Cycling a Lithium Metal Anode at 90 °C in a Liquid Electrolyte

Stable operation at elevated temperature is necessary for lithium metal anode. However, Li metal anode generally has poor performance and safety concerns at high temperature (>55 °C) owing to the thermal instability of the electrolyte and solid electrolyte interphase in a routine liquid electrolyte. Herein a Li metal anode working at an elevated temperature (90 °C) is demonstrated in a thermotolerant electrolyte. In a Li|LiFePO₄ battery working at 90 °C, the anode undergoes 100 cycles compared with 10 cycles in a practical carbonate electrolyte. During the formation of the solid electrolyte interphase, independent and incomplete decomposition of Li salts and solvents aggravate. Some unstable intermediates emerge at 90 °C, degenerating the uniformity of Li deposition. This work not only demonstrates a working Li metal anode at 90 °C, but also provides fundamental understanding of solid electrolyte interphase and Li deposition at elevated temperature for rechargeable batteries.     

Air‐Stable Oxyallyl Patterns and a Switchable N‐Heterocyclic Carbene

Oxyallyl derivatives are typically elusive compounds. Even recently reported “stabilized” 1,3‐diaminooxyallyl species are still highly reactive and have short lifetimes at room temperature. Herein, we report the synthesis and preliminary study of mesoionic pyrimidine derivatives that feature 1,3‐bis(dimethylamino)oxyallyl patterns with an unprecedented level of stabilization. The latter are not only insensitive towards air and moisture, but they are also compatible with the formation of an ancillary stable N‐heterocyclic carbene moiety. As the oxyallyl pattern is proton‐responsive, it allows the reversible switching of the electronic properties of the carbene, as a ligand.     

Lead Mixed Oxyhalides Satisfying All Fundamental Requirements for High‐Performance Mid‐Infrared Nonlinear Optical Materials

To design high‐performance mid‐infrared (mid‐IR) nonlinear optical (NLO) materials, we have focused on the combination of a heavy metal lone pair cation, Pb²⁺ and mixed oxyhalides. A systematic investigation in PbO‐PbCl₂‐PbBr₂ system led us to discover the first examples of NLO lead mixed oxyhalides, namely, Pb₁₃O₆Cl₄Br₁₀, Pb₁₃O₆Cl₇Br₇, and Pb₁₃O₆Cl₉Br₅. All the reported materials have remarkably comprehensive properties including broad IR transparency (up to 14.0 μm), qualified second harmonic generation (SHG) responses (0.6–0.9×AgGaS₂), wide band gaps (3.05–3.21 eV), and ease of crystal growth. Interestingly, a centimeter‐sized single crystal (2.9×1.3×0.5 cm³) of Pb₁₃O₆Cl₉Br₅ revealing a wide transparent range (0.384–14.0 μm) and high laser damage threshold (LDT) (14.6×AgGaS₂) has been successfully grown in an open system. The study suggests that all the reported mixed oxyhalides are outstanding candidates for mid‐IR NLO materials.     

Solvent‐Free Self‐Assembly for Scalable Preparation of Highly Crystalline Mesoporous Metal Oxides

Mesoporous metal oxides (MMOs) have been demonstrated great potential in various applications. Up to now, the direct synthesis of MMOs is still limited to the solvent induced inorganic‐organic self‐assembly process. Here, we develop a facile, general, and high throughput solvent‐free self‐assembly strategy to synthesize a series of MMOs including single‐component MMOs and multi‐component MMOs (e.g., doped MMOs, composite MMOs, and polymetallic oxide) with high crystallinity and remarkable porous properties by grinding and heating raw materials. Compared with the traditional solution self‐assembly process, the avoidance of solvents in this method not only greatly increases the yield of target products and synthesis efficiency, but also reduces the environmental pollution and the consumption of cost and energy. We believe the presented approach will pave a new avenue for scalable production of advanced mesoporous materials for various applications.     

