Direct conversion of solar energy into chemical energy in an environmentally friendly manner is one of the most promising strategies to deal with the environmental pollution and energy crisis.Among a variety of materi...Direct conversion of solar energy into chemical energy in an environmentally friendly manner is one of the most promising strategies to deal with the environmental pollution and energy crisis.Among a variety of materials developed as photocatalysts,the core-shell metal/covalent-organic framework(MOF or COF)photocatalysts have garnered significant attention due to their highly porous structure and the adjustability in both structure and functionality.The existing reviews on core-shell organic framework photocatalytic materials have mainly focused on core-shell MOF materials.However,there is still a lack of indepth reviews specifically addressing the photocatalytic performance of core-shell COFs and MOFs@COFs.Simultaneously,there is an urgent need for a comprehensive review encompassing these three types of core-shell structures.Based on this,this review aims to provide a comprehensive understanding and useful guidelines for the exploration of suitable core-shell organic framework photocatalysts towards appropriate photocatalytic energy conversion and environmental governance.Firstly,the classification,synthesis,formation mechanisms,and reasonable regulation of core-shell organic framework were summarized.Then,the photocatalytic applications of these three kinds of core-shell structures in different areas,such as H_(2)evolution,CO_(2)reduction,and pollutants degradation are emphasized.Finally,the main challenges and development prospects of core-shell organic framework photocatalysts were introduced.This review aims to provide insights into the development of a novel generation of efficient and stable core-shell organic framework materials for energy conversion and environmental remediation.展开更多
The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves...The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves the pretreatment of HMX to endow—OH groups on the surface via polyalcohol bonding agent modification and in situ coating with nitrate ester-containing polymer,was proposed to address the problem.Two types of energetic polyether—glycidyl azide polymer(GAP)and nitrate modified GAP(GNP)were grafted onto HMX crystal based on isocyanate addition reaction bridged through neutral polymeric bonding agent(NPBA)layer.The morphology and structure of the HMX-based composites were characterized in detail and the core-shell structure was validated.The grafted polymers obviously enhanced the adhesion force between HMX crystals and fluoropolymer(F2314)binder.Due to the interfacial reinforcement among the components,the two HMX-based composites exhibited a remarkable increment of phase transition peak temperature by 10.2°C and 19.6°C with no more than 1.5%shell content,respectively.Furthermore,the impact and friction sensitivity of the composites decreased significantly as a result of the barrier produced by the grafted polymers.These findings will enhance the future prospects for the interface design of energetic composites aiming to solve the weak interface and safety concerns.展开更多
Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas denitrification.However,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption...Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas denitrification.However,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption and waste gas emissions.To address this,electrocatalytic nitric oxide reduction reaction(NORR)has emerged as a promising strategy to bridge NH3consumption to NH3production,harnessing renewable electricity for a sustainable future.Copper(Cu)stands out as a prominent electrocatalyst for NO reduction,given its exceptional NH3yield and selectivity.However,a crucial aspect that remains insufficiently explored is the effects of morphology and valence states of Cu on the NORR performance.In this investigation,we synthesized CuO nanowires(CuO-NF)and Cu nanocubes(Cu-NF)as cathodes through an in situ growth method.Remarkably,CuO-NF exhibited an impressive NH3yield of 0.50±0.02 mg cm^(-2)h^(-1)at-0.6 V vs.reversible hydrogen electrode(RHE)with faradaic efficiency of29,68%±1,35%,surpassing that of Cu-NF(0.17±0.01 mg cm^(-2)h^(-1),16.18%±1.40%).Throughout the electroreduction process,secondary cubes were generated on the CuO-NF surface,preserving their nanosheet cluster morphology,sustained by an abundant supply of subsurface oxygen(s-O)even after an extended duration of 10 h,until s-O depletion ensued.Conversely,Cu-NF exhibited inadequate s-O content,leading to rapid crystal collapse within the same timeframe.The distinctive current-potential relationship,akin to a volcano-type curve,was attributed to distinct NO hydrogenation mechanisms.Further Tafel analysis revealed the exchange current density(i0)and standard heterogeneous rate constant(k0)for CuO-NF,yielding 3.44×10^(-6)A cm^(-2)and 3.77×10^(-6)cm^(-2)s^(-1)when NORR was driven by overpotentials.These findings revealed the potential of CuO-NF for NO reduction and provided insights into the intricate interplay between crystal morphology,valence states,and electrochemical performance.展开更多
As the global electric vehicle market continues to grow,the recycling of Li-ion battery (LIB) becomes more important worldwide and the resynthesis of cathode materials would be the most value-added recycling approach ...As the global electric vehicle market continues to grow,the recycling of Li-ion battery (LIB) becomes more important worldwide and the resynthesis of cathode materials would be the most value-added recycling approach taking into account limited metal resources.Although resynthesized homogenous LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM) from spent LIB leachate shows comparable battery performance to pristine NCM from virgin materials,there is general concern in its cycling performance.Here,we synthesize core–shell(CS) Ni-rich NCM,which consists of Ni-rich NCM as the core and NCM derived from the original or purified leachate of spent LIBs as the shell.Resynthesized CS Ni-rich NCM exhibits improved rate capability resulting from expanded interslab thickness in the NCM structure.CS Ni-rich NCM from purified LIB leachate shows improvement in cycling performance and thermal stability.It specifically delivers a capacity retention of 86.6%at a high temperature after 80 cycles compared to that (75.0%) of pristine CS Ni-rich NCM.These improvements are caused by a relatively high Mg content on the shell and the widespread distribution of Al through the CS structure.CS Ni-rich NCM derived from spent LIB leachate provides a new alternative approach to conventional LIB recycling methods,which would utilize efficiently limited metal resources for the sustainable LIB production.展开更多
