Due to its high energy density and low cost, Li-rich Mn-based layered oxides are considered potential cathode materials for next generation Li-ion batteries. However, they still suffer from serious obstacles of low initial Coulombic efficiency, which is detrimental to their practical application. Here, an efficient surface modification method via NH4H2PO4 assisted pyrolysis is performed to improve the Coulombic efficiency of Li1.2Mn0.54Ni0.13Co0.13O2, where appropriate oxygen vacancies, Li3PO4 and spinel phase are synchronously generated in the surface layer of LMR microspheres. Under the synergistic effect of the oxygen vacancies and spinel phase, the unavoidable oxygen release in the cycling process was effectively suppressed. Moreover, the induced Li3PO4 nanolayer could boost the lithium-ion diffusion and mitigate the dissolution of transition metal ions, especially manganese ions, in the material. The optimally modified sample yielded an impressive initial Coulombic efficiency and outstanding rate performance.

The production and degradation of polyesters are two crucial processes in polyester materials’life cycle. In this work, multi-functional organocatalysts based on fluorides for both processes are described. Organofluorides were developed as catalysts for ring-opening polymerization of lactide (lactone). Compared with a series of organohalides, organofluoride performed the best catalytic reactivity because of the hydrogen bond interaction between F– and alcohol initiator. The Mn values of polyester products could be up to 72 kg mol–1. With organofluoride catalysts, the ring-opening copolymerization between various anhydrides and epoxides could be established. Furthermore, terpolymerization of anhydride, epoxide, and lactide could be constructed by the self-switchable organofluoride catalyst to yield a block polymer with a strictly controlled polymerization sequence. Organofluorides were also efficient catalysts for upcycling polyester plastic wastes via alcoholysis. Mixed polyester materials could also be hierarchically recycled.

High-density polyethylene (HDPE) and isotactic polypropylene (iPP) are widely used in industrial and residential applications due to their low cost and chemical stability, thus their recycling process can contribute to a circular economy. However, both polymers are non-polar materials, and the incompatibility with most other materials leads to substantially inferior properties of blends. In this work, we propose a flexible compatibilization strategy to improve the compatibility of HDPE/iPP blends. Ozone was adopted to induce reactive extrusion for rapid oxidation of HDPE and chain-branching reactions for both HDPE and HDPE/iPP blends. During extrusion process, ozone oxidizes HDPE effectively in a short time and introduces oxygen-containing groups such as carbonyl and ester group, which improves the hydrophilicity. The addition of trimethylolpropane triacrylate (TMPTA) could promote branching reaction and facilitate the formation of HDPE-g-iPP copolymers, which improved the compatibility for HDPE/iPP. As a result, the impact strength of ozone-modified HDPE and HDPE/iPP blends increased by 22% and 82%, respectively, and the tensile strength also increased. This strategy would have potential applications in the field of sorting-free and solvent-free recycling of waste polyolefin plastics.

Recently, interest in converting bio-derived fatty acid methyl esters (FAMEs) into added-value products has significantly increased. The selectivity of ketonization reaction in the conversion of the FAMEs has significantly hampered the efficiency of this process. Herein, we prepared catalysts with different levels of oxygen vacancies while the crystal phase remained unchanged. The catalyst with the highest level of oxygen vacancy exhibited the maximum selectivity. The density functional theory (DFT) simulation showed an increase in interatomic distances leading to the formation of frustrated Lewis pairs (FLPs) upon the creation of oxygen vacancies. The surface measurements, type and density of acid sites of the catalysts, showed that the Lewis acid sites enhanced the selectivity for ketone production; while Bronsted acid sites increased the formation of by-products. Moreover, the ketone formation rate was directly proportional to acid density. The findings of this research provide a different approach for catalyst design, based on defects engineering and their effect on the surface activity, which could be used for enhancing the catalytic performance of novel metal oxides.

Using their own triazine groups as natural receptors, the introduction of various donor units to construct donor-receptor configuration in covalent triazine frameworks (CTFs) has been shown to be an effective strategy to improve photocatalytic activity. In this work, the effect of donor unit content (D-content) on the photoelectric properties and photocatalytic activity of CTFs was thoroughly investigated. Four analogous CTFs with different D-content have been rationally designed and synthesized, in which the bithiophene (Btp) as the donor unit and triazine as the acceptor unit. And CTF-Btp with the highest D-content showed the best photocatalytic activity. The experimental and theoretical results indicated this improvement is attributed to stronger visible light absorption capacity and higher photoinduced charge carrier separation efficiency. This study elucidates the relationship between the structural features of CTFs with varying D-content and their photocatalytic activity, offering a promising strategy for developing efficient photocatalysts.

