Synchrotron radiation (SR) provides highly brilliant light with tunable wavelength from hard X-ray to far infrared, on which scattering, spectroscopy and imaging techniques with high time and spatial resolutions hav...Synchrotron radiation (SR) provides highly brilliant light with tunable wavelength from hard X-ray to far infrared, on which scattering, spectroscopy and imaging techniques with high time and spatial resolutions have been developed for in situ study on biological system and materials like polymer. With examples on flow-induced crystallization of polymer, deformation of nanoparticle filler network in rubber composite and necking propagation in tensile stretch, current work attempts to demonstrate the advantages of in situ synchrotron radiation X-ray scattering, X-ray nano-CT and infrared imaging in the study of deformation-induced multi-scale structural evolutions of polymers. With time resolution up to sub-ms, synchrotron radiation is expected to play a great role in understanding non-equilibrium polymer physics under processing and service conditions, while high-throughput characterization platform based on synchrotron radiation opens the possibility to establish polymer Materials Genome database in processing parameter space within reasonable time, which can serve as the roadmap for industrial polymer processing and accelerate material innovation.展开更多
Simultaneously realizing improved activity and stability of acidic oxygen evolution reaction(OER) electrocatalysts is highly promising for developing cost-effective sustainable energy in the splitting of water techniq...Simultaneously realizing improved activity and stability of acidic oxygen evolution reaction(OER) electrocatalysts is highly promising for developing cost-effective sustainable energy in the splitting of water technique.Herein,we report iridium nanocrystals embedded into 3D conductive clothes(Ir-NCT/CC) as a low iridium electrocatalyst realizing ultrahigh acidic OER activity and robust stability.The well-designed Ir-NCT/CC requires a low overpotential of 202 mV to reach the current density of 10 mA cm^(-2)with a high mass activity of 1754 A g^(-1).Importantly,in acidic overall water splitting,Ir-NCT/CC merely delivers a cell voltage of 1.469 V at a typical current density of 10 mA cm^(-2)and also maintains robust durability under continuous operation.We identify that a low working voltage drives the formation of a highly stable amorphous IrOxactive phase over the surface of Ir nanocrystals(surface heterojunction IrOx/Ir-NCT) during operating conditions,which contributes to an effective and durable OER process.展开更多
Excessive inter-contamination with heavy metals hampers the application of biological treatment products derived from mixed or mechanically-sorted municipal solid waste(MSW). In this study, we investigated fine part...Excessive inter-contamination with heavy metals hampers the application of biological treatment products derived from mixed or mechanically-sorted municipal solid waste(MSW). In this study, we investigated fine particles of 〈 2 mm, which are small fractions in MSW but constitute a significant component of the total heavy metal content, using bulk detection techniques. A total of 17 individual fine particles were evaluated using synchrotron radiation-based micro-X-ray fluorescence and micro-X-ray diffraction. We also discussed the association, speciation and source apportionment of heavy metals. Metals were found to exist in a diffuse distribution with heterogeneous intensities and intense hot-spots of 〈 10 μm within the fine particles. Zn–Cu, Pb–Fe and Fe–Mn–Cr had significant correlations in terms of spatial distribution. The overlapped enrichment, spatial association, and the mineral phases of metals revealed the potential sources of fine particles from size-reduced waste fractions(such as scraps of organic wastes or ceramics) or from the importation of other particles. The diverse sources of heavy metal pollutants within the fine particles suggested that separate collection and treatment of the biodegradable waste fraction(such as food waste) is a preferable means of facilitating the beneficial utilization of the stabilized products.展开更多