Semiconductor photocatalysis holds great promise for renewable energy generation and environment remediation,but generally suffers from the serious drawbacks on light absorption,charge generation and transport,and str...Semiconductor photocatalysis holds great promise for renewable energy generation and environment remediation,but generally suffers from the serious drawbacks on light absorption,charge generation and transport,and structural stability that limit the performance.The core-shell semiconductorgraphene(CSSG)nanoarchitectures may address these issues due to their unique structures with exceptional physical and chemical properties.This review explores recent advances of the CSSG nanoarchitectures in the photocatalytic performance.It starts with the classification of the CSSG nanoarchitectures by the dimensionality.Then,the construction methods under internal and external driving forces were introduced and compared with each other.Afterward,the physicochemical properties and photocatalytic applications of these nanoarchitectures were discussed,with a focus on their role in photocatalysis.It ends with a summary and some perspectives on future development of the CSSG nanoarchitectures toward highly efficient photocatalysts with extensive application.By harnessing the synergistic capabilities of the CSSG architectures,we aim to address pressing environmental and energy challenges and drive scientific progress in these fields.展开更多
The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by ...The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.展开更多
The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To ad...The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To address such issue,herein,Fe-N_(x) sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution,thus enhancing the intrinsic catalytic activity.Precisely,atomically dispersed Fe-N_(x) sites supported on N/S-doped mesoporous carbon(NSC)coupled with FeS@C core-shell nanoparticles(FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis.Due to the presence of an in situ-grown conductive graphitic layer(shell),the FeS nanoparticles(core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions.Consequently,FAS-NSC@950displays a more positive half-wave potential(E_(1/2)) of 0.871 V with a significantly boosted ORR kinetics(Tafel slope=52.2 mV dec^(-1)),outpacing the commercial Pt/C(E_(1/2)=0.84 V and Tafel slope=54.6 mV dec^(-1)).As a bifunctional electrocatalyst,it displays a smaller bifunctional activity parameter(ΔE) of 0.673 V,surpassing the Pt/C-RuO_(2) combination(ΔE=0.724 V).Besides,the FAS-NSC@950-based zincair battery(ZAB) displays superior power density,specific capacity,and long-term cycling performance to the Pt/C-Ir/C-based ZAB.This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR,with potential implications for energy conversion and storage technologies.展开更多
The discharge morphology of pulsed dielectric barrier discharge(PDBD) plays important roles in its applications. Here, we systematically investigated the effects of the voltage amplitude,discharge gap, and O_(2)conten...The discharge morphology of pulsed dielectric barrier discharge(PDBD) plays important roles in its applications. Here, we systematically investigated the effects of the voltage amplitude,discharge gap, and O_(2)content on the PDBD morphology, and revealed the possible underlying mechanism of the U-shaped formation. First, the morphological evolution under different conditions was recorded. A unique U-shaped region appears in the middle edge region when the gap is larger than 2 mm, while the entire discharge region remains columnar under a 2 mm gap in He PDBD. The width of the discharge and the U-shaped region increase with the increase in voltage, and decrease with the increase of the gap and O_(2)content. To explain this phenomenon,a two-dimensional symmetric model was developed to simulate the spatiotemporal evolution of different species and calculate the electric thrust. The discharge morphology evolution directly corresponds to the excited-state atomic reduction process. The electric thrust on the charged particles mainly determines the reaction region and strongly influences the U-shaped formation.When the gap is less than 2 mm, the electric thrust is homogeneous throughout the entire region,resulting in a columnar shape. However, when the gap is larger than 2 mm or O_(2)is added, the electric thrust in the edge region becomes greater than that in the middle, leading to the U-shaped formation. Furthermore, in He PDBD, the charged particles generating electric thrust are mainly electrons and helium ions, while in He/O_(2)PDBD those that generate electric thrust at the outer edge of the electrode surface are mainly various oxygen-containing ions.展开更多
A covalent organic frameworks(COFs)material with regular pores and stable structure can be used as the host of lithium-sulfur batteries to improve battery kinetics and polysulfides conversion.Herein,we designed and sy...A covalent organic frameworks(COFs)material with regular pores and stable structure can be used as the host of lithium-sulfur batteries to improve battery kinetics and polysulfides conversion.Herein,we designed and synthesized two kinds of rod-liked bulk COFs by adjusting different pore sizes(COF-BTD and COF-TFB),unfortunately,the active sites masking and sluggish kinetics have not met our expectations.Generally,the available layered COFs prepared from mechanochemical can expose abundant active sites and favorable kinetics than bulk COFs.Thus,simple mechanical ball milling is applied to activate the above COFs(M-COFs group).It is worth noting that layered R-COF-BTD is directly synthesized from rod-liked precursors by simple morphological reconstruction.A series of characterization methods are used to systematically explore the advantages of the group of M-COFs@S electrodes in the cycling process,including the effects of specific morphology on the kinetics and transformation of polysulfides.Our research provides a feasible plan for the development and selection of the host material of lithium-sulfur batteries.展开更多
