by the National Natural Science Foundation of China(Nos.51602281 and 52100014)the Natural Science Foundation of Jiangsu Province(No.BK20180938)the Yangzhou University High-end Talent Support Program and the“Qinglan Project”of Jiangsu Universities。
文摘Bi_(2)O_(2)CO_(3)(BOC)/Bi_(4)O_5Br_(2)(BOB)/reduced graphene oxide(rGO)Z-scheme heterojunction with promising photocatalytic properties was synthesized via a facile one-pot room-temperature method.Ultra-thin nanosheets of BOC and BOB were grown in situ on r GO.The formed 2D/2D direct Z-scheme heterojunction of BOC/BOB with oxygen vacancies(OVs)effectively leads to lower negative electron reduction potential of BOB as well as higher positive hole oxidation potential of BOC,showing improved reduction/oxidation ability.Particularly,rGO is an acceptor of the electrons from the conduction band of BOC.Its dual roles significantly improve the transfer performance of photo-induced charge carriers and accelerate their separation.With layered nanosheet structure,rich OVs,high specific surface area,and increased utilization efficiency of visible light,the multiple synergistic effects of BOC/BOB/rGO can achieve effective generation and separation of the electron-holes,thereby generating more·O_(2)^(-)and h^(+).The photocatalytic reduction efficiency of CO_(2)to CO(12.91μmol/(g·hr))is three times higher than that of BOC(4.18μmol/(g·hr)).Moreover,it also achieved almost 100%removal of Rhodamine B and cyanobacterial cells within 2 hours.
基金supported by the National Natural Science Foundation of China(41977085)the Qing Lan Project,the 333 Project of Jiangsu Province(BRA202030)+4 种基金the Six Talent Peaks Project in Jiangsu Province(2018-TD-JNHB-012)the Lvyang Jinfeng Fund of Yangzhou(137012724)the Research Foundation of Yangzhou University(137012446)Doctor of Mass Entrepreneurship and Innovation of Jiangsu Province(337090323)the Innovation Fostering Fund of Yangzhou University.
基金supported by the National Natural Science Foundation of China(Grant Nos.52072150 and 51972146)Shandong Province Key Fundamental Research Program(Grant No.ZR2022ZD39).
文摘The rapidly advancing energy storage performance of dielectric ceramics capacitors has garnered significant interest for applications in fast charge/discharge and high-power electronic techniques.Exploring the exceptional electrical properties in harsh environments can further promote their practical applications.Defect carriers can be excited under luminance irradiation,thereby leading to degradation of energy storage performance.Herein,a synergic optimization strategy is proposed to enhance energy storage properties and luminance resistance of(K_(0.5)Na_(0.5))NbO_(3)-base(KNN)ceramics.First,the introduction of Bi(Zn0.5Ti0.5)O_(3) solid solution and La3+ions disrupts the long-range polar orders and enhances super paraelectric relaxation characteristics.Additionally,doping La3+ions can increase the band gap and reduce oxygen vacancy concentration,resulting in excellent luminance resistance.Finally,the viscous polymer process is employed to suppress the grain growth and promote chemical homogeneity.As a result,ultrahigh recoverable energy storage density(Wrec)of 8.11 J/cm3 and high efficiency(η)of 80.98%are achieved under an electric field of 568 kV/cm.Moreover,the variations in Wrec andηare only 12.45%and 1.75%,respectively,under 500 W xenon lamp irradiation compared to the performance under a dark environment.These findings hold great potential in facilitating the practical application of dielectric ceramic capacitors in luminance irradiation environments.
基金supported by the National Natural Science Foundation of China(Grant No.52072150)the Young Elite Scientists Sponsorship Program of the Chinese Academy of Space Technology(CAST)and Open Foundation of Guangdong Provincial Key Laboratory of Electronic Functional Materials and Devices(EFMD2021002Z).
