Mesoscale interplay among composition heterogeneity,lattice deformation,and redox stratification in single-crystalline layered oxide cathode

Single-crystalline layered oxide materials for lithium-ion batteries are featured by their excellent capacity retention over their polycrystalline counterparts,making them sought-after cathode candidates.Their capacity degradation,however,becomes more severe under high-voltage cycling,hindering many high-energy applications.It has long been speculated that the interplay among composition heterogeneity,lattice deformation,and redox stratification could be a driving force for the performance decay.The underlying mechanism,however,is not well-understood.In this study,we use X-ray microscopy to systematically examine single-crystalline NMC particles at the mesoscale.This technique allows us to capture detailed signals of diffraction,spectroscopy,and fluorescence,offering spatially resolved multimodal insights.Focusing on early high-voltage charging cycles,we uncover heterogeneities in valence states and lattice structures that are inherent rather than caused by electrochemical abuse.These heterogeneities are closely associated with compositional variations within individual particles.Our findings provide useful insights for refining material synthesis and processing for enhanced battery longevity and efficiency.

COMPOSITIONAL HETEROGENEITY OF ETHYLENE OXIDE-BUTYLENE TEREPHTHALATE SEGMENTED COPOLYMER

A series of ethylene oxide-butylene terephthalate (EOBT) segmented copolymers with different soft segment length and hard segment content were synthesized. The compositional heterogeneity was studied by solvent extraction. The results show that the compositional heterogeneity increases when soft segment length and hard segment content increase. The compositional heterogeneity is also reflected in the crystallization behavior and morphology of soft and hard segment in EOBT segmented copolymer. The more compositional heterogeneous the EOBT segmented copolymer is, the more different the morphology and the crystallization behavior between separated fractions. Compared with ethylene oxide-ethylene terephthalate (EOET) segmented copolymer, compositional heterogeneity in EOBT segmented copolymer is weaker. But the compositional heterogeneity in EOBT segmented copolymer with long soft segment and high hard segment content is still obvious.

Achieving high strength and ductility in high-entropy alloys via spinodal decomposition-induced compositional heterogeneity

The compositional heterogeneity in high-entropy alloys(HEAs)has been reported to be an inherent en-tity,which significantly alters the mechanical properties of materials by tuning the variation of lattice resistance for dislocation motion.However,since the body-centered cubic(BCC)structure is not close-packed,the change of lattice resistance is less sensitive to the normal concentration wave compared to that in face-centered cubic(FCC)structured materials.In this work,we selected a refractory bcc HEAs TiZrNbTa for the matrix and added a small amount of Al to facilitate the special spinodal decomposition structure.In particular,(TiZrNbTa)98.5 Al 1.5 displayed a typical basket-weave fabric morphology of spinodal decomposition structure with a characteristic periodicity of∼8 nm and had an optimal combination of strength and ductility(the yield strength of 1123±9 MPa and ductility of∼20.7%±0.6%).It was de-termined that by doing in situ TEM mechanical testing,the plastic deformation was dominated by the formation and operation of dislocation loops which provided both edge and screw components of dislo-cations.The synergetic effect of the remarkable chemical heterogeneity created by the spinodal decompo-sition and the spreading lattice distortion in high entropy alloys is quite effective in tuning the mobility of different types of dislocations and facilitates dislocation interactions,enabling the combination of high strength and ductility.

Evolutionary timescale of chalcidoid wasps inferred from over one hundred mitochondrial genomes

Chalcidoidea is one of the most biologically diverse groups among Hymenoptera.Members are characterized by extraordinary parasitic lifestyles and extensive host ranges,among which several species attack plants or serve as pollinators.However,higher-level chalcidoid relationships remain controversial.Here,we performed mitochondrial phylogenomic analyses for major clades(18out of 25 families)of Chalcidoidea based on 139 mitochondrial genomes.The compositional heterogeneity and conflicting backbone relationships in Chalcidoidea were assessed using various datasets and tree inferences.Our phylogenetic results supported the monophyly of 16families and polyphyly of Aphelinidae and Pteromalidae.Our preferred topology recovered the relationship(Mymaridae+(Signiphoridae+Leucospidae)+(Chalcididae+((Perilampidae+Eucharitidae)+remaining Chalcidoidea))).The monophyly of Agaonidae and Sycophaginae was rejected,while the gall-associated((Megastigmidae+Ormyridae)+(Ormocerinae+Eurytomidae))relationship was supported in most results.A six-gene inversion may be a synapomorphy for most families,whereas other derived gene orders may introduce confusion in phylogenetic signals at deeper nodes.Dating estimates suggested that Chalcidoidea arose near the Jurassic/Cretaceous boundary and that two dynamic shifts in diversification occurred during the evolution of Chalcidoidea.We hypothesized that the potential codiversification between chalcidoids and their hosts may be crucial for accelerating the diversification of Chalcidoidea.Ancestral state reconstruction analyses supported the hypothesis that gallinducers were mainly derived from parasitoids of gallinducers,while other gall-inducers were derived from phytophagous groups.Taken together,these findings advance our understanding of mitochondrial genome evolution in the major interfamilial phylogeny of Chalcidoidea.

