Confined Element Distribution with Structure-driven Energy Coupling for Enhanced Prussian Blue Analogue Cathode.

The structural failure of Na2Mn[Fe(CN)6] could not be alleviated with traditional modification strategies through the adjustable composition property of Prussian blue analogues (PBAs), considering that the accumulation and release of stress derived from the MnN6 octahedrons are unilaterally restrained. Herein, a novel application of adjustable composition property, through constructing a coordination competition relationship between chelators and [Fe(CN)6]4- to directionally tune the enrichment of elements, is proposed to restrain structural degradation and induce unconventional energy coupling phenomenon. The non-uniform distribution of elements at the M1 site of PBAs (NFM-PB) is manipulated by the sequentially precipitated Ni, Fe, and Mn according to the Irving-William order. Electrochemically active Fe is operated to accompany Mn, and zero-strain Ni is modulated to enrich at the surface, synergistically mitigating with the enrichment and release of stress and then significantly improving the structural stability. Furthermore, unconventional energy coupling effect, a fusion of the electrochemical behavior between FeLS and MnHS, is triggered by the confined element distribution, leading to the enhanced electrochemical stability and anti-polarization ability. Consequently, the NFM-PB demonstrates superior rate performance and cycling stability. These findings further exploit potentialities of the adjustable composition property and provide new insights into the component design engineering for advanced PBAs.

Annealing Modulation Defect Chemistry toward High-Performance Sodium-Layered Cathodes.

Layered sodium transition-metal oxides generally encounter severe capacity decay and inferior rate performance during cycling, especially at a high state of charge. Herein, defect concentration is rationally modulated to explore the impact on electrochemical behavior in NaNi1/3Fe1/3Mn1/3O2 layered oxides. Bulk vacancies are increased through annealing in an oxygen-rich atmosphere, demonstrated by electron paramagnetic resonance measurement. It is found that the cathode with enriched oxygen vacancies exhibits significantly enhanced reversibility of redox reactions with a higher initial Coulombic efficiency of 90.0%. Furthermore, the reduced volume variations during the initial charge/discharge process are also confirmed by in situ X-ray diffraction. As a result, the oxygen-vacancy-rich cathode shows great cycling stability and superior rate performances. Also, full cells deliver a specific capacity of approximately 145.2 mAh g-1 at 0.5 C, with a high capacity retention of 78.3% after 100 cycles. This work presents a viable strategy for designing Na+ intercalated cathodes with a high-energy density.

Trace Fluorinated Carbon dots driven Li-Garnet Solid-State Batteries.

Garnet solid-state electrolyte Li6.5La3Zr1.5Ta0.5O12 (LLZTO) holds significant promise. However, the practical utilization has been seriously impeded by the poor contact of Li|garnet and electron leakage. Herein, one new type garnet-based solid-state batteries is prososed with high-performance  through the disparity in interfacial energy, induced by the reaction between trace fluorinated carbon dots (FCDs) and Li. The work of adhesion of Li|garnet is increased by the acquired Li-FCD composite, which facilitates an intimate Li|garnet interface with the promoted uniform Li+ deposition, revealed by density functional theory (DFT) calculations. It is futher validated that a concentrated C-Li2O-LiF component at the Li|garnet interface is spontaneously constructed, due to the the significant disparity in interfacial energy between C-Li2O-LiF|LLZTO and C-Li2O-LiF|Li. Furthermore, The electron transport and Li dendrites penetration are effectively hindered by the formed Li2O and LiF. The Li-FCD|LLZTO|Li-FCD symmetrical cells demonstrate stable cycling performance for over 3000 hours at 0.3 mA cm-2 and 800 hours at 0.5 mA cm-2. Furthermore, the LFP|garnet|Li-FCD full cell exhibit remarkable cycling performance (91.6% capacity retention after 500 cycles at 1 C). Our research has revealed a novel approach to establish a dendrite-free Li|garnet interface, laying the groundwork for future advancements in garnet-based solid-state batteries.

A nitrogen-doped carbon fiber coating embedded in the separator for stable zinc batteries.