In the present work,the focus has been shifted to the relationship between the PANI morphology and the physicochemical properties,controlled by the amount of added ionic liquids,of the polymerization medium instead of...In the present work,the focus has been shifted to the relationship between the PANI morphology and the physicochemical properties,controlled by the amount of added ionic liquids,of the polymerization medium instead of focusing on the structure of the ionic liquids as used to be in the litterature.For that reason,PANI has been synthesized in different weight ratio of[Pyrr][PTS]/water following the standard experimental process.The addition of[Pyrr][PTS]into the polymerization medium controls the morphology of PANI without affecting its structure.Moreover,[Pyrr][PTS]promotes a viscous reaction system without the need of an external source.The viscosity of the polymerization system restricts the diffusion of species that leads to the predominance of the homogeneous nucleation mode during the course of polymerization and,thus,nanostructuring of PANI morphology.As for the ionic conductivity,it reflects the mobility of the ions of the polymerization medium and,thus,the way of its interference with the formed PANI that affects the arrangement and the shape of formed PANI fibers.This relationship between PANI morphology and the physicochemical properties,adjusted by adding ionic liquids,of the polymerization medium is prelaminar and promising.The effect of the ionic liquids on the viscosity as well as on the mobility of the polymerization medium have to be taken into consideration to choose the ionic liquids,which lead to the PANI with desired morphology.展开更多
Objectives To investigate the morphologic characteristics of intramural hematoma(IMH)on CT angiography(CTA),and evaluate the possible correlation of serum C-reactive protein(CRP)with morphologic characteristics of IMH...Objectives To investigate the morphologic characteristics of intramural hematoma(IMH)on CT angiography(CTA),and evaluate the possible correlation of serum C-reactive protein(CRP)with morphologic characteristics of IMH.Material and Methods Forty-two patients who were initially diagnosed as IMH by aortic CTA and also had serum CRP examination on the same day of CTA were enrolled in this retrospective study,including 30 males and 12 females,with the mean age of 61±14 years old.The volumetric CT data were retrospectively processed and analyzed on post-processing workstation.Based on the thickness of IMH and the length-area curve,the crosssectional area of true lumen and total vessel were measured,the hematoma-vessel ratio(HVR)was calculated.Imaging characteristics were compared between patients who had pathological elevated CRP(>0.8 mg/dl)and those did not.Spearman correlation analyses of CRP level and morphological characteristics of IMH were performed,and the receiver operating characteristic(ROC)curve was used to evaluate the diagnostic validity of CRP.Results Of all 42 IMH patients,the mean serum CRP was 3.94±4.71 mg/dl,and the mean HVR was 46.7%±14.2%.HVR in patients with elevated CRP was significantly higher than those with normal CRP(49.7%±15.0%vs.40.7%±10.5%,P=0.030).HVR was mildly correlated with CRP in all patients(r=0.48,P<0.001).CRP levels differed neither between patients with Stanford type A and B(P=0.207),nor between patients with and without intimal disruption(P=0.230).To discriminate HVR>47%(the mean value),the area under curve(AUC)were 0.700(95%CI:0.535-0.865)for CRP at a cutoff point of 3.55 mg/dl,with a sensitivity of 54.5%and a specificity of 90.0%.Conclusion CRP was mildly correlated with the severity of cross-sectional hematoma area of IMH,but not with Stanford types and the presence of intimal disruption.展开更多
Through one hundred years of adaptation in China, The Acer negundo Linn. (as hlea f maple), originally grown in North America, has developed morphological charact er istics to cope the severe situation of its habitats...Through one hundred years of adaptation in China, The Acer negundo Linn. (as hlea f maple), originally grown in North America, has developed morphological charact er istics to cope the severe situation of its habitats. Two ecotypes from different vegetation belts in the ecotone of eastern Inner Mongolia Autonomous Region wer e detected. Although there was no macroscopic difference, contrasting micro-ch a racteristics had been observed between the two sources. The leaves from more dro ught and warmer zone were found with more trichomes, more and smaller stomata, l arger subsidiary cells, thicker palisade and flatter epidermal wax than those of leaves from the more humid and colder zone. Microstructures of the leaves from xeric sources can more effectively reduce leaf temperature and conserving water than those of mesic sources. Intra-species difference of the two ecotypes is th e result of adaptation in different environments. This should be considered when characteristics of foliage are used as characters of species in taxonomy.展开更多
A series of ZSM-5 zeolites, with the morphologies of sphere, sphere with cubic particles on the surface, and cubic particles, were synthesized by hydrothermal method using n-butylamine as the template, assisted by the...A series of ZSM-5 zeolites, with the morphologies of sphere, sphere with cubic particles on the surface, and cubic particles, were synthesized by hydrothermal method using n-butylamine as the template, assisted by the addition of NaC1 and crystal seed. X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray fluorescence (XRF) and temperature-programmed desorption of ammonia (NH3-TPD) were used to characterize these samples. The samples were tested with toluene methylation reaction. The modified sample composed of spherical particles with 3 μm crystal particles on the surface had a para-xylene selectivity of 95% and maintained 79% of the initial conversion after running the reaction for 50 h. This modified samole showed the best stability amonz the tested three modified samoles.展开更多
