Optimization Design of Fluoro-Cyanogen Copolymer Electrolyte to Achieve 4.7 V High-Voltage Solid Lithium Metal Battery.

Raising the charging voltage and employing high-capacity cathodes like lithium cobalt oxide (LCO) are efficient strategies to expand battery capacity. High voltage, however, will reveal major issues such as the electrolyte's low interface stability and weak electrochemical stability. Designing high-performance solid electrolytes from the standpoint of substance genetic engineering design is consequently vital. In this instance, stable SEI and CEI interface layers are constructed, and a 4.7 V high-voltage solid copolymer electrolyte (PAFP) with a fluoro-cyanogen group is generated by polymer molecular engineering. As a result, PAFP has an exceptionally broad electrochemical window (5.5 V), a high Li+ transference number (0.71), and an ultrahigh ionic conductivity (1.2 mS cm-2) at 25 °C. Furthermore, the Li||Li symmetric cell possesses excellent interface stability and 2000 stable cycles at 1 mA cm-2. The LCO|PAFP|Li batteries have a 73.7% retention capacity after 1200 cycles. Moreover, it still has excellent cycling stability at a high charging voltage of 4.7 V. These characteristics above also allow PAFP to run stably at high loading, showing excellent electrochemical stability. Furthermore, the proposed PAFP provides new insights into high-voltage resistant solid polymer electrolytes.

Exploring the lipid oxidation mechanisms during pumpkin seed kernels storage based on lipidomics: From phenomena, substances, and metabolic mechanisms.

The study investigated the lipid oxidation of pumpkin seed kernels (PSK) under different storage conditions (room temperature, vacuum-room temperature, refrigeration, and vacuum-refrigeration) using HPLC-MS and GC-MS. Experimental results found the vacuum-refrigeration group showed the lowest PV (0.24 g/100 g), diene (8.68), hexanal (356.64 ± 16.06 ng/g), and nonanal (132.05 ± 8.38 ng/g) after a 9-month storage. A total of 586 lipids, including 6 classes and 27 subclasses, were detected, 46 of which showed significant differences. Refrigeration samples had the highest diacylglycerol content, while room temperature samples demonstrated the highest triacylglycerol and phosphatidylcholine content. Differential lipid metabolite analyses indicated that storage conditions mainly affected glycerolipid metabolism, glycerophospholipid metabolism, and sphingolipid metabolism pathways in PSK, while glycerolipid and glycerophospholipid metabolism were still dominant. It revealed that refrigeration was more effective than vacuum in inhibiting the oxidation of PSK. These findings could offer valuable references for the storage, transportation, preservation, and the development and utilization of PSK.

Designing dynamic coordination bonds in polar hybrid crystals for a high-temperature ferroelastic transition.

Ferroelastic materials have gained widespread attention as promising candidates for mechanical switches, shape memory, and information processing. Their phase-transition mechanisms usually originate from conventional order-disorder and/or displacive types, while those involving dynamic coordination bonds are still scarce. Herein, based on a strategic molecular design of organic cations, we report three new polar hybrid crystals with a generic formula of AA'RbBiCl6 (A = A' = Me3SO+ for 1; A = Me3SO+ and A' = Me4N+ for 2; A = A' = Me3NNH2+ for 3). Their A-site cations link to the [RbBiCl6]n2n- inorganic framework with lon topology through Rb-O/N coordination bonds, while their significantly different interactions between A'-site cations and inorganic frameworks provide distinct phase-transition behaviour. In detail, the strongly coordinative A'-site Me3SO+ cations prevent 1 from a structural phase transition, while coordinatively free A'-site Me4N+ cations trigger a conventional order-disorder ferroelastic transition at 247 K in 2, accompanied by a latent heat of 0.63 J g-1 and a usual "high → low" second-harmonic-generation (SHG) switch. Interestingly, the A'-site Me3NNH2+ cations in 3 reveal unusual dynamic coordination bonds, driving a high-temperature ferroelastic transition at 369 K with a large latent heat of 18.34 J g-1 and an unusual "low → high" SHG-switching behaviour. This work provides an effective molecular assembly strategy to establish dynamic coordination bonds in a new type of host-guest model and opens an avenue for designing advanced ferroelastic multifunctional materials.