A separator modification strategy was proposed by placing nitrogen-doped carbon fibers (NCF700) in the middle of the separator to prevent direct contact between the coating and the rigid zinc metal anode, resulting in coating cracks. The NCF700 coating can homogenize the electric field distribution and increase the transference number of zinc ions. Therefore, the battery assembled with the NCF700 coated separator exhibits superior cycling stability compared to the bare separator.

Biomass-Derived Hard Carbon for Sodium-Ion Batteries: Basic Research and Industrial Application.

Sodium-ion batteries (SIBs) have significant potential for applications in portable electric vehicles and intermittent renewable energy storage due to their relatively low cost. Currently, hard carbon (HC) materials are considered commercially viable anode materials for SIBs due to their advantages, including larger capacity, low cost, low operating voltage, and inimitable microstructure. Among these materials, renewable biomass-derived hard carbon anodes are commonly used in SIBs. However, the reports about biomass hard carbon from basic research to industrial applications are very rare. In this paper, we focus on the research progress of biomass-derived hard carbon materials from the following perspectives: (1) sodium storage mechanisms in hard carbon; (2) optimization strategies for hard carbon materials encompassing design, synthesis, heteroatom doping, material compounding, electrolyte modulation, and presodiation; (3) classification of different biomass-derived hard carbon materials based on precursor source, a comparison of their properties, and a discussion on the effects of different biomass sources on hard carbon material properties; (4) challenges and strategies for practical of biomass-derived hard carbon anode in SIBs; and (5) an overview of the current industrialization of biomass-derived hard carbon anodes. Finally, we present the challenges, strategies, and prospects for the future development of biomass-derived hard carbon materials.

Manipulating Local Chemistry and Coherent Structures for High-Rate and Long-Life Sodium-Ion Battery Cathodes.

Layered sodium transition-metal (TM) oxides generally suffer from severe capacity decay and poor rate performance during cycling, especially at a high state of charge (SoC). Herein, an insight into failure mechanisms within high-voltage layered cathodes is unveiled, while a two-in-one tactic of charge localization and coherent structures is devised to improve structural integrity and Na+ transport kinetics, elucidated by density functional theory calculations. Elevated Jahn-Teller [Mn3+O6] concentration on the particle surface during sodiation, coupled with intense interlayer repulsion and adverse oxygen instability, leads to irreversible damage to the near-surface structure, as demonstrated by X-ray absorption spectroscopy and in situ characterization techniques. It is further validated that the structural skeleton is substantially strengthened through the electronic structure modulation surrounding oxygen. Furthermore, optimized Na+ diffusion is effectively attainable via regulating intergrown structures, successfully achieved by the Zn2+ inducer. Greatly, good redox reversibility with an initial Coulombic efficiency of 92.6%, impressive rate capability (86.5 mAh g-1 with 70.4% retention at 10C), and enhanced cycling stability (71.6% retention after 300 cycles at 5C) are exhibited in the P2/O3 biphasic cathode. It is believed that a profound comprehension of layered oxides will herald fresh perspectives to develop high-voltage cathode materials for sodium-ion batteries.

Combined of plasma-activated water and dielectric barrier discharge atmospheric cold plasma treatment improves the characteristic flavor of Asian sea bass (Lates calcarifer) through facilitating lipid oxidation.

To explore the combination effects of plasma-activated water and dielectric barrier discharge (PAW-DBD) cold plasma treatment on the formation of volatile flavor and lipid oxidation in Asian sea bass (ASB), the volatile flavor compounds and lipid profiles were characterized by gas chromatography-ion mobility spectrometry and LC-MS-based lipidomics analyses. In total, 38 volatile flavor compound types were identified, and the PAW-DBD group showed the most kinds of volatile components with a significant (p < 0.05) higher content in aldehydes, ketones, and alcohols. A total of 1500 lipids was detected in lipidomics analysis, phosphatidylcholine was the most followed by triglyceride. The total saturated fatty acids content in PAW-DBD group increased by 105.02 µg/g, while the total content of unsaturated fatty acids decreased by 275.36 µg/g. It can be concluded that the PAW-DBD processing increased both the types and amounts of the volatile flavor in ASB and promoted lipid oxidation by altering lipid profiles.

Aluminum ion chemistry of Na4Fe3(PO4)2(P2O7) for all-climate full Na-ion battery.