In this work, we present a feasible scheme based on framework of the sophisticated Voronoi tessellation method in order to evaluate what clusters should be preferred for building blocks in any given metallic glass, by...In this work, we present a feasible scheme based on framework of the sophisticated Voronoi tessellation method in order to evaluate what clusters should be preferred for building blocks in any given metallic glass, by analysing the fivefold-symmetry axes as well as the degree of structural regularity in various clusters. This scheme is well proved by a group of experiments and calculations, which may have broad implications for exploration of obtaining explicit and proper structural pictures, and understanding the structural origin of the unique properties and glass forming ability in these novel amorphous alloys.展开更多
The present study aims to monitor and assess the water quality of the Bezerra River located in the Western Brazilian Parana state. For the monitoring of river waters, six samplings were established per month during on...The present study aims to monitor and assess the water quality of the Bezerra River located in the Western Brazilian Parana state. For the monitoring of river waters, six samplings were established per month during one year. As indicators of the water quality, physico-chemical parameters such as water temperature, pH, turbidity, dissolved oxygen and COD (chemical oxygen demand) were chosen, as well as trace and majority element concentrations. It is noteworthy that the mean annual values of conductivity, turbidity and COD have progressively increased along the river with maximum values after the Cascavel western sewage treatment plant. Only 13 elements were found in the six collection points, but the metallic elements Cr, Mn, Fe, Cu and Zn have shown concentrations above the maximum limits recommended by Brazilian environmental legislation, suggesting the presence of highly polluting anthropogenic sources. Correlation analyses were used to determine the spatio-variability of water quality variables. The six collection sites were grouped into two clusters, with the element composition in the first cluster (sites 1, 2 and 6) being due to strong anthropogenic activities. The study of the Bezerra River water quality could help to develop municipal environmental policies and help with the management of water conservation in the Bezerra River basin.展开更多
Liberty State Park in New Jersey,USA,is a "brownfield" site containing various levels of contaminants.To investigate metal uptake and distributions in plants on the brownfield site,Phragmites australis and Typha lat...Liberty State Park in New Jersey,USA,is a "brownfield" site containing various levels of contaminants.To investigate metal uptake and distributions in plants on the brownfield site,Phragmites australis and Typha latifolia were collected in Liberty State Park during the growing season(May–September)in 2011 at two sites with the high and low metal loads,respectively.The objective of this study was to understand the metal(Fe,Mn,Cu,Pb and Zn)concentration and spatial distributions in P.australis and T.latifolia root systems with micro-meter scale resolution using synchrotron X-ray microfluorescence(μXRF)and synchrotron X-ray computed microtomography(μCMT)techniques.The root structure measurement by synchrotron μCMT showed that high X-ray attenuation substance appeared in the epidermis.Synchrotron μXRF measurement showed that metal concentrations and distributions in the root cross-section between epidermis and vascular tissue were statistically different.Significant correlations were found between metals(Cu,Mn,Pb and Zn)and Fe in the epidermis,implying that metals were scavenged by Fe oxides.The results from this study suggest that the expression of metal transport and accumulation within the root systems may be element specific.The information derived from this study can improve our current knowledge of the wetland plant ecological function in brownfield remediation.展开更多
The neutral oxygen reduction reaction(ORR)has attracted tremendous attention for its broad prospects in next-generation power storage systems.However,the extremely sluggish cathodic reaction process and the limited co...The neutral oxygen reduction reaction(ORR)has attracted tremendous attention for its broad prospects in next-generation power storage systems.However,the extremely sluggish cathodic reaction process and the limited cognition of the reaction mechanism greatly hinder its practical application.Here,we demonstrate a dynamic reconstruction behavior induced by sulfur of the iron-nitrogen(Fe-Nx)species in neutral solution.Our developed FeS_(1)N_(3)-OH configuration effectively optimizes the reaction kinetics by regulating the adsorption energy of oxygen intermediates for central catalytic sites.Consequently,this structure exhibits over 363%enhancement in ORR mass activity compared to the pristine FeN_(4) sites under neutral electrolyte.Moreover,a neutral zinc-air battery assembled with this electrocatalyst reached an ultrahigh peak power density(81.2 mW cm^(−2)),robust stability(more than 100 h)as well as superior tolerance to extreme environments(operating between−20°C and 60°C),representing a critical breakthrough for neutral ORR exploration and application.展开更多