Characteristics and Origin of Yacheng Gas Field in Qiongdongnan Basin,South China Sea

The Yacheng gas field lies in the foot wall of the No. 1 fault, the boundary fault between the Yinggehai and Qiongdongnan basins. An overpressured system developed in the Meishan Formation near the No. 1 fault in the gas field and in the adjacent Yinggehai basin. Away from this fault into the Qiongdongnan basin, the overpressure diminishes. Below 3 600 m in the gas field, an obvious thermal anomaly occurs. The gases show obvious compositional heterogeneities which reflect reservoir filling process and origin of the gas field. The gas field was charged from both the Qiongdongnan and the Yinggehai basins but mainly from the former. Hydrocarbons sourced from the Qiongdongnan basin have relatively low maturities while hydrocarbons from the Yinggehai basin have relatively high maturities.

Heterogeneous MXene-based films with graded electrical conductivity towards highly efficient EMI shielding and electrothermal heating

The increasing need for electromagnetic interference(EMI)shielding of electronics in cold environments such as those in aircraft,space exploration,and wearable heaters to avoid hazardous icing conditions or hypothermia requires the development of thin and lightweight EMI shielding materials preferably by absorbing rather than reflecting electromagnetic(EM)waves while also generating heat through energy-efficient electrothermal conversion.However,it is challenging to achieve absorption-dominant EMI shielding and energy-efficient electrothermal heating simultaneously in a thin and lightweight structure.Here,we develop a heterogeneous composite film comprising a porous multi-walled carbon nanotubes(MWCNTs)/bacterial cellulose(BC)film and an aligned MXene/Ag nanowires(NWs)backing via a sequential vacuum filtration process.The porous film contains random conductive networks of MWCNTs with moderate conductivity while the aligned MXene sheets atop Ag NWs network affords high conductivity in the backing,giving rise to graded electrical conductivity for absorption-dominant EMI shielding.The increasing Ag NW coverage leads to significantly increased electrical conductivity without increasing the EM wave reflection as well as the density and thickness of the film,yielding excellent specific EMI shielding effectiveness(>8500 dB/(g·cm^(2))),low driving voltage for energy-efficient electrothermal heating(163℃at 2.5 V),and fast response time(60 s)at a low areal density of 0.015 mg/cm^(2).Combining EMI shielding and electrothermal heating,the heterogeneous film developed here are promising contenders for the protection of electronic equipment in low-temperature environment.

Regulating Oxygen Vacancy Defects in Heterogeneous NiO-CeO_(2)−δ Hollow Multi-shelled Structure for Boosting Oxygen Evolution Reaction

CeO_(2) with excellent oxygen storage-exchange capacity and NiO with excellent surface activity were used to construct a heterogeneous NiO-CeO_(2)−δhollow multi-shelled structure(HoMS)by spray drying.It turned out that as the proportion of CeO_(2) increases,the overpotential and Tafel slope of NiO-CeO_(2)−δHoMSs first decreased and then increased.This is mainly because the construction of the NiO-CeO_(2)−δHoMSs not only increases the specific surface area,but also introduces oxygen vacancy defects,thus improving the interface charge transfer capability of the materials and further improving the oxygen evolution reaction(OER)performance.However,the increase of the calcination temperature will induce the decay of the OER performance of NiO-CeO_(2)−δHoMSs,which is mainly due to the decrease of the specific surface area,the reduction of oxygen vacancy defects,and the weakening of interface charge transfer capability.Furthermore,a series of heterogeneous composite HoMSs,such as Ni/Co,Mo/Ni,Al/Ni and Fe/Ni oxides was successfully constructed by spray drying,which enriched the diversity of HoMSs.