Na4Fe3(PO4)2(P2O7) (NFPP) is currently drawing increased attention as a sodium-ion batteries (SIBs) cathode due to the cost-effective and NASICON-type structure features. Owing to the sluggish electron and Na+ conductivities, however, its real implementation is impeded by the grievous capacity decay and inferior rate capability. Herein, multivalent cation substituted microporous Na3.9Fe2.9Al0.1(PO4)2(P2O7) (NFAPP) with wide operation-temperature is elaborately designed through regulating structure/interface coupled electron/ion transport. Greatly, the derived Na vacancy and charge rearrangement induced by trivalent Al3+ substitution lower the ions diffusion barriers, thereby endowing faster electron transport and Na+ mobility. More importantly, the existing Al-O-P bonds strengthen the local environment and alleviate the volume vibration during (de)sodiation, enabling highly reversible valence variation and structural evolution. As a result, remarkable cyclability (over 10,000 loops), ultrafast rate capability (200 C), and exceptional all-climate stability (-40-60 °C) in half/full cells are demonstrated. Given this, the rational work might provide an actionable strategy to promote the electrochemical property of NFPP, thus unveiling the great application prospect of sodium iron mixed phosphate materials.

Expression of red/green-cone opsin mutants K82E, P187S, M273K result in unique pathobiological perturbations to cone structure and function.

Long-and middle-wavelength cone photoreceptors, which are responsible for our visual acuity and color vision, comprise ~95% of our total cone population and are concentrated in the fovea of our retina. Previously, we characterized the disease mechanisms of the L/M-cone opsin missense mutations N94K, W177R, P307L, R330Q and G338E, all of which are associated with congenital blue cone monochromacy (BCM) or color-vision deficiency. Here, we used a similar viral vector-based gene delivery approach in M-opsin knockout mice to investigate the pathogenic consequences of the BCM or color-vision deficient associated L-cone opsin (OPN1LW) mutants K82E, P187S, and M273K. We investigated their subcellular localization, the pathogenic effects on cone structure, function, and cone viability. K82E mutants were detected predominately in cone outer segments, and its expression partially restored expression and correct localization of cone PDE6α' and cone transducin γ. As a result, K82E also demonstrated the ability to mediate cone light responses. In contrast, expression of P187S was minimally detected by either western blot or by immunohistochemistry, probably due to efficient degradation of the mutant protein. M273K cone opsin appeared to be misfolded as it was primarily localized to the cone inner segment and endoplasmic reticulum. Additionally, M273K did not restore the expression of cone PDE6α' and cone transducin γ in dorsal cone OS, presumably by its inability to bind 11-cis retinal. Consistent with the observed expression pattern, P187S and M273K cone opsin mutants were unable to mediate light responses. Moreover, expression of K82E, P187S, and M273K mutants reduced cone viability. Due to the distinct expression patterns and phenotypic differences of these mutants observed in vivo, we suggest that the pathobiological mechanisms of these mutants are distinct.

Effects of Gas Composition on the Lipid Oxidation and Fatty Acid Concentration of Tilapia Fillets Treated with In-Package Atmospheric Cold Plasma.

Cold plasma (CP) is a non-thermal preservation technology that has been successfully used to decontaminate and extend the shelf life of aquatic products. However, the preservation effect of CP treatment is determined by several factors, including voltage, time, and gas compositions. Therefore, this study aimed to investigate the effects of gas composition (GasA: 10% O2, 50% N2, 40% CO2; GasB: air; GasC: 30% O2, 30% N2, 40% CO2) on the lipid oxidation of tilapia fillets treated after CP treatment. Changes in the lipid oxidation values, the percentages of fatty acids, and sensory scores were studied during 8 d of refrigerator storage. The results showed that the CP treatment significantly increased all the primary and secondary lipid oxidation values measured in this study, as well as the percentages of saturated fatty acids, but decreased the percentages of unsaturated fatty acids, especially polyunsaturated fatty acids. The lipid oxidation values were significantly increased in the GasC-CP group. After 8 d, clearly increased percentages of saturated fatty acids, a low level of major polyunsaturated fatty acids (especially linoleic (C18:2n-6)), and a decrease in the percentages of eicosapentaenoic acid (C20:5n-3) and docosahexaenoic acid (C22:6n-3) were found in GasC-CP; that is, the serious oxidation of lipids was found in the high O2 concentration group. In addition, the sensory score was also lower than that of the hypoxia CP group. Therefore, high O2 concentrations can enhance lipid oxidation and the changes in the fatty acid concentration. Controlling the O2 concentration is reasonable to limit the degree to which lipids are oxidized in tilapia after the in-package CP treatment.