A Novel Framed Slotted Aloha Medium Access Control Protocol Based on Capture Effect in Vehicular Ad Hoc Networks.

The capture effect is a frequently observed phenomenon in vehicular ad hoc networks (VANETs) communication. When conflicts arise during time slot access, failure to access does not necessarily occur; instead, successful access may still be achieved. The capture effect can enhance the likelihood of multiple access and improve communication efficiency. The security of VANETs communication is undoubtedly the primary concern. One crucial approach to enhance security involves the design of an efficient and reliable medium access control (MAC) protocol. Taking into account both aspects, we propose a novel framed slotted Aloha (FSA) MAC protocol model. Firstly, we derive the closed-form expression for the capture probability in the Rician fading channel in this paper. Subsequently, we analyze how the number of vehicles and time slots influence the success probability of vehicle access channels as well as examine the impact of the capture effect on this success probability. Then, under constraints regarding vehicle access channel success probability, we derive optimal values for slot numbers, access times, and transmission power while proposing a comprehensive implementation method to ensure high access channel success probabilities. We verify both theoretical derivations and proposed methods through simulation experiments.

Exploring the oxidative rancidity mechanism and changes in volatile flavors of watermelon seed kernels based on lipidomics.

Watermelon seed kernels (WSK) are prone to oxidative rancidity, while their evaluation biomarkers and changes in volatile flavor are still unknown. The research tracked the changes in volatile compounds and lipid components before and after rancidity using HS-SPME-GC-O-MS and lipidomic techniques. The results showed the flavor of watermelon seed kernels changed significantly before and after rancidity, from mild aroma to rancidity. A total of 42 volatile compounds were detected via GC-O-MS, and a total of 220 lipid molecules were detected via lipidomic technology. 55 lipids with significant differences were screened via multivariate statistical analysis. Combining the above analysis, it found that glycerol phospholipid and glyceride pathways were the most important metabolic pathways and 1-Pentanol and styrene could be used as potential biomarkers to judge the rancidity process of watermelon seed kernels. The research could provide powerful technical support for the storage, transportation and freshness preservation of watermelon seed kernels.

ZIFs-Derived Hollow Nanostructures via a Strong/Weak Coetching Strategy for Long-Life Rechargeable Zn-Air Batteries.

Recently, zeolitic imidazolate frameworks (ZIFs) composites have emerged as promising precursors for synthesizing hollow-structured N-doped carbon-based noble-metal materials with diverse structures and compositions. Here, a strong/weak competitive coordination strategy is presented for synthesizing high-performance electrocatalysts with hollow features. During the competitive coordination process, the cubic zeolitic-imidazole framework-8 (Cube-8)@ZIF-67 with core-shell structures are transformed into Cube-8@ZIF-67@PF/POM with yolk-shell nanostructures employing phosphomolybdic acid (POM) and potassium ferricyanide (PF) as the strong chelator and the weak chelator, respectively. After calcination, the hollow Mo/Fe/Co@NC catalyst exhibits superior performance in both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Interestingly, the Mo/Fe/Co@NC catalyst exhibits efficient electrocatalytic performance for Zn-air batteries (ZABs), with a high power density (≈150 mW cm-2 ) and superior cycling life (≈500 h) compared to commercial platinum/carbon (Pt/C) and ruthenium dioxide (RuO2 ) mixture benchmarks catalysts. In addition, the density functional theory further proves that after the introduction of Mo and Fe atoms, the adsorption energy with the adsorption intermediates is weakened by adjusting the d-band center, thus weakening the reaction barrier and promoting the reaction kinetics of OER. Undoubtedly, this study presents novel insights into the fabrication of ZIFs-derived hollow structure bifunctional oxygen electrocatalysts for clean-energy diverse applications.

Low-cost flexible textile electrocatalyst for overall water splitting.