Fluorinated and nitrogen-doped graphdiyne(F/N-GDY)have been used in the active layer of perovskite solar cells(PSCs)for the first time.The introduction of heteroatoms turns out to be an effective method for boosted so...Fluorinated and nitrogen-doped graphdiyne(F/N-GDY)have been used in the active layer of perovskite solar cells(PSCs)for the first time.The introduction of heteroatoms turns out to be an effective method for boosted solar cells performance,which increases by 32.8%and 33.0%,better than the pristine or GDY doped PSCs.The enhanced performance can be attributed firstly to the superiority of F/N-GDY originated from the unique structure and optoelectronic properties of GDY.Then,both can further reduce surface defects and improve surface and bulk crystallinity than pristine GDY.What's more,efficiency increase caused by F-GDY is mainly attributed to the improvement of fill factor(FF),while the higher short-circuit current(Jsc)plays more important role by N-GDY doping.Most importantly,the detailed mechanism brought about by doping of F-GDY or N-GDY is expounded by systematical characterizations,especially the synchrotron radiation technique.Doping of F-GDY causes Pb and forms new Pb-F bonds between F-GDY and Pb ions.Doping of N-GDY or GDY brings about Pb(N-GDY doping induces more deviation than that of GDY due to the participation of imine N),improving its electron density and conductivity.展开更多
基金financially supported by the National Natural Science Foundation of China (No. 51633009)
文摘Synchrotron radiation (SR) provides highly brilliant light with tunable wavelength from hard X-ray to far infrared, on which scattering, spectroscopy and imaging techniques with high time and spatial resolutions have been developed for in situ study on biological system and materials like polymer. With examples on flow-induced crystallization of polymer, deformation of nanoparticle filler network in rubber composite and necking propagation in tensile stretch, current work attempts to demonstrate the advantages of in situ synchrotron radiation X-ray scattering, X-ray nano-CT and infrared imaging in the study of deformation-induced multi-scale structural evolutions of polymers. With time resolution up to sub-ms, synchrotron radiation is expected to play a great role in understanding non-equilibrium polymer physics under processing and service conditions, while high-throughput characterization platform based on synchrotron radiation opens the possibility to establish polymer Materials Genome database in processing parameter space within reasonable time, which can serve as the roadmap for industrial polymer processing and accelerate material innovation.
基金supported by the National Natural Science Foundation of China(12205300 and 12135012)the Natural Science Foundation of Anhui Province(2208085QA28 and 2208085J01)。
文摘Simultaneously realizing improved activity and stability of acidic oxygen evolution reaction(OER) electrocatalysts is highly promising for developing cost-effective sustainable energy in the splitting of water technique.Herein,we report iridium nanocrystals embedded into 3D conductive clothes(Ir-NCT/CC) as a low iridium electrocatalyst realizing ultrahigh acidic OER activity and robust stability.The well-designed Ir-NCT/CC requires a low overpotential of 202 mV to reach the current density of 10 mA cm^(-2)with a high mass activity of 1754 A g^(-1).Importantly,in acidic overall water splitting,Ir-NCT/CC merely delivers a cell voltage of 1.469 V at a typical current density of 10 mA cm^(-2)and also maintains robust durability under continuous operation.We identify that a low working voltage drives the formation of a highly stable amorphous IrOxactive phase over the surface of Ir nanocrystals(surface heterojunction IrOx/Ir-NCT) during operating conditions,which contributes to an effective and durable OER process.
