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Highlights The well-conceived Pt–Ni3S2 heteronanocrystals with dual-monodispersed characteristics are synthesized through interfacial electronic modulation. The asymmetrical charge distribution at Pt–Ni3S2 hetero-interface results in the formation of high-valent Ni sites and negatively-charged Pt δ−. It eventually accelerates water dissociation and achieves the steady concurrent generation of value-added formate and hydrogen.

Abstract Solid electrolyte is vital to ensure all-solid-state batteries with improved safety, long cyclability, and feasibility at different temperatures. Herein, we report a new family of amorphous solid electrolytes, xLi2O-MCly (M = Ta or Hf, 0.8 ≤ x ≤ 2, y = 5 or 4). xLi2O-MCly amorphous solid electrolytes can achieve desirable ionic conductivities up to 6.6 × 10−3 S cm−1 at 25 °C, which is one of the highest values among all the reported amorphous solid electrolytes and comparable to those of the popular crystalline ones. The mixed-anion structural models of xLi2O-MCly amorphous SEs are well established and correlated to the ionic conductivities. It is found that the oxygen-jointed anion networks with abundant terminal chlorines in xLi2O-MCly amorphous solid electrolytes play an important role for the fast Li-ion conduction. More importantly, all-solid-state batteries using the amorphous solid electrolytes show excellent electrochemical performance at both 25 °C and −10 °C. Long cycle life (more than 2400 times of charging and discharging) can be achieved for all-solid-state batteries using the xLi2O-TaCl5 amorphous solid electrolyte at 400 mA g−1, demonstrating vast application prospects of the oxychloride amorphous solid electrolytes.

Probing the direct effect of grain boundaries as active catalytic sites is very challenging. Here, the authors reveal that the d z 2 orbital energy level of Mo atoms in grain boundaries exhibits an intrinsic relationship with the hydrogen evolution activity.

Metallic zinc is an ideal anode material for aqueous rechargeable batteries but reversibility is a challenge. Here, the authors realise a dynamic real-time reconstructed interphase on zinc anode formed by graphitic carbon nitride quantum dot as an electrolyte additive to improve the performance of Zn metal anodes.

Abstract Electrochemical reduction of CO2 to formate is economically attractive but improving the reaction selectivity and activity remains challenging. Herein, we introduce boron (B) atoms to modify the local electronic structure of bismuth with positive valence sites for boosting conversion of CO2 into formate with high activity and selectivity in a wide potential window. By combining experimental and computational investigations, our study indicates that B dopant differentiates the proton participations of rate-determining steps in CO2 reduction and in the competing hydrogen evolution. By comparing the experimental observations with the density functional theory, the dominant mechanistic pathway of B promoted formate generation and the B concentration modulated effects on the catalytic property of Bi are unravelled. This comprehensive study offers deep mechanistic insights into the reaction pathway at an atomic and molecular level and provides an effective strategy for the rational design of highly active and selective electrocatalysts for efficient CO2 conversion.

Stable solid electrolyte interface (SEI) is heavily investigated due to its role in improving lithium metal batteries. Here, the authors present a new strategy by employing electrolyte additives to construct stable multifunctional SEI via in situ anionic polymerization.

The origin of Dzi beads, also called “tian zhu”, has always been a mystery. These beads come in a variety of patterns, shapes and sizes. They have cultural and heritage significance in Tibet and areas surrounding the Himalayas. The most recognized beads are those with the “eye” pattern. They are said to ward off evil spirits. Due to their reputation, the demand for Dzi beads has increased in Asia. Herein, we report a study of a Dzi bead with a three-eye pattern using X-ray diffraction (XRD), X-ray fluorescence (XRF), X-ray absorption near edge structure (XANES) and imaging techniques. This is a novel area for Dzi bead research using X-rays from a synchrotron light source to determine the chemical composition of the bead, if the pattern is natural or man-made or if the bead is genuine or a replica. These techniques revealed the bead to be composed of agate (silicon dioxide). An interesting feature on the bead’s surface was the etched rings, which were observed to contain regular copper hot spots on their circumference. Our results suggest that the Dzi bead was genuine and started out as an earth-formed agate, with the pattern crafted.

Tungsten carbide has yet to live up to its long-believed potential as a replacement for precious metal electrocatalysts. Here, Li and co-workers demonstrate that ditungsten carbide in the form of ultrasmall, phase-pure nanoparticles is a better candidate for the hydrogen evolution reaction.

Anthropogenic activities at the HudBay Minerals, Inc., Flin Flon (Manitoba, Canada) mining and processing facility have severely affected the surrounding boreal forest ecosystem. Soil contamination occurred via a combination of metal and sulfuric acid deposition and has resulted in forest dieback and ineffective natural recovery. A community-led effort to revegetate areas of the landscape through the application of a dolomitic limestone has been met with varied success. Zinc (Zn) speciation has shown to be closely linked to the presence or absence of an invasive metal-tolerant grass species, with soils being broadly classed into two revegetation response groups. Group I, characterized by the absence of metal-tolerant grasses, and group II, characterized by the presence of metal-tolerant grasses. The systematic approach used to lime areas of the landscape produced a liming chronosequence for each group. This study used a combination of X-ray absorption spectroscopy, X-ray fluorescence mapping, and X-ray diffraction techniques to determine the effect of liming on Zn speciation in these chronosequences. Liming group I soils resulted in the formation of a neo-phase Zn-Al-hydroxy interlayer coprecipitate and subsequent rapid boreal forest revegetation. The effect of liming on Zn speciation on the group II soils resulted in a gradual transition of increasingly stable adsorption species, culminating with a stable Zn-Al-layered double hydroxide precipitate. Boreal forest vegetation has failed to recolonize group II soils during the study. However, the formation of the layered double hydroxide species resulted in a significant reduction in CaCl2-extractable Zn. Further research is required to determine how to promote the revegetation of these soils. [ABSTRACT FROM AUTHOR]