Through the braidability of cotton fiber and the richness of surface functional groups, cotton fiber can be woven into any shape, and catalytically active centers can be stably anchored on the fibers. During the electrocatalytic overall water splitting (OWS) process, catalyst shedding and activity reduction can be effectively avoided.

Characterization and genomic analysis of a novel bacteriophage BUCT_49532 lysing Klebsiella pneumoniae.

Bacteriophages are a type of virus widely distributed in nature that demonstrates a remarkable aptitude for selectively recognizing and infecting bacteria. In particular, Klebsiella pneumoniae is acknowledged as a clinical pathogen responsible for nosocomial infections and frequently develops multidrug resistance. Considering the increasing prevalence of antibiotic-resistant bacteria, bacteriophages have emerged as a compelling alternative therapeutic approach. In this study, a novel phage named BUCT_49532 was isolated from sewage using K. pneumoniae K1119 as the host. Electron microscopy revealed that BUCT_49532 belongs to the Caudoviricetes class. Further analysis through whole genome sequencing demonstrated that BUCT_49532 is a Jedunavirus comprised of linear double-stranded DNA with a length of 49,532 bp. Comparative genomics analysis based on average nucleotide identity (ANI) values revealed that BUCT_49532 should be identified as a novel species. Characterized by a good safety profile, high environmental stability, and strong lytic performance, phage BUCT_49532 presents an interesting case for consideration. Although its host range is relatively narrow, its application potential can be expanded by utilizing phage cocktails, making it a promising candidate for biocontrol approaches.

A hybrid double perovskite ferroelastic exhibiting the highest number of orientation states.

Integrating NH4+ as a B'-site ion within a three-dimensional double hybrid perovskite resulted in a novel high-temperature ferroelastic, (Me3NOH)2(NH4)[Co(CN)6], which uniquely demonstrates a reversible triclinic-to-cubic phase transition at 369 K and offers a record-setting 24 orientation states, the highest ever reported among all ferroelastics.

Capture-Aware Dense Tag Identification Using RFID Systems in Vehicular Networks.

Passive radio-frequency identification (RFID) systems have been widely applied in different fields, including vehicle access control, industrial production, and logistics tracking, due to their ability to improve work quality and management efficiency at a low cost. However, in an intersection situation where tags are densely distributed with vehicle gathering, the wireless channel becomes extremely complex, and the readers on the roadside may only decode the information from the strongest tag due to the capture effect, resulting in tag misses and considerably reducing the performance of tag identification. Therefore, it is crucial to design an efficient and reliable tag-identification algorithm in order to obtain information from vehicle and cargo tags under adverse traffic conditions, ensuring the successful application of RFID technology. In this paper, we first establish a Nakagami-m distributed channel capture model for RFID systems and provide an expression for the capture probability, where each channel is modeled as any relevant Nakagami-m distribution. Secondly, an advanced capture-aware tag-estimation scheme is proposed. Finally, extensive Monte Carlo simulations show that the proposed algorithm has strong adaptability to circumstances for capturing under-fading channels and outperforms the existing algorithms in terms of complexity and reliability of tag identification.

Hybrid Crosslinked Solid Polymer Electrolyte via In-Situ Solidification Enables High-Performance Solid-State Lithium Metal Batteries.

Solid-state lithium-metal batteries constructed by in-situ solidification of cyclic ether are considered to be a critical strategy for the next generation of solid-state batteries with high energy density and safety. However, the poor thermal/electrochemical stability of linear polyethers and severe interfacial reactions limit its further development. Herein, in-situ ring-opening hybrid crosslinked polymerization is proposed for organic/inorganic hybrid polymer electrolyte (HCPE) with superior ionic conductivity of 2.22 × 10-3 S cm-1 at 30 °C, ultrahigh Li+ transference number of 0.88, and wide electrochemical stability window of 5.2 V. These allow highly stable lithium stripping/plating cycling for over 1000 h at 1 mA cm-2 , which also reveal a well-defined interfacial stabilization mechanism. Thus, HCPE endows assembled solid-state lithium-metal batteries with excellent long-cycle performance over 600 cycles at 2 C (25 °C) and superior capacity retention of 92.1%. More importantly, the proposed noncombustible HCPE opens up a new frontier to promote the practical application of high safety and high energy density solid-state batteries via in-situ solidification.

