In Situ Synchrotron Radiation Techniques: Watching Deformation-induced Structural Evolutions of Polymers

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.

Dynamically-evolved surface heterojunction in iridium nanocrystals boosting acidic oxygen evolution and overall water splitting

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.

Insights into metals in individual fine particles from municipal solid waste using synchrotron radiation-based micro-analytical techniques

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.

Preferred clusters in metallic glasses

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.

Synchrotron micro-scale measurement of metal distributions in Phragmites australis and Typha latifolia root tissue from an urban brownfield site

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.

Sulfur-induced dynamic reconstruction of iron-nitrogen species for highly active neutral oxygen reduction reactions

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.

Different mechanisms of improving CH_(3)NH_(3)PbI_(3) perovskite solar cells brought by fluorinated or nitrogen doped graphdiyne

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.