LC-MS-based lipidomics analyses of alterations in lipid profiles of Asian sea bass (Lates calcarifer) induced by plasma-activated water treatment.

A lipidomics approach based on liquid chromatography-mass spectrometry was employed to investigate alterations in lipid profiles within the muscles of Asian sea bass (ASB) (Lates calcarifer) post-treatment with plasms-activated water (PAW). Lipidomics studies detected 1500 diverse lipid types in ASB muscles; the phosphatidylcholine (PC) lipid subclass constituted the highest number of lipids (21.07 %), followed by triglycerides (TGs, 20.53 %) and phosphatidylethanolamine (PE, 12.73 %). Comparative analysis between PAW-treated ASB and raw ASB revealed the presence of differentially abundant lipids, with 48 lipids accumulating at high levels and 92 at low levels. Pathway enrichment analysis identified a total of seven lipid-related metabolic pathways; glycerophospholipid metabolism emerged as the predominant pathway. Furthermore, the content of saturated fatty acids in PAW-treated ASB increased from 1059.81 µg/g (raw ASB) to 1099.77 µg/g. Conversely, the content of monounsaturated and polyunsaturated fatty acids decreased from 645.81 µg/g and 875.02 µg/g to 640.80 µg/g and 825.25 µg/g, respectively. Collectively, these results indicate significant alterations in ASB lipid profiles following PAW treatment, establishing a theoretical foundation for understanding the mechanism involved in promoting lipid oxidation.

Identification of clinical prognostic factors and analysis of ferroptosis-related gene signatures in the bladder cancer immune microenvironment.

BACKGROUND: Bladder cancer (BLCA) is a prevalent malignancy affecting the urinary system and poses a significant burden in terms of both incidence and mortality rates on a global scale. Among all BLCA cases, non-muscle invasive bladder cancer constitutes approximately 75% of the total. In recent years, the concept of ferroptosis, an iron-dependent form of regulated cell death marked by the accumulation of lipid peroxides, has captured the attention of researchers worldwide. Nevertheless, the precise involvement of ferroptosis-related genes (FRGs) in the anti-BLCA response remains inadequately elucidated. METHODS: The integration of BLCA samples from the TCGA and GEO datasets facilitated the quantitative evaluation of FRGs, offering potential insights into their predictive capabilities. Leveraging the wealth of information encompassing mRNAsi, gene mutations, CNV, TMB, and clinical features within these datasets further enriched the analysis, augmenting its robustness and reliability. Through the utilization of Lasso regression, a prediction model was developed, enabling accurate prognostic assessments within the context of BLCA. Additionally, co-expression analysis shed light on the complex relationship between gene expression patterns and FRGs, unraveling their functional relevance and potential implications in BLCA. RESULTS: FRGs exhibited increased expression levels in the high-risk cohort of BLCA patients, even in the absence of other clinical indicators, suggesting their potential as prognostic markers. GSEA revealed enrichment of immunological and tumor-related pathways specifically in the high-risk group. Furthermore, notable differences were observed in immune function and m6a gene expression between the low- and high-risk groups. Several genes, including MYBPH, SOST, SPRR2A, and CRNN, were found to potentially participate in the oncogenic processes underlying BLCA. Additionally, CYP4F8, PDZD3, CRTAC1, and LRTM1 were identified as potential tumor suppressor genes. Significant discrepancies in immunological function and m6a gene expression were observed between the two risk groups, further highlighting the distinct molecular characteristics associated with different prognostic outcomes. Notably, strong correlations were observed among the prognostic model, CNVs, SNPs, and drug sensitivity profiles. CONCLUSIONS: FRGs are associated with the onset and progression of BLCA. A FRGs signature offers a viable alternative to predict BLCA, and these FRGs show a prospective research area for BLCA targeted treatment in the future.