Molecular Design of a Metal-Nitrosyl Ferroelectric with Reversible Photoisomerization.

The development of photo-responsive ferroelectrics whose polarization may be remotely controlled by optical means is of fundamental importance for basic research and technological applications. Herein, we report the design and synthesis of a new metal-nitrosyl ferroelectric crystal (DMA)(PIP)[Fe(CN)5(NO)] (1) (DMA = dimethylammonium, PIP = piperidinium) with potential phototunable polarization via a dual-organic-cation molecular design strategy. Compared to the parent non-ferroelectric (MA)2[Fe(CN)5(NO)] (MA = methylammonium) material with a phase transition at 207 K, the introduction of larger dual organic cations both lowers the crystal symmetry affording robust ferroelectricity and increases the energy barrier of molecular motions, endowing 1 with a large polarization of up to 7.6 µC cm-2 and a high Curie temperature (Tc) of 316 K. Infrared spectroscopy shows that the reversible photoisomerization of the nitrosyl ligand is accomplished by light irradiation. Specifically, the ground state with the N-bound nitrosyl ligand conformation can be reversibly switched to both the metastable state I (MSI) with isonitrosyl conformation and the metastable state II (MSII) with side-on nitrosyl conformation. Quantum chemistry calculations suggest that the photoisomerization significantly changes the dipole moment of the [Fe(CN)5(NO)]2- anion, thus leading to three ferroelectric states with different values of macroscopic polarization. Such optical accessibility and controllability of different ferroelectric states via photoinduced nitrosyl linkage isomerization open up a new and attractive route to optically controllable macroscopic polarization.

Low-Cost, High-Strength Cellulose-based Quasi-Solid Polymer Electrolyte for Solid-State Lithium-Metal Batteries.

Solid-state lithium-metal batteries are considered as the next generation of high-energy-density batteries. However, their solid electrolytes suffer from low ionic conductivity, poor interface performance, and high production costs, restricting their commercial application. Herein, a low-cost cellulose acetate-based quasi-solid composite polymer electrolyte (C-CLA QPE) was developed with a high Li+ transference number ( t L i + ${{t}_{{{\rm L}{\rm i}}^{+}}}$ ) of 0.85 and excellent interface stability. The prepared LiFePO4 (LFP)|C-CLA QPE|Li batteries exhibited excellent cycle performance with a capacity retention of 97.7 % after 1200 cycles at 1 C and 25 °C. The experimental results and Density Function Theory (DFT) simulation revealed that the partially esterified side groups in the CLA matrix contribute to the migration of Li+ and enhance electrochemical stability. This work provides a promising strategy for fabricating cost-effective, stable polymer electrolytes for solid-state lithium batteries.

Efficient microwave-assisted mineralization of oxytetracycline driven by persulfate and hypochlorite over Cu-biochar catalyst.

Microwave (MW)-assisted catalytic degradation of organic pollutants draws increasing attention owing to its high efficiency in wastewater treatment. This work developed Cu-loaded biochar (CuBC) catalysts for time-efficient mineralization of refractory and high-concentration oxytetracycline (OTC). With only 1 min at 80 °C, Na2S2O8 achieved 100% total organic carbon (TOC) removal over the Cu5BC, while NaClO mineralized 73.3% TOC over the metal-free BC, in contrast to a relatively low mineralization efficiency (< 35%) achieved by H2O2. The high efficiency in MW-assisted oxidation systems could be ascribed to reactive oxidizing species (•SO4- or •ClO), which otherwise were barely detectable in a conventional heating system. The interactions between CuBC and MW were revealed by correlating the physiochemical characteristics to the MW absorption ability. The proposed catalytic systems can contribute to the development of a high-throughput and low-carbon wastewater treatment technology.

Adsorption-reduction coupling mechanism and reductive species during efficient florfenicol removal by modified biochar supported sulfidized nanoscale zerovalent iron.