基金supported by the National Basic Research Program of China (No. 2011CB201500)the National Social Science Fund of China (No. 12&ZD236)the National Natural Science Foundation of China (No. 21277096)
文摘Excessive inter-contamination with heavy metals hampers the application of biological treatment products derived from mixed or mechanically-sorted municipal solid waste(MSW). In this study, we investigated fine particles of 〈 2 mm, which are small fractions in MSW but constitute a significant component of the total heavy metal content, using bulk detection techniques. A total of 17 individual fine particles were evaluated using synchrotron radiation-based micro-X-ray fluorescence and micro-X-ray diffraction. We also discussed the association, speciation and source apportionment of heavy metals. Metals were found to exist in a diffuse distribution with heterogeneous intensities and intense hot-spots of 〈 10 μm within the fine particles. Zn–Cu, Pb–Fe and Fe–Mn–Cr had significant correlations in terms of spatial distribution. The overlapped enrichment, spatial association, and the mineral phases of metals revealed the potential sources of fine particles from size-reduced waste fractions(such as scraps of organic wastes or ceramics) or from the importation of other particles. The diverse sources of heavy metal pollutants within the fine particles suggested that separate collection and treatment of the biodegradable waste fraction(such as food waste) is a preferable means of facilitating the beneficial utilization of the stabilized products.
基金Project supported by the National Natural Science Foundation of China (Grant No. 10805027)the Natural Science Foundation of Jiangsu Province of China (Grant No. BK2008397)the Nanjing University of Aeronautics and Astronautics Research Funding,China (Grant No. NS2010168)
文摘In this work, we present a feasible scheme based on framework of the sophisticated Voronoi tessellation method in order to evaluate what clusters should be preferred for building blocks in any given metallic glass, by analysing the fivefold-symmetry axes as well as the degree of structural regularity in various clusters. This scheme is well proved by a group of experiments and calculations, which may have broad implications for exploration of obtaining explicit and proper structural pictures, and understanding the structural origin of the unique properties and glass forming ability in these novel amorphous alloys.
文摘The present study aims to monitor and assess the water quality of the Bezerra River located in the Western Brazilian Parana state. For the monitoring of river waters, six samplings were established per month during one year. As indicators of the water quality, physico-chemical parameters such as water temperature, pH, turbidity, dissolved oxygen and COD (chemical oxygen demand) were chosen, as well as trace and majority element concentrations. It is noteworthy that the mean annual values of conductivity, turbidity and COD have progressively increased along the river with maximum values after the Cascavel western sewage treatment plant. Only 13 elements were found in the six collection points, but the metallic elements Cr, Mn, Fe, Cu and Zn have shown concentrations above the maximum limits recommended by Brazilian environmental legislation, suggesting the presence of highly polluting anthropogenic sources. Correlation analyses were used to determine the spatio-variability of water quality variables. The six collection sites were grouped into two clusters, with the element composition in the first cluster (sites 1, 2 and 6) being due to strong anthropogenic activities. The study of the Bezerra River water quality could help to develop municipal environmental policies and help with the management of water conservation in the Bezerra River basin.
基金supported in part by the Margaret and Herman Sokol Foundation(HF)China Scholarship Council(YQ)+6 种基金the State Key Laboratory of Estuarine and Coastal Research Open Research Fund(Ref #:SKLEC-KF201304)(HF,WZ,LY,YQ)supported in part by the U.S.Department of Energy,Office of Science,Office of Workforce Development for Teachers and Scientists(WDTS)under the Visiting Faculty Program(VFP)(HF)Portions of this work were performed at Beamline X27A,National Synchrotron Light Source(NSLS),and Biosciences Department,Brookhaven National LaboratoryWork in Bioscience Department,BNL,was partially supported by the Division of Chemical Sciences,Geosciences,and Biosciences,Office of Basic Energy Sciences of the US Department of Energy through Grant DEAC0298CH10886the National Science Foundation through grant MCB-1051675(CJL)X27A is supported in part by the U.S.Department of Energy--Geosciences(DE-FG02-92ER14244 to The University of Chicago-CARS)Use of the NSLS was supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,under Contract No.DE-AC02-98CH10886
文摘Liberty State Park in New Jersey,USA,is a "brownfield" site containing various levels of contaminants.To investigate metal uptake and distributions in plants on the brownfield site,Phragmites australis and Typha latifolia were collected in Liberty State Park during the growing season(May–September)in 2011 at two sites with the high and low metal loads,respectively.The objective of this study was to understand the metal(Fe,Mn,Cu,Pb and Zn)concentration and spatial distributions in P.australis and T.latifolia root systems with micro-meter scale resolution using synchrotron X-ray microfluorescence(μXRF)and synchrotron X-ray computed microtomography(μCMT)techniques.The root structure measurement by synchrotron μCMT showed that high X-ray attenuation substance appeared in the epidermis.Synchrotron μXRF measurement showed that metal concentrations and distributions in the root cross-section between epidermis and vascular tissue were statistically different.Significant correlations were found between metals(Cu,Mn,Pb and Zn)and Fe in the epidermis,implying that metals were scavenged by Fe oxides.The results from this study suggest that the expression of metal transport and accumulation within the root systems may be element specific.The information derived from this study can improve our current knowledge of the wetland plant ecological function in brownfield remediation.