文摘With the increasing demand of high-power and pulsed power electronic devices,environmental-friendly potassium sodium niobate((Na_(0.5)K_(0.5))NbO_(3),KNN)ceramic-based capacitors have attracted much attention in recent years owning to the boosted energy storage density(W_(rec)).Nevertheless,the dielectric loss also increases as the external electric field increases,which will generate much dissipated energy and raise the temperature of ceramic capacitors.Thus,an effective strategy is proposed to enhance the energy storage efficiency(η)via tailoring relaxor behavior and bad gap energy in the ferroelectric 0.9(Na_(0.5)K_(0.5))-NbO_(3)-0.1Bi(Zn_(2/3)(Nb_(x)Ta_(1−x))1/3)O_(3) ceramics.On the one hand,the more diverse ions in the B-sites owing to introducing the Ta could further disturb the long-range ferroelectric polar order to form the short−range polar nanoregions(PNRs),resulting in the highη.On the other hand,the introduction of Ta ions could boost the intrinsic band energy gap and thus improve the Eb.As a result,high Wrec of 3.29 J/cm^(3) and ultrahighηof 90.1%at the high external electric field of 310 kV/cm are achieved in x=0.5 sample.These results reveal that the KNN-based ceramics are promising lead-free candidate for high-power electronic devices.
基金supported by the National Natural Science Foundation of China (Nos. 41771349, 41977117, 41977085)Qing-Lan Project of Yangzhou University (2020)+2 种基金High-level Talent Support Plan of Yangzhou University (2019)the Key Research and Development Program of Zhejiang Province (No. 2019C02053)Foreign Expert Recruitment Program of Jiangsu Province (No. BX2020050)。
文摘Herein,a one-step co-pyrolysis protocol was adopted for the first time to prepare a novel pyrogenic carbon-Cu^(0)/Fe_(3)O_(4)heteroatoms (FCBC) in CO_(2)ambiance to discern the roles of each component in PDS activation.During co-pyrolysis,CO_(2)catalyzed formation of reducing gases by biomass which facilitated reductive transformation of Fe^(3+)and Cu^(2+)to Cu^(0)and Fe_(3)O_(4),respectively.According to the analysis,the resulting metal (oxide) catalyzed graphitization of biocharand decomposition of volatile substances resulting in an unprecedented surface area (1240 m^(2)/g).The resulting FCBC showed greater structural defects and less electrical impedance.Batch experiments indicated that Rhodamine B (RhB) degradation by FCBC (100%) was superior to Fe_(3)O_(4)(50%) and Cu^(0)/Fe_(3)O_(4)(76.4%) in persulfate (PDS) system,which maintained reasonable efficiency (75.6%-63.6%) within three cycles.The reactive oxygen species (ROS) associated with RhB degradation was identified by an electron paramagnetic resonance and confirmed by scavenging experiments.RhB degradation invoked both(sulfate and dominantly hydroxyl) radical and non-radical (singlet oxygen,^(1)O_(2)) pathways.Regarding FCBC,Cu^(0)can continuously react with Fe^(3+)in Fe_(3)O_(4)to generate larger quantities of Fe^(2+),and both Cu^(0)and Fe^(2+)activated PDS to yield sulfate radicals which was quickly converted to hydroxyl radical.Besides,Cu^(0)/Cu^(2+)could complex with PDS to form a metastable complex,which particularly contributed to1O_(2)generation.These cascade reactions by FCBC were reinforced by carbonyl group of biochar and favorable electron transfer ability.This work highlighted a new approach to prepare a magnetic and environment-benign heterogonous catalyst to remove organic pollutants in water.
基金National Natural Science Foundation of China(51602281)Innovative Science and Technology Platform Project of Cooperation between Yangzhou City and Yangzhou University,China(No.YZ202026308)+1 种基金Yangzhou University self-made experimental equipment special fund(YZUZZ2022-13)Yangzhou University High-end Talent Support Program,the“Qinglan Project”of Jiangsu University and Postgraduate Research&Practice Innovation Program of Jiangsu Province(SJCX22_1735)。
文摘Herein,we report the synthesis of interconnected hierarchical pore biochar(HTB)via an ice-templating strategy using bio-waste(tofukasu).The abundance of N-and O-containing functional groups in tofukasu makes it easy to form hydrogen bonds with water molecules and water clusters,resulting in nano-micro structures like ice clusters and snow crystals during freezing process.More importantly,tofukasu will be squeezed by micron-scale snow crystals to form coiled sheet-like structures,and its surface and interior will be affected by needle-like ice nanocrystals from several nanometers to tens of nanometers to form transverse groove needles and mesopores.The ice crystals are then removed by sublimation with tofukasu,leaving the interconnected pore structure intact.Therefore,the ice template synthesis strategy endowed the interconnected hierarchical pore structure of HTB with a large specific surface area(SBET,733 m^(2)⋅g^(−1))and hierarchical porosity(30.30%for mesopores/total pore volume ratio),which is significantly higher than the normal dry treated tofukasu biochar(TB),which had a SBET of 436 m^(2)⋅g^(−1) and contained 1.53%mesopores.In addition,the sheet-like structure with interconnected pores of HTB favors high exposure of active sites(N-and O-containing functional groups),and a fast electron transport rate.As a result,HTB had an excellent adsorption capacity of 159.65 mg⋅g^(−1),which is 4.7 times that of typical block biochar of TB(33.89 mg⋅g^(−1))according to Langmuir model.Electrochemical characterization,FTIR and XPS analysis showed that the mechanism of Cr(Ⅵ)removal by HTB included electrostatic attraction,pore filling,reduction and surface complexation.