Sulfidized nanoscale zerovalent iron (S-nZVI) was a promising material for degrading halogenated contaminants, but the easy aggregation limits its application for in-situ groundwater remediation. Hence, S-nZVI was decorated onto modified biochar (mBC) to obtain better dispersity and reactivity with florfenicol (FF), a widely used antibiotic. Uniform dispersion of S-nZVI particles were achieved on the mBC with plentiful oxygen-containing functional groups and negative surface charge. Thus, the removal rate of FF by S-nZVI@mBC was 2.5 and 3.1 times higher than that by S-nZVI and S-nZVI@BC, respectively. Adsorption and dechlorination of FF showed synergistic effect under appropriate mBC addition (e.g., C/Fe mass ratio = 1:3, 1:1), probably due to the enrichment of FF facilitates its reduction. In contrast, the contact between FF and S-nZVI could be hindered under more mBC addition, significantly decrease the reduction rate of FF and the reduction capacity of per unit Fe0. In addition, sulfur dose altered the surface species of surface Fe and S, and removal rates of FF correlated well with surface reductive species, i.e., FeS (r = 0.90, p < 0.05) and Fe0 (r = 0.98, p < 0.01). These mechanistic insights indicate the importance of rational design for biochar supported S-nZVI, which can lead to more efficient FF degradation.

Could sulfidation enhance the long-term performance of nano-zero valent iron in the peroxymonosulfate activation to degrade 2-chlorobiphenyl?

Sulfidation can enhance the hydrophobicity of nano-zero valent iron (nZVI) and improve its long-term degradation performance in reduction technology. However, whether sulfidation can enhance its long-term performance in sulfate radical-based advanced oxidation processes hasn't been systematically studied. Herein sulfide-modified nZVI (S-nZVI) was prepared by different sulfidation methods and S/Fe ratios. The behavior of S-nZVI on the peroxymonosulfatec (PMS) activation to degrade 2-chlorobiphenyl for continuous 5 rounds was investigated. The results showed that sulfidation couldn't always promote the long-term degradation performance. S-nZVI prepared by one-step sulfidation method with high S/Fe ratio (S-nZVIonestep-7%, S-nZVIonestep-14%) exhibited inferior degradation performance than unmodified nZVI (52.2%). This was because that the electron donor Fe0 was consumed rapidly and the crystalline lepidocrocite accumulated on the surface, thus inhibited PMS activation. In contrast, S-nZVI prepared by post-sulfidation method with high S/Fe ratio (S-nZVIpost-7%, S-nZVIpost-14%) exhibited more Fe0 residual, less FeOx accumulation, and more catalytic Fe2+ regeneration. Consequently, S-nZVIpost exhibited superior degradation capacity (69.3%). Moreover, the radical quenching experiments revealed that the primary free radicals involved in the degradation were transformed from SO4•- to •OH with prolongation of the degradation. Additionally, Fe (IV) contributed to the degradation through non-radical mechanism, especially in the S-nZVIpost-7%/PMS system.

Improving kitchen waste composting maturity by optimizing the processing parameters based on machine learning model.

As a novel analytical method based on big data, machine learning model can explore the relationship between different parameters and draw universal conclusions, which was used to predict composting maturity and identify key parameters in this study. The results showed that the Stacking model exhibited excellent prediction accuracy. SHapley Additive exPlanations (SHAP) and Partial Dependence Analysis (PDA) were performed to evaluate the importance of different parameters as well as their optimal interval. Optimal starting conditions should be maintained in the mesophilic state (temperature: 30-45℃, moisture content: 55-65%, pH: 6.3-8.0), and nutrients (total nitrogen > 2.3%, total organic carbon > 35%) should be adjusted in the thermophilic state. Experiments revealed that model-based optimization strategies could improve composting maturity because they could optimize compost microbial flora and perform complex carbon cycle functions. In conclusion, this study provides new insights into the enhancement of the composting process.