The great implication of nanobubbles at a solid/water interface has drawn wide attention of the scientific community and industries. However, the fundamental properties of nanobubbles remain unknown as yet. In this pa...The great implication of nanobubbles at a solid/water interface has drawn wide attention of the scientific community and industries. However, the fundamental properties of nanobubbles remain unknown as yet. In this paper, the temperature effects on the morphology of nanobubbles at the mica/water interface are explored through the combination of AFM direct image with the temperature control. The results demonstrate that the apparent height of nanobubbles in AFM images is kept almost constant with the increase of temperature, whilst the lateral size of nanobubbles changes significantly. As the temperature increases from 28℃ to 42℃, the lateral size of nanobubbles increases, reaching a maximum at about 37℃, and then decreases at a higher temperature. The possible explanation for the size change of nanobubbles with temperature is suggested.展开更多
In this study,the impact of morphology of conductive agent and anode material(Fe3O4)on lithium storage properties was throughly investigated.Granular and belt-like Fe3O4active materials were separately blended with tw...In this study,the impact of morphology of conductive agent and anode material(Fe3O4)on lithium storage properties was throughly investigated.Granular and belt-like Fe3O4active materials were separately blended with two kinds of conductive agents(i.e.,granular acetylene black and multi-walled carbon nanotube)as anodes in lithium-ion batteries(LIBs),respectively.It was found that the morphology of conductive agent is of utmost importance in determining LIBs storage properties.In contrast,not as the way we anticipated,the morphology of anode material merely plays a subordinate role in their electrochemical performances.Further,the morphology-matching principle of electrode materials was discussed so as to render their utilization more rational and effective in LIBs.展开更多
Pore structure plays an important role in the gas storage and flow capacity of shale gas reservoirs. Fieldemission environmental scanning electron microscopy(FE-SEM) in combination with low-pressure carbon dioxide g...Pore structure plays an important role in the gas storage and flow capacity of shale gas reservoirs. Fieldemission environmental scanning electron microscopy(FE-SEM) in combination with low-pressure carbon dioxide gas adsorption(CO2GA),nitrogen gas adsorption(N2GA),and high-pressure mercury intrusion(HPMI) were used to study the nanostructure pore morphology and pore-size distributions(PSDs) of lacustrine shale from the Upper Triassic Yanchang Formation,Ordos Basin. Results show that the pores in the shale reservoirs are generally nanoscale and can be classified into four types: organic,interparticle,intraparticle,and microfracture. The interparticle pores between clay particles and organic-matter pores develop most often,l with pore sizes that vary from several to more than 100 nm. Mercury porosimetry analysis shows total porosities ranging between 1.93 and 7.68%,with a mean value of 5.27%. The BET surface areas as determined by N2 adsorption in the nine samples range from 10 to 20 m2/g and the CO2 equivalent surface areas(2 nm)vary from 18 to 71 m2/g. Together,the HPMI,N2 GA,and CO2 GA curves indicate that the pore volumes are mainly due to pores 100 nm in size. In contrast,however,most of the specific surface areas are provided by the micropores. The total organic carbon(TOC) and clay minerals are the primary controls of the structures of nanoscale pores(especially micropores and mesopores). Micropores are predominantly determined by the content of the TOC,and mesopores are possibly related to the content of clay minerals,particularly the illite-montmorillonite mixed-layer content.展开更多
Hierarchical ZnO@metal-organic framework @polyaniline(ZnO@MOF@PANI) core-shell nanorod arrays on carbon cloth has been fabricated by combining electrodeposition and hydrothermal method. Well-ordered Zn O nanorods not ...Hierarchical ZnO@metal-organic framework @polyaniline(ZnO@MOF@PANI) core-shell nanorod arrays on carbon cloth has been fabricated by combining electrodeposition and hydrothermal method. Well-ordered Zn O nanorods not only act as a scaffold for growth of MOF/PANI shell but also as Zn source for the formation of MOF. The morphology of ZnO@MOF@PANI composite is greatly influenced by the number of PANI electrodeposition cycles. Their structural and electrochemical properties were characterized with different techniques. The results indicate that the Zn O@MOF@PANI with 13 CV cycles of PANI deposition demonstrates the maximum specific capacitance of 340.7 F g-1 at 1.0 A g-1, good rate capability with84.3% capacitance retention from 1.0 to 10 A g-1 and excellent cycling life of 82.5% capacitance retention after 5000 cycles at high current density of 2.0 A g-1. This optimized core-shell nanoarchitecture endows the composite electrode with short ion diffusion pathway, rapid ion/electron transfer and high utilization of active materials, which thus result in excellent electrochemical performance of the ternary composite.展开更多