基金the financial support by Natural Science Foundation of Jiangsu Province(No.BK20210827)China Postdoctoral Science Foundation(No.2021M700117)+3 种基金National Natural Science Foundation of China(Nos.U1904215 and 41977085)Program for Young Changjiang Scholars of the Ministry of Education(No.Q2018270)Six Talent Peaks Project in Jiangsu Province(No.TD-JNHB-012)333 Project in Jiangsu Province(No.BRA2020300).
文摘In this work,taking NiSe_(2)as a prototype to be used as cocatalyst in photocatalytic hydrogen evolution,we demonstrate that the crystal phase of NiSe_(2)plays a vital role in determining the catalytic stability,rather than activity.Theoretical and experimental results indicate that the phase structure shows negligible influence to the charge transport and hydrogen adsorption capacity.When integrating with carbon nitride(CN)photocatalyst forming hybrids(m-NiSe_(2)/CN and p-NiSe_(2)/CN),the hybrids show comparable photocatalytic hydrogen evolution rates(3.26μmol/h and 3.75μmol/h).Unlike the comparable catalytic activity,we found that phase-engineered NiSe_(2)exhibits distinct stability,i.e.,m-NiSe_(2)can evolve H_(2) steadily,but p-NiSe_(2)shows a significant decrease in catalytic process(∼57.1%decrease in 25 h).The factor leading to different catalytic stability can be ascribed to the different surface conversion behavior during photocatalytic process,i.e.,chemical structure of m-NiSe_(2)can be well preserved in catalytic process,but partial p-NiSe_(2)tends to be converted to NiOOH.
基金supported by China Ministry of Science and Technology(2021YFA1500404)the Anhui Provincial Natural Science Foundation(2108085QB70,2108085UD06)+2 种基金the Collaborative Innovation Program of Hefei Science Center,CAS(2021HSC-CIP002)the Natural Science Foundation of Hefei,China(Grant No.2021044)the Fundamental Research Funds for the Central Universities(WK2060000004,WK2060000021,WK2060000025,KY2060000180,and KY2060000195).
文摘Reactive oxygen species(ROS)have a significant part in the elimination of recalcitrant organic pollutants and commonly coexist in one advanced oxidation system.It is difficult for us to make clear the effect of the co-instantaneous generation of radicals and nonradicals,which would cover and obscure the transformation pathway.Herein,a coordinate welding process is presented for fabricating accessible Mn1 site catalysts(Mn SSCs)in order to clarify the nonradical(singlet oxygen/^(1)O_(2))generated pathway and transformation in oxidative removal of contaminants.The Mn SSCs achieve nearly 100%^(1)O_(2) fabrication by activating peroxymonosulfate,which displays an excellent sulfamethoxazole elimination performance,super anti-anion interference,and extraordinary stability.As revealed by density functional theory calculations,the Mn SSCs with a special welded three-dimensional nanostructure could significantly boost the activation process by oxidizing the peroxymonosulfate at the interlayer of Mn SSCs and reducing dissolved oxygen on the surface of Mn SSCs.This design of Mn SSCs with a three-dimensional welded nanostructure might offer a potential approach for employing single site catalysts for environmental remediation.
基金supported by the National Natural Science Foundation of China(Grant Nos.52072150,51702119,51702122,51972146)Young Elite Scientists Sponsorship Program by CAST.