Controlled release of silibinin in GelMA hydrogels inhibits inflammation by inducing M2-type macrophage polarization and promotes vascularization in vitro.

A dry socket is one of the most common complications after tooth extraction. The main etiologies are the loss of blood clots in the socket and the inflammation reaction caused by infection. Current studies on how to prevent dry sockets could not solve these two etiologies at the same time. Recent studies have demonstrated the anti-inflammation role of silibinin. In this study, silibinin was engineered into GelMA hydrogels (Sil-GelMA) with a concentration of 30 mM. The surface characteristics were observed by scanning electron microscopy and the successful loading of silibinin was detected by FTIR spectrometry. The Sil-GelMA hydrogels presented the sustained release ability of silibinin and slow degradation performance of GelMA. Furthermore, silibinin inhibited the inflammatory reaction by inducing M2-type macrophage polarization, promoting the secretion of anti-inflammatory factors (CD206, IL-10) and inhibiting the secretion of anti-inflammatory factors (IL-1ß, iNOS). Silibinin also increased the secretion of vascularization-related factor VEGF and promoted vascularization in vitro. This study suggested that the Sil-GelMA hydrogels not only had an anti-inflammatory effect, but also had the potential to promote vascularization. Based on these results, the Sil-GelMA hydrogels might provide a promising prospect for prevention of dry sockets in the future.

Neglected resistance risks: Cooperative resistance of antibiotic resistant bacteria influenced by primary soil components.

Various antibiotic resistant bacteria (ARB) can thrive in soil and resist such environmental pressures as antibiotics through cooperative resistance, thereby promoting ARB retention and antibiotic resistance genes transmission. However, there has been finite knowledge in regard to the mechanisms and potential ecological risks of cooperative resistance in soil microbiome. In this study, soil minerals and organic matters were designed to treat a mixture of two Escherichia coli strains with different antibiotic resistance (E. coli DH5α/pUC19 and E. coli XL2-Blue) to determine how soil components affected cooperative resistance, and Luria-Bertani plates containing two antibiotics were used to observe dual-drug resistant bacteria (DRB) developed via cooperative resistance. Results showed quartz, humic acid, and biochar promoted E. coli XL2-Blue with high fitness costs, whereas kaolin, montmorillonite, and soot inhibited both strains. Using fluorescence microscope and PCR, it was speculated DRB could resist the antibiotic pressure via E. coli XL2-Blue coating E. coli DH5α/pUC19. E. coli DH5α/pUC19 dominated cooperative resistance. Correlation analysis and scanning electron microscope images indicated soil components influenced cooperative resistance. Biochar promoted cooperative resistance by increasing intracellular reactive oxygen species, thereby reducing the dominant strain concentration required for DRB development. Kaolin inhibited cooperative resistance the most, followed by soot and montmorillonite.

Exploiting Molecular Dynamics in Composite Coatings to Design Robust Super-Repellent Surfaces.

Fluorinated motifs are promising for the engineering of repellent coatings, however, a fundamental understanding of how to effectively bind these motifs to various substrates is required to improve their stability in different use scenarios. Herein, the binding of fluorinated polyhedral oligomeric silsesquioxanes (POSS) using a cyanoacrylate glue (binder) is computationally and experimentally evaluated. The composite POSS-binder coatings display ultralow surface energy (≈10 mJ m-2 ), while still having large surface adhesions to substrates (300-400 nN), highlighting that super-repellent coatings (contact angles >150°) can be readily generated with this composite approach. Importantly, the coatings show super-repellency to both corrosive liquids (e.g., 98 wt% H2 SO4 ) and ultralow surface tension liquids (e.g., alcohols), with ultralow roll-off angles (<5°), and tunable resistance to liquid penetration. Additionally, these coatings demonstrate the potential in effective cargo loading and robust self-cleaning properties, where experimental datasets are correlated with both relevant theoretical predictions and systematic all-atom molecular dynamics simulations of the repellent coatings. This work not only holds promise for chemical shielding, heat transfer, and liquid manipulations but offers a facile yet robust pathway for engineering advanced coatings by effectively combining components for their mutually desired properties.