We present a path morphology method to separate total rock pore space into matrix, fractures and vugs and derive their pore structure spectrum. Thus, we can achieve fine pore evaluation in fracture–vug reservoirs bas...We present a path morphology method to separate total rock pore space into matrix, fractures and vugs and derive their pore structure spectrum. Thus, we can achieve fine pore evaluation in fracture–vug reservoirs based on electric imaging logging data. We automatically identify and extract fracture–vug information from the electric imaging images by adopting a path morphological operator that remains flexible enough to fit rectilinear and slightly curved structures because they are independent of the structuring element shape. The Otsu method was used to extract fracture–vug information from the background noise caused by the matrix. To accommodate the differences in scale and form of the different target regions,including fracture and vug path, operators with different lengths were selected for their recognition and extraction at the corresponding scale. Polynomial and elliptic functions are used to fit the extracted fractures and vugs, respectively, and the fracture–vug parameters are deduced from the fitted edge. Finally, test examples of numerical simulation data and several measured well data have been provided for the verification of the effectiveness and adaptability of the path morphology method in the application of electric imaging logging data processing. This also provides algorithm support for the fine evaluation of fracture–vug reservoirs.展开更多
基金supported by the National Natural Science Foundation of China(52161145409,21976116)SAFEA of China("Belt and Road”Innovative Talent Exchange Foreign Expert Project#2023041004L)(High-end Foreign Expert Project#G2023041021L)the Alexander-von-Humboldt Foundation of Germany(GroupLinkage Program)。
文摘Direct conversion of solar energy into chemical energy in an environmentally friendly manner is one of the most promising strategies to deal with the environmental pollution and energy crisis.Among a variety of materials developed as photocatalysts,the core-shell metal/covalent-organic framework(MOF or COF)photocatalysts have garnered significant attention due to their highly porous structure and the adjustability in both structure and functionality.The existing reviews on core-shell organic framework photocatalytic materials have mainly focused on core-shell MOF materials.However,there is still a lack of indepth reviews specifically addressing the photocatalytic performance of core-shell COFs and MOFs@COFs.Simultaneously,there is an urgent need for a comprehensive review encompassing these three types of core-shell structures.Based on this,this review aims to provide a comprehensive understanding and useful guidelines for the exploration of suitable core-shell organic framework photocatalysts towards appropriate photocatalytic energy conversion and environmental governance.Firstly,the classification,synthesis,formation mechanisms,and reasonable regulation of core-shell organic framework were summarized.Then,the photocatalytic applications of these three kinds of core-shell structures in different areas,such as H_(2)evolution,CO_(2)reduction,and pollutants degradation are emphasized.Finally,the main challenges and development prospects of core-shell organic framework photocatalysts were introduced.This review aims to provide insights into the development of a novel generation of efficient and stable core-shell organic framework materials for energy conversion and environmental remediation.
基金the support for this work by National Natural Science Foundation of China(Grant Nos.22175139 and 22105156)。
文摘The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves the pretreatment of HMX to endow—OH groups on the surface via polyalcohol bonding agent modification and in situ coating with nitrate ester-containing polymer,was proposed to address the problem.Two types of energetic polyether—glycidyl azide polymer(GAP)and nitrate modified GAP(GNP)were grafted onto HMX crystal based on isocyanate addition reaction bridged through neutral polymeric bonding agent(NPBA)layer.The morphology and structure of the HMX-based composites were characterized in detail and the core-shell structure was validated.The grafted polymers obviously enhanced the adhesion force between HMX crystals and fluoropolymer(F2314)binder.Due to the interfacial reinforcement among the components,the two HMX-based composites exhibited a remarkable increment of phase transition peak temperature by 10.2°C and 19.6°C with no more than 1.5%shell content,respectively.Furthermore,the impact and friction sensitivity of the composites decreased significantly as a result of the barrier produced by the grafted polymers.These findings will enhance the future prospects for the interface design of energetic composites aiming to solve the weak interface and safety concerns.
基金supported by the Fundamental Research Funds for the Central Universities(FRF-EYIT-23-07)。
文摘Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas denitrification.However,the conventional NH3production process,namely the Haber-Bosch process,leads to considerable energy consumption and waste gas emissions.To address this,electrocatalytic nitric oxide reduction reaction(NORR)has emerged as a promising strategy to bridge NH3consumption to NH3production,harnessing renewable electricity for a sustainable future.Copper(Cu)stands out as a prominent electrocatalyst for NO reduction,given its exceptional NH3yield and selectivity.However,a crucial aspect that remains insufficiently explored is the effects of morphology and valence states of Cu on the NORR performance.In this investigation,we synthesized CuO nanowires(CuO-NF)and Cu nanocubes(Cu-NF)as cathodes through an in situ growth method.Remarkably,CuO-NF exhibited an impressive NH3yield of 0.50±0.02 mg cm^(-2)h^(-1)at-0.6 V vs.reversible hydrogen electrode(RHE)with faradaic efficiency of29,68%±1,35%,surpassing that of Cu-NF(0.17±0.01 mg cm^(-2)h^(-1),16.18%±1.40%).Throughout the electroreduction process,secondary cubes were generated on the CuO-NF surface,preserving their nanosheet cluster morphology,sustained by an abundant supply of subsurface oxygen(s-O)even after an extended duration of 10 h,until s-O depletion ensued.Conversely,Cu-NF exhibited inadequate s-O content,leading to rapid crystal collapse within the same timeframe.The distinctive current-potential relationship,akin to a volcano-type curve,was attributed to distinct NO hydrogenation mechanisms.Further Tafel analysis revealed the exchange current density(i0)and standard heterogeneous rate constant(k0)for CuO-NF,yielding 3.44×10^(-6)A cm^(-2)and 3.77×10^(-6)cm^(-2)s^(-1)when NORR was driven by overpotentials.These findings revealed the potential of CuO-NF for NO reduction and provided insights into the intricate interplay between crystal morphology,valence states,and electrochemical performance.