Transcriptome Analysis Reveals Novel Insights into the Hyperaccumulator Phytolacca acinosa Roxb. Responses to Cadmium Stress.

Cadmium (Cd) is a highly toxic heavy metal that causes serious damage to plant and human health. Phytolacca acinosa Roxb. has a large amount of aboveground biomass and a rapid growth rate, and it has been identified as a novel type of Cd hyperaccumulator that can be harnessed for phytoremediation. However, the molecular mechanisms underlying the response of P. acinosa to Cd2+ stress remain largely unclear. In this study, the phenotype, biochemical, and physiological traits of P. acinosa seeds and seedlings were analyzed under different concentrations of Cd2+ treatments. The results showed higher Cd2+ tolerance of P. acinosa compared to common plants. Meanwhile, the Cd2+ content in shoots reached 449 mg/kg under 10 mg/L Cd2+ treatment, which was obviously higher than the threshold for Cd hyperaccumulators. To investigate the molecular mechanism underlying the adaptability of P. acinosa to Cd stress, RNA-Seq was used to examine transcriptional responses of P. acinosa to Cd stress. Transcriptome analysis found that 61 genes encoding TFs, 48 cell wall-related genes, 35 secondary metabolism-related genes, 133 membrane proteins and ion transporters, and 96 defense system-related genes were differentially expressed under Cd2+ stress, indicating that a series of genes were involved in Cd2+ stress, forming a complex signaling regulatory mechanism. These results provide new scientific evidence for elucidating the regulatory mechanisms of P. acinosa response to Cd2+ stress and new clues for the molecular breeding of heavy metal phytoremediation.

Structural and functional rescue of cones carrying the most common cone opsin C203R missense mutation.

An arginine to cysteine substitution at amino acid position 203 (C203R) is the most common missense mutation in human cone opsin. Linked to color blindness and blue cone monochromacy (BCM), C203 is involved in a crucial disulfide bond required for proper folding. It has previously been postulated that expression of mutant C203R cone opsin exerts a toxic effect on cone photoreceptors, similar to some well-characterized missense mutations in rhodopsin that lead to protein misfolding. In this study, we generated and characterized a BCM mouse model carrying the equivalent C203R mutation (Opn1mwC198R Opn1sw-/-) to investigate the disease mechanism and develop a gene therapy approach for this disorder. Untreated Opn1mwC198R Opn1sw-/- cones phenocopied affected cones in human patients with the equivalent mutation, exhibiting shortened or absent cone outer segments and loss of function. We determined that gene augmentation targeting cones specifically yielded robust rescue of cone function and structure when Opn1mwC198R Opn1sw-/- mice were treated at early ages. Importantly, treated cones displayed elaborated outer segments and replenished expression of crucial cone phototransduction proteins. Interestingly, we were unable to detect OPN1MWC198R mutant opsin at any age. We believe this is the first proof-of-concept study exploring the efficacy of gene therapy in BCM associated with a C203R mutation.

Lc-ms-based lipidomics analyses revealed changes in lipid profiles in Asian sea bass (Lates calcarifer) with dielectric barrier discharge (DBD) atmospheric plasma treatment.

A comprehensive LC-MS-based lipidomics analysis of Asian sea bass (Lates calcarifer) muscle after dielectric barrier discharge (DBD) atmospheric plasma treatment was performed. Through the analysis, 1500 lipid species were detected, phosphatidylcholine (PC, 27.80%) was the most abundant lipid, followed by triglyceride (TG, 20.50%) and phosphatidylethanolamine (PE, 17.10%). Among them, 125 lipid species were detected and identified as differentially abundant lipids in Asian sea bass (ASB). PCA and OPLS-DA showed that ASB lipids changed significantly after DBD treatment. Moreover, glycerophospholipid metabolism was key metabolic pathways, as PC, PE, and lysophosphatidylcholine (LPC) were key lipid metabolites. The findings concerning fatty acids revealed that the saturated fatty acids (SFA) content of ASB after DBD treatment increased by 8.54%, while the content of monounsaturated fatty acids (