HudBay Minerals, Inc., has mined and/or processed Zn and Cu ore in Flin Flon, MB, Canada, since the 1930s. The boreal forest ecosystem and soil surrounding these facilities have been severely impacted by mixed metal contamination and H2SO4 deposition. Zinc is one of the most prevalent smelter-derived contaminants and has been identified as a key factor that may be limiting revegetation. Metal toxicity is related to both total concentrations and speciation; therefore, X-ray absorption spectroscopy and X-ray fluorescence mapping were used to characterize Zn speciation in soils throughout the most heavily contaminated areas of the landscape. Zinc speciation was linked to two distinct soil types. Group I soils consist of exposed soils in weathered positions of bedrock outcrops with Zn present primarily as franklinite, a (ZnFe2O4) spinel mineral. Group II soils are stabilized by an invasive metal-tolerant grass species, with Zn found as a mixture of octahedral (Fe oxides) and tetrahedral Mn oxides) adsorption complexes with a franklinite component. Soil erosion influences Zn speciation through the redistribution of Zn and soil particulates from Group I landscape positions to Group II soils. Despite Group II soils having the highest concentrations of CaCl2-extractable Zn, they support metal-tolerant plant growth. The metal-tolerant plants are probably preferentially colonizing these areas due to better soil and nutrient conditions as a result of soil deposition from upslope Group I areas. Zinc concentration and speciation appears to not influence the colonization by metal-tolerant grasses, but the overall soil properties and erosion effects prevent the revegetation by native boreal forest species. [ABSTRACT FROM AUTHOR]

The bend magnet VESPERS beamline on the third generation CLS synchrotron has been equipped with capabilities for X-ray fluorescence (SXRF) excitation with micro-focussed white radiation, as well as with broad and narrow bandpass monochromatised radiation. Using the former two conditions, SXRF studies have been conducted on several reference materials and metals with known elemental concentrations. The resultant spectral line shapes have been analysed using newly developed software that facilitates ready identification of K, L and M lines present as well as their subsequent spatial mapping. Using both white and broad bandpass radiation, K lines for elements from magnesium to indium and L lines from hafnium to uranium were measured and sensitivity values (S) determined. White radiation provided much higher sensitivity for most elements, and a narrower range of Svalues makes it possible to use a single white radiation experiment to determine a wide range of elements in the periodic table. Additionally, the variances in Svalues for several low Z matrices were relatively low, thus making it possible to estimate elemental concentration ranges using a reference material. [ABSTRACT FROM AUTHOR]

Ionic photofragmentation of SO2 in the sulfur 2p and 2s regions has been investigated using monochromatic synchrotron radiation. Multi-stop time-of-flight mass spectrometry was used to collect photoelectron–photoion coincidence (PEPICO), photoion–photoion coincidence (PIPICO) and photoelectron–photoion–photoion coincidence (PEPIPICO) spectra simultaneously. Partial ion yields and partial ion-pair yields have been determined. Dissociation mechanisms of the productions of ion-pairs O+—S+ and O+—SO+ have been discussed briefly. [Copyright &y& Elsevier]

In this study, the thermomechanical characteristics of copper through-silicon via (Cu TSV) structures were studied using synchrotron x-ray microdiffraction, electron backscattered diffraction (EBSD), and nonlinear numerical modeling. The strain and stress distribution in the Si substrate was measured by synchrotron x-ray microdiffraction from the tops of the TSV structures. The strain distribution map in a Cu via was determined from EBSD data by the kernel average misorientation (KAM) method and microstructural characteristics of the Cu via were investigated. The results offered direct evaluation of the local strain and stress induced in the Cu via and its surrounding silicon substrate. A finite element model including nonlinear plastic deformation was built for predicting thermomechanical behaviors of Cu TSV structures. The results show that the stress distribution obtained by finite element modeling is in relatively good agreement with the measurements of synchrotron x-ray microdiffraction and EBSD. [ABSTRACT FROM AUTHOR]

Abstract The electrification of the transport sector has created an increasing demand for lithium‐ion batteries that can provide high power intermittently while maintaining a high energy density. Given the difficulty in designing a single redox material with both high power and energy density, electrodes based on composites of several electroactive materials optimized for power or capacity are being studied extensively. Among others, fast‐charging LiFePO4 and high energy Li(NixMnyCoz)O2 are commonly employed in industrial cell manufacturing. This study focuses on comparing different approaches to combining these two active materials into a single electrode. These arrangements were compared using standard electrochemical (dis)charge procedures and using synchrotron X‐ray fluorescence to identify variations in solution concentration gradient formation. The electrochemical performance of the layered electrodes with the high‐power material on top is found to be enhanced relative to its blended electrode counterpart when (dis)charged at the same specific currents. These findings highlight dual‐layer lithium‐ion batteries as an inexpensive way of increasing energy and power density of lithium‐ion batteries as well as a model system to study and exploit the synergistic effects of blended electrodes.

The article offers information on O-coordinated W-Mo dual-atom catalyst for pH-universal electrocatalytic hydrogen evolution. Topics discussed include use of Single-atom catalysts (SACs) for hydrogen evolution reaction (HER); deveopment of dual-atom catalyst (DAC) consisting of O-coordinated W-Mo heterodimer embedded in N-doped graphene; and use of electron delocalization of W─O─Mo─O─C configuration which provides optimal adsorption strength of hydrogen.