基金supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2023R1A2C100571511,RS-2023-00254424)the Ministry of Education(2020R1A6A1A03038540)。
文摘As the global electric vehicle market continues to grow,the recycling of Li-ion battery (LIB) becomes more important worldwide and the resynthesis of cathode materials would be the most value-added recycling approach taking into account limited metal resources.Although resynthesized homogenous LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM) from spent LIB leachate shows comparable battery performance to pristine NCM from virgin materials,there is general concern in its cycling performance.Here,we synthesize core–shell(CS) Ni-rich NCM,which consists of Ni-rich NCM as the core and NCM derived from the original or purified leachate of spent LIBs as the shell.Resynthesized CS Ni-rich NCM exhibits improved rate capability resulting from expanded interslab thickness in the NCM structure.CS Ni-rich NCM from purified LIB leachate shows improvement in cycling performance and thermal stability.It specifically delivers a capacity retention of 86.6%at a high temperature after 80 cycles compared to that (75.0%) of pristine CS Ni-rich NCM.These improvements are caused by a relatively high Mg content on the shell and the widespread distribution of Al through the CS structure.CS Ni-rich NCM derived from spent LIB leachate provides a new alternative approach to conventional LIB recycling methods,which would utilize efficiently limited metal resources for the sustainable LIB production.
基金supported by the National Natural Science Foundation of China(61974125)the Open Innovation Fund for undergraduate students of Xiamen University(KFJJ-202411).
文摘Semiconductor photocatalysis holds great promise for renewable energy generation and environment remediation,but generally suffers from the serious drawbacks on light absorption,charge generation and transport,and structural stability that limit the performance.The core-shell semiconductorgraphene(CSSG)nanoarchitectures may address these issues due to their unique structures with exceptional physical and chemical properties.This review explores recent advances of the CSSG nanoarchitectures in the photocatalytic performance.It starts with the classification of the CSSG nanoarchitectures by the dimensionality.Then,the construction methods under internal and external driving forces were introduced and compared with each other.Afterward,the physicochemical properties and photocatalytic applications of these nanoarchitectures were discussed,with a focus on their role in photocatalysis.It ends with a summary and some perspectives on future development of the CSSG nanoarchitectures toward highly efficient photocatalysts with extensive application.By harnessing the synergistic capabilities of the CSSG architectures,we aim to address pressing environmental and energy challenges and drive scientific progress in these fields.
基金supported by the National Natural Science Foundation of China(Nos.22176145,82172612)the State Key Laboratory of Fine Chemicals,Dalian University of Technology(KF 2001)the Fundamental Research Funds for the Central Universities(22120210137).
文摘The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.
基金financially supported by the National Natural Science Foundation of China(21773024)the Natural Science Foundation of Sichuan Province of China(2023NSFC0084)the China Postdoctoral Science Foundation(2019M663469)。
文摘The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To address such issue,herein,Fe-N_(x) sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution,thus enhancing the intrinsic catalytic activity.Precisely,atomically dispersed Fe-N_(x) sites supported on N/S-doped mesoporous carbon(NSC)coupled with FeS@C core-shell nanoparticles(FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis.Due to the presence of an in situ-grown conductive graphitic layer(shell),the FeS nanoparticles(core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions.Consequently,FAS-NSC@950displays a more positive half-wave potential(E_(1/2)) of 0.871 V with a significantly boosted ORR kinetics(Tafel slope=52.2 mV dec^(-1)),outpacing the commercial Pt/C(E_(1/2)=0.84 V and Tafel slope=54.6 mV dec^(-1)).As a bifunctional electrocatalyst,it displays a smaller bifunctional activity parameter(ΔE) of 0.673 V,surpassing the Pt/C-RuO_(2) combination(ΔE=0.724 V).Besides,the FAS-NSC@950-based zincair battery(ZAB) displays superior power density,specific capacity,and long-term cycling performance to the Pt/C-Ir/C-based ZAB.This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR,with potential implications for energy conversion and storage technologies.
基金financial support from the Interdisciplinary Fund of the Wuhan National High Magnetic Field Center (No. WHMFC202101)。
文摘The discharge morphology of pulsed dielectric barrier discharge(PDBD) plays important roles in its applications. Here, we systematically investigated the effects of the voltage amplitude,discharge gap, and O_(2)content on the PDBD morphology, and revealed the possible underlying mechanism of the U-shaped formation. First, the morphological evolution under different conditions was recorded. A unique U-shaped region appears in the middle edge region when the gap is larger than 2 mm, while the entire discharge region remains columnar under a 2 mm gap in He PDBD. The width of the discharge and the U-shaped region increase with the increase in voltage, and decrease with the increase of the gap and O_(2)content. To explain this phenomenon,a two-dimensional symmetric model was developed to simulate the spatiotemporal evolution of different species and calculate the electric thrust. The discharge morphology evolution directly corresponds to the excited-state atomic reduction process. The electric thrust on the charged particles mainly determines the reaction region and strongly influences the U-shaped formation.When the gap is less than 2 mm, the electric thrust is homogeneous throughout the entire region,resulting in a columnar shape. However, when the gap is larger than 2 mm or O_(2)is added, the electric thrust in the edge region becomes greater than that in the middle, leading to the U-shaped formation. Furthermore, in He PDBD, the charged particles generating electric thrust are mainly electrons and helium ions, while in He/O_(2)PDBD those that generate electric thrust at the outer edge of the electrode surface are mainly various oxygen-containing ions.
基金supported by the National Natural Science Foundation of China,China(No.81927809).
文摘A covalent organic frameworks(COFs)material with regular pores and stable structure can be used as the host of lithium-sulfur batteries to improve battery kinetics and polysulfides conversion.Herein,we designed and synthesized two kinds of rod-liked bulk COFs by adjusting different pore sizes(COF-BTD and COF-TFB),unfortunately,the active sites masking and sluggish kinetics have not met our expectations.Generally,the available layered COFs prepared from mechanochemical can expose abundant active sites and favorable kinetics than bulk COFs.Thus,simple mechanical ball milling is applied to activate the above COFs(M-COFs group).It is worth noting that layered R-COF-BTD is directly synthesized from rod-liked precursors by simple morphological reconstruction.A series of characterization methods are used to systematically explore the advantages of the group of M-COFs@S electrodes in the cycling process,including the effects of specific morphology on the kinetics and transformation of polysulfides.Our research provides a feasible plan for the development and selection of the host material of lithium-sulfur batteries.