文摘Relaxor dielectric ceramic capacitors are very attractive for high-power energy storage.However,the low breakdown strength severely restricts improvements to the energy storage density and practical application.Here,a strategy of designing small grain sizes and abundant amorphous grain boundaries is proposed to improve the energy storage properties under the guidance of phase field theory.0.925(K_(0.5)Na_(0.5))NbO_(3)-e0.075Bi(Zn_(2/3)(Ta_(0.5)Nb_(0.5))1/3)O_(3)(KNNe-BZTN)relaxor ferroelectric ceramic is taken as an example to verify our strategy.The grain sizes and grain boundaries of the KNNeBZTN ceramics are carefully controlled by the high-energy ball milling method and twoestep sintering strategy.Impedance analysis and diffusion reflectance spectra demonstrate that KNNeBZTN ceramics with a small grain size and abundant amorphous grain boundary exhibit a lower charge carrier concentration and higher band gap.As a consequence,the breakdown electric field of KNNeBZTN ceramics increases from 222 kV/cm to 317 kV/cm when the grain size is decreased from 410 nm to 200 nm,accompanied by a slightly degraded maximum polarization.KNNeBZTN ceramics with an average grain size of~250 nm and abundant amorphous grain boundaries exhibit optimum energy storage properties with a high recoverable energy density of 4.02 J/cm^(3) and a high energy efficiency of 87.4%.This successful local structural design opens up a new paradigm to improve the energy storage performance of other dielectric ceramic capacitors for electrical energy storage.
基金financially supported by the National Natural Science Foundation of China (No. 51602281)the China Postdoctoral Science Foundation (No. 2017M621832)+3 种基金the Science and Technology Innovation Cultivation Fund project of Yangzhou University (No. 2019CXJ092)the project of national local joint engineering laboratory to functional adsorption material technology for the environmental protection, Soochow University (No. SDGC2124)Yangzhou University High-end Talent Support Programthe “Qinglan Project” of Jiangsu Universities
文摘In this work,a high-efficiency photocatalytic BiOCl material with a visible light absorption range was successfully prepared by one-pot molecular self-assembly and particle recrystallization method at room temperature.In the process of crystal growth,tartaric acid,as a structure control agent,gradually transforms the stacked two-dimensional nano-sheet-like BiOCl into a hierarchical structure composed of petallike nano-sheets through hydrogen bonding.Besides,the acid etching of organic carboxylic acid on the crystal surface increases the number of micropores and mesopores,thereby the reaction interface.The thiourea(TU)molecules adsorbed on the BiOCl surface with a strong electronic effect introduce oxygen vacancies(OVs)under the condition of low oxygen content.The synergistic effect of hierarchical structure and OVs reduces the recombination of photogenerated carriers,but absorbs more O_(2)and OH−to generate a large number of superoxide radicals(·O_(2)−)and hydroxyl radicals(·OH)effectively.The photocatalytic performance of the synthesized BiOCl material has been significantly improved,and it can effectively degrade 94.15%of rhodamine B(RhB)within 20 min.Furthermore,90.95%of tetracycline(TC),93.76%of ciprofloxacin(CIP),and 85.53%of methyl orange(MO)can be removed in 80 min.Therefore,our work provides an effective method for preparing BiOCl with visible light catalytic activity,which,of course,can be used to treat and repair actual environmental problems under mild conditions.
基金This work was supported by the National Natural Science Foundation of China(grants nos.52072150,51972146,and 51772175)the China Association for Science and Technology(Young Elite Scientists Sponsorship Program)the State Key Laboratory of New Ceramic and Fine Processing Tsinghua University(project no.KF202002).
文摘Although dielectric ceramic capacitors possess attractive properties for high-power energy storage,their pronounced electrostriction effect and high brittleness are conducive to easy initiation and propagation of cracks that significantly deteriorate electrical reliability and lifetime of capacitors in practical applications.Herein,a new strategy for designing relaxor ferroelectric ceramics with K_(0.5)Na_(0.5)NbO_(3)-core/SiO_(2)-shell structured grains was proposed to simultaneously reduce the electric-field-induced strain and enhance the mechanical strength of the ceramics.The simulation and experiment declared that the bending strength and compression strength of the core-shell structured ceramic were shown to increase by more than 50% over those of the uncoated sample.Meanwhile,the electric-field-induced strain was reduced by almost half after adding the SiO_(2) coating.The suppressed electrical deformation and enhanced mechanical strength could alleviate the probability of generation of cracks and prevent their propagation,thus remarkably improving breakdown strength and fatigue endurance of the ceramics.As a result,an ultra-high breakdown strength of 425 kV cm^(-1) and excellent recoverable energy storage density(Wrec~4.64 J cm^(-3))were achieved in the core-shell structured sample.More importantly,the unique structure could enhance the cycling stability of the ceramic(Wrec variation<±2% after 105 cycles).Thus,mechanical performance optimization via grain structure engineering offers a new paradigm for improving electrical breakdown strength and fatigue endurance of dielectric ceramic capacitors.