A Highly Efficient All‐Solid‐State Lithium/Electrolyte Interface Induced by an Energetic Reaction

The energetic chemical reaction between Zn(NO₃)₂ and Li is used to create a solid‐state interface between Li metal and Li_6.4La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) electrolyte. This interlayer, composed of Zn, ZnLi_x alloy, Li₃N, Li₂O, and other species, possesses strong affinities with both Li metal and LLZTO and affords highly efficient conductive pathways for Li⁺ transport through the interface. The unique structure and properties of the interlayer lead to Li metal anodes with longer cycle life, higher efficiency, and better safety compared to the current best Li metal electrodes operating in liquid electrolytes while retaining comparable capacity, rate, and overpotential. All‐solid‐state Li||Li cells can operate at very demanding current–capacity conditions of 4 mA cm^?2–8 mAh cm^?2. Thousands of hours of continuous cycling are achieved at Coulombic efficiency >99.5 % without dendrite formation or side reactions with the electrolyte.     

In Situ Dispersion of Palladium on TiO2 During Reverse Water–Gas Shift Reaction: Formation of Atomically Dispersed Palladium

The application of single‐atom catalysts (SACs) to high‐temperature hydrogenation requires materials that thermodynamically favor metal atom isolation over cluster formation. We demonstrate that Pd can be predominantly dispersed as isolated atoms onto TiO₂ during the reverse water–gas shift (rWGS) reaction at 400 °C. Achieving atomic dispersion requires an artificial increase of the absolute TiO₂ surface area by an order of magnitude and can be accomplished by physically mixing a precatalyst (Pd/TiO₂) with neat TiO₂ prior to the rWGS reaction. The in situ dispersion of Pd was reflected through a continuous increase of rWGS activity over 92 h and supported by kinetic analysis, infrared and X‐ray absorption spectroscopies and scanning transmission electron microscopy. The thermodynamic stability of Pd under high‐temperature rWGS conditions is associated with Pd‐Ti coordination, which manifests upon O‐vacancy formation, and the artificial increase in TiO₂ surface area.     

Identifying the Types and Characterization of the Active Sites on M−X−C Single-Atom Catalysts

Single atom catalysts (SACs) have attracted much attention in recent years. As an essential group in SACs, M−X−C (X=nonmetallic element) materials have been demonstrated to be efficient in many reactions. However, identifying the active sites on M−X−C, especially under working conditions, is still challenging, which is crucial for chemists to further understand the mechanism underlying the reaction and better design proper SACs for specific reactions. Herein, the types and characterization of M−X−C are comprehensively summarized and discussed in this review. In addition to the basic information above, the challenges and opportunities remaining in this field will be also proposed to present a perspective to the research on the next step.     

Chromatographic separation simulation of metal‐chelating peptides from surface plasmon resonance binding parameters

Some metal‐chelating peptides have antioxidant properties, with potential nutrition, health, and cosmetics applications. This study aimed to simulate their separation on immobilized metal ion affinity chromatography from their affinity constant for immobilized metal ion determined in surface plasmon resonance, both technics are based on peptide‐metal ion interactions. In our approach, first, the affinity constant of synthetic peptides was determined by surface plasmon resonance and used as input data to numerically simulate the chromatographic separation with a transport‐dispersive model based on Langmuir adsorption isotherm. Then, chromatographic separation was applied on the same peptides to determine their retention time and compare this experimental t_R with the simulated t_R obtained from simulation from surface plasmon resonance data. For the investigated peptides, the relative values of t_R were comparable. Hence, our study demonstrated the pertinence of such numerical simulation correlating immobilized metal ion affinity chromatography and surface plasmon resonance.     

Photocatalysis: an overview of recent developments and technological advancements

Photocatalysis,which is the catalyzation of redox reactions via the use of energy obtained from light sources,is a topic that has garnered a lot of attention in recent years as a means of addressing the environmental and economic issues plaguing society today.Of particular interest are photosynthesis can potentially mimic a variety of vital reactions,many of which hold the key to develop sustainable energy economy.In light of this,many of the technological and procedural advancements that have recently occurred in the field are discussed in this review,namely those linked to:(1)photocatalysts made from metal oxides,nitride,and sulfides;(2)photocatalysis via polymeric carbon nitride(PCN);and(3)general advances and mechanistic insights related to TiO2-based catalysts.The challenges and opportunities that have arisen over the past few years are discussed in detail.Basic concepts and experimental procedures which could be useful for eventually overcoming the problems associated with photocatalysis are presented herein.