基金funded by RESCOLL French society and the Lebanese University。
文摘In the present work,the focus has been shifted to the relationship between the PANI morphology and the physicochemical properties,controlled by the amount of added ionic liquids,of the polymerization medium instead of focusing on the structure of the ionic liquids as used to be in the litterature.For that reason,PANI has been synthesized in different weight ratio of[Pyrr][PTS]/water following the standard experimental process.The addition of[Pyrr][PTS]into the polymerization medium controls the morphology of PANI without affecting its structure.Moreover,[Pyrr][PTS]promotes a viscous reaction system without the need of an external source.The viscosity of the polymerization system restricts the diffusion of species that leads to the predominance of the homogeneous nucleation mode during the course of polymerization and,thus,nanostructuring of PANI morphology.As for the ionic conductivity,it reflects the mobility of the ions of the polymerization medium and,thus,the way of its interference with the formed PANI that affects the arrangement and the shape of formed PANI fibers.This relationship between PANI morphology and the physicochemical properties,adjusted by adding ionic liquids,of the polymerization medium is prelaminar and promising.The effect of the ionic liquids on the viscosity as well as on the mobility of the polymerization medium have to be taken into consideration to choose the ionic liquids,which lead to the PANI with desired morphology.
基金Fund supported by the Clinical Research Supporting Fund of Chinese PLA General Hospital(2016FC-TSYS-1039)~~
文摘Objectives To investigate the morphologic characteristics of intramural hematoma(IMH)on CT angiography(CTA),and evaluate the possible correlation of serum C-reactive protein(CRP)with morphologic characteristics of IMH.Material and Methods Forty-two patients who were initially diagnosed as IMH by aortic CTA and also had serum CRP examination on the same day of CTA were enrolled in this retrospective study,including 30 males and 12 females,with the mean age of 61±14 years old.The volumetric CT data were retrospectively processed and analyzed on post-processing workstation.Based on the thickness of IMH and the length-area curve,the crosssectional area of true lumen and total vessel were measured,the hematoma-vessel ratio(HVR)was calculated.Imaging characteristics were compared between patients who had pathological elevated CRP(>0.8 mg/dl)and those did not.Spearman correlation analyses of CRP level and morphological characteristics of IMH were performed,and the receiver operating characteristic(ROC)curve was used to evaluate the diagnostic validity of CRP.Results Of all 42 IMH patients,the mean serum CRP was 3.94±4.71 mg/dl,and the mean HVR was 46.7%±14.2%.HVR in patients with elevated CRP was significantly higher than those with normal CRP(49.7%±15.0%vs.40.7%±10.5%,P=0.030).HVR was mildly correlated with CRP in all patients(r=0.48,P<0.001).CRP levels differed neither between patients with Stanford type A and B(P=0.207),nor between patients with and without intimal disruption(P=0.230).To discriminate HVR>47%(the mean value),the area under curve(AUC)were 0.700(95%CI:0.535-0.865)for CRP at a cutoff point of 3.55 mg/dl,with a sensitivity of 54.5%and a specificity of 90.0%.Conclusion CRP was mildly correlated with the severity of cross-sectional hematoma area of IMH,but not with Stanford types and the presence of intimal disruption.
文摘Through one hundred years of adaptation in China, The Acer negundo Linn. (as hlea f maple), originally grown in North America, has developed morphological charact er istics to cope the severe situation of its habitats. Two ecotypes from different vegetation belts in the ecotone of eastern Inner Mongolia Autonomous Region wer e detected. Although there was no macroscopic difference, contrasting micro-ch a racteristics had been observed between the two sources. The leaves from more dro ught and warmer zone were found with more trichomes, more and smaller stomata, l arger subsidiary cells, thicker palisade and flatter epidermal wax than those of leaves from the more humid and colder zone. Microstructures of the leaves from xeric sources can more effectively reduce leaf temperature and conserving water than those of mesic sources. Intra-species difference of the two ecotypes is th e result of adaptation in different environments. This should be considered when characteristics of foliage are used as characters of species in taxonomy.
文摘A series of ZSM-5 zeolites, with the morphologies of sphere, sphere with cubic particles on the surface, and cubic particles, were synthesized by hydrothermal method using n-butylamine as the template, assisted by the addition of NaC1 and crystal seed. X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray fluorescence (XRF) and temperature-programmed desorption of ammonia (NH3-TPD) were used to characterize these samples. The samples were tested with toluene methylation reaction. The modified sample composed of spherical particles with 3 μm crystal particles on the surface had a para-xylene selectivity of 95% and maintained 79% of the initial conversion after running the reaction for 50 h. This modified samole showed the best stability amonz the tested three modified samoles.
基金Project supported by the National Natural Science Foundation of China (Grant Nos 20403010 and 10335070) and the Science and Technology Commission of Shanghai Municipality (Grant Nos 0352nm116 and 0452nm007).