基金financially supported by the National Natural Science Foundation of China(No.21925110,91745113,22102170,21890751)the National Program for Support of Top-Notch Young Professionals+3 种基金the Fundamental Research Funds for the Central Universities(No.WK 2060190084)the Youth Innovation Promotion Association of Chinese academy of Sciences(No.Y201877)the Institute of Energy,Hefei Comprehensive National Science Center(Grant No.21KZS213)the support from the Major/Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology。
文摘The neutral oxygen reduction reaction(ORR)has attracted tremendous attention for its broad prospects in next-generation power storage systems.However,the extremely sluggish cathodic reaction process and the limited cognition of the reaction mechanism greatly hinder its practical application.Here,we demonstrate a dynamic reconstruction behavior induced by sulfur of the iron-nitrogen(Fe-Nx)species in neutral solution.Our developed FeS_(1)N_(3)-OH configuration effectively optimizes the reaction kinetics by regulating the adsorption energy of oxygen intermediates for central catalytic sites.Consequently,this structure exhibits over 363%enhancement in ORR mass activity compared to the pristine FeN_(4) sites under neutral electrolyte.Moreover,a neutral zinc-air battery assembled with this electrocatalyst reached an ultrahigh peak power density(81.2 mW cm^(−2)),robust stability(more than 100 h)as well as superior tolerance to extreme environments(operating between−20°C and 60°C),representing a critical breakthrough for neutral ORR exploration and application.
基金supported financially by the National Key Research and Development Program of China(Nos.2018YFA0703504 and 2017YFA0403403)the National Basic Research Program of China(No.2016YFA0203200)+1 种基金the National Natural Science Foundation of China(Nos.21971242,11705211,and U1532104)Young Scientist Innovative Foundation of IHEP(Nos.E05469U2 and Y95461C).
文摘Fluorinated and nitrogen-doped graphdiyne(F/N-GDY)have been used in the active layer of perovskite solar cells(PSCs)for the first time.The introduction of heteroatoms turns out to be an effective method for boosted solar cells performance,which increases by 32.8%and 33.0%,better than the pristine or GDY doped PSCs.The enhanced performance can be attributed firstly to the superiority of F/N-GDY originated from the unique structure and optoelectronic properties of GDY.Then,both can further reduce surface defects and improve surface and bulk crystallinity than pristine GDY.What's more,efficiency increase caused by F-GDY is mainly attributed to the improvement of fill factor(FF),while the higher short-circuit current(Jsc)plays more important role by N-GDY doping.Most importantly,the detailed mechanism brought about by doping of F-GDY or N-GDY is expounded by systematical characterizations,especially the synchrotron radiation technique.Doping of F-GDY causes Pb and forms new Pb-F bonds between F-GDY and Pb ions.Doping of N-GDY or GDY brings about Pb(N-GDY doping induces more deviation than that of GDY due to the participation of imine N),improving its electron density and conductivity.