With their high volumetric capacity and electronic conductivity, sodium-selenium (Na-Se) batteries have attracted attention for advanced battery systems. However, the irreversible deposition of sodium selenide (Na2Se) results in rapid capacity degradation and poor Coulombic efficiency. To address these issues, cubic α-Mn2O3 is introduced herein as an electrocatalyst to effectively catalyze Na2Se conversion and improve the utilization of active materials. The results show that the addition of 10 wt% Mn2O3 in the Se/KB composite enhances the conversion from Na2Se to Se by lowering activation energy barrier and leads to fast sodium-ion kinetics and low internal resistance. Consequently, the Mn2O3-based composite delivers a high specific capacity of 635 mAh·g-1 at 675 mA·g-1 after 250 cycles as well as excellent cycling stability for 800 cycles with a high specific capacity of 317 mAh·g-1 even at the high current density of 3375 mA·g-1. Due to the cubic Mn2O3 electrocatalyst, the performance of the composites is mostly superior to existing state-of-the-art Na-Se batteries reported in the literature.

In recent years, there is growing interest in solid-state electrolytes due to their many promising properties, making them key to the future of battery technology. This future depends among other things on easy processing technologies for the solid electrolyte. The sodium superionic conductor (NASICON) Na3Zr2Si2PO12 is a promising sodium solid electrolyte; however, reported methods of synthesis are time and energy consuming. To this effect, attempt was made to develop a simple time efficient alternative processing route. Firstly, a comparative study between a new method and commonly reported methods was carried out to gain a clear insight into the mechanism of formation of sodium superionic conductors (NASICON). It was observed that through a careful selection of precursors, and the use of high-energy milling (HEM) the NASICON conversion process was enhanced and optimized, this reduces the processing time and required energy, and opens up a new alternative route for synthesis. The obtained solid electrolyte was stable during Na cycling vs. Na-metal at 1mA/cm2, and a room temperature conductivity of 1.8 mS/cm was attained.

Carbohydrazide electrooxidation reaction (COR) is a potential alternative to oxygen evolution reaction in water splitting process. However, the sluggish kinetics process impels to develop efficient catalysts with the aim of the widespread use of such catalytic system. Since COR concerns the adsorption/desorption of reactive species on catalysts, the electronic structure of electrocatalyst can affect the catalytic activity. Interface charge distribution engineering can be considered to be an efficient strategy for improving catalytic performance, which facilitates the cleavage of chemical bond. Herein, highly dispersed Pd nanoparticles on CeO2/C catalyst are prepared and the COR catalytic performance is investigated. The self-driven charge transfer between Pd and CeO2 can form the local nucleophilic and electrophilic region, promoting to the adsorption of electron-withdrawing and electron-donating group in carbohydrazide molecule, which facilitates the cleavage of C-N bond and the carbohydrazide oxidation. Due to the local charge distribution, the Pd-CeO2/C exhibits superior COR catalytic activity with a potential of 0.27 V to attain 10 mA cm-2. When this catalyst is used for energy-efficient electrolytic hydrogen production, the carbohydrazide electrolysis configuration exhibits a low cell voltage (0.6 V at 10 mA cm-2). This interface charge distribution engineering can provide a novel strategy for improving COR catalytic activity.

The practical implementation of the lithium metal anode (LMA) has long been pursued due to its extremely high specific capacity and low electrochemical equilibrium potential. However, the unstable interfaces resulting from lithium ultrahigh reactivity have significantly hindered the use of LMA. This instability directly leads to dendrite growth behavior, dead lithium, low Coulombic efficiency, and even safety concerns. Therefore, artificial solid electrolyte interfaces (ASEI) with enhanced physicochemical and electrochemistry properties have been explored to stabilize LMA. Polymer materials, with their flexible structures and multiple functional groups, offer a promising way for structurally designing ASEIs to address the challenges faced by LMA. This Concept demonstrates an overview of polymer ASEIs with different functionalities, such as providing uniform lithium ion and single-ion transportation, inhibiting side reactions, possessing self-healing ability, and improving air stability. Furthermore, challenges and prospects for the future application of polymeric ASEIs in commercial lithium metal batteries (LMBs) are also discussed.

Making ammonia: How and where? Novel biological and electrochemical pathways require further large improvements to compete with Haber-Bosch. While their production flexibility improves the economics of on-farm synthesis, other drivers will encourage centralized green ammonia production.

Abstract

Prospects of recent promising methods of producing ammonia without fossil fuels are discussed. Despite demonstrating efficiency gains over previous similar approaches, the novel biological and electrochemical pathways require further large improvements to compete with electricity-powered Haber-Bosch. As some literature asserts that future production will shift to smaller scales, such as on-farm, we qualitatively discuss the economics of scale of future green ammonia production.