文摘The great implication of nanobubbles at a solid/water interface has drawn wide attention of the scientific community and industries. However, the fundamental properties of nanobubbles remain unknown as yet. In this paper, the temperature effects on the morphology of nanobubbles at the mica/water interface are explored through the combination of AFM direct image with the temperature control. The results demonstrate that the apparent height of nanobubbles in AFM images is kept almost constant with the increase of temperature, whilst the lateral size of nanobubbles changes significantly. As the temperature increases from 28℃ to 42℃, the lateral size of nanobubbles increases, reaching a maximum at about 37℃, and then decreases at a higher temperature. The possible explanation for the size change of nanobubbles with temperature is suggested.
基金financial aid from the National Natural Science Foundation of China(NSFC No.51472133)
文摘In this study,the impact of morphology of conductive agent and anode material(Fe3O4)on lithium storage properties was throughly investigated.Granular and belt-like Fe3O4active materials were separately blended with two kinds of conductive agents(i.e.,granular acetylene black and multi-walled carbon nanotube)as anodes in lithium-ion batteries(LIBs),respectively.It was found that the morphology of conductive agent is of utmost importance in determining LIBs storage properties.In contrast,not as the way we anticipated,the morphology of anode material merely plays a subordinate role in their electrochemical performances.Further,the morphology-matching principle of electrode materials was discussed so as to render their utilization more rational and effective in LIBs.
文摘Pore structure plays an important role in the gas storage and flow capacity of shale gas reservoirs. Fieldemission environmental scanning electron microscopy(FE-SEM) in combination with low-pressure carbon dioxide gas adsorption(CO2GA),nitrogen gas adsorption(N2GA),and high-pressure mercury intrusion(HPMI) were used to study the nanostructure pore morphology and pore-size distributions(PSDs) of lacustrine shale from the Upper Triassic Yanchang Formation,Ordos Basin. Results show that the pores in the shale reservoirs are generally nanoscale and can be classified into four types: organic,interparticle,intraparticle,and microfracture. The interparticle pores between clay particles and organic-matter pores develop most often,l with pore sizes that vary from several to more than 100 nm. Mercury porosimetry analysis shows total porosities ranging between 1.93 and 7.68%,with a mean value of 5.27%. The BET surface areas as determined by N2 adsorption in the nine samples range from 10 to 20 m2/g and the CO2 equivalent surface areas(2 nm)vary from 18 to 71 m2/g. Together,the HPMI,N2 GA,and CO2 GA curves indicate that the pore volumes are mainly due to pores 100 nm in size. In contrast,however,most of the specific surface areas are provided by the micropores. The total organic carbon(TOC) and clay minerals are the primary controls of the structures of nanoscale pores(especially micropores and mesopores). Micropores are predominantly determined by the content of the TOC,and mesopores are possibly related to the content of clay minerals,particularly the illite-montmorillonite mixed-layer content.
基金supported by the National Key R&D Program of China(2016YFE0131200)the National Natural Science Foundation of China(51702098)+1 种基金International Cooperation Project of Shanghai Municipal Science and Technology Committee(15520721100,18520744400)Research Program supported by the Ministry of Education,Youth,and Sports of the Czech Republic(LTACH17015)
文摘Hierarchical ZnO@metal-organic framework @polyaniline(ZnO@MOF@PANI) core-shell nanorod arrays on carbon cloth has been fabricated by combining electrodeposition and hydrothermal method. Well-ordered Zn O nanorods not only act as a scaffold for growth of MOF/PANI shell but also as Zn source for the formation of MOF. The morphology of ZnO@MOF@PANI composite is greatly influenced by the number of PANI electrodeposition cycles. Their structural and electrochemical properties were characterized with different techniques. The results indicate that the Zn O@MOF@PANI with 13 CV cycles of PANI deposition demonstrates the maximum specific capacitance of 340.7 F g-1 at 1.0 A g-1, good rate capability with84.3% capacitance retention from 1.0 to 10 A g-1 and excellent cycling life of 82.5% capacitance retention after 5000 cycles at high current density of 2.0 A g-1. This optimized core-shell nanoarchitecture endows the composite electrode with short ion diffusion pathway, rapid ion/electron transfer and high utilization of active materials, which thus result in excellent electrochemical performance of the ternary composite.
基金granted access to projects supported by the National Major Fundamental Research Program of China ‘‘On basic research problems in applied geophysics for deep oil and gas fields’’(Grant Number 2013CB228605)CNPC Science and Technology Project(Grant Number 2016A-3303)and CNPC Logging Project(Grant Number 2017E-15)
文摘We present a path morphology method to separate total rock pore space into matrix, fractures and vugs and derive their pore structure spectrum. Thus, we can achieve fine pore evaluation in fracture–vug reservoirs based on electric imaging logging data. We automatically identify and extract fracture–vug information from the electric imaging images by adopting a path morphological operator that remains flexible enough to fit rectilinear and slightly curved structures because they are independent of the structuring element shape. The Otsu method was used to extract fracture–vug information from the background noise caused by the matrix. To accommodate the differences in scale and form of the different target regions,including fracture and vug path, operators with different lengths were selected for their recognition and extraction at the corresponding scale. Polynomial and elliptic functions are used to fit the extracted fractures and vugs, respectively, and the fracture–vug parameters are deduced from the fitted edge. Finally, test examples of numerical simulation data and several measured well data have been provided for the verification of the effectiveness and adaptability of the path morphology method in the application of electric imaging logging data processing. This also provides algorithm support for the fine evaluation of fracture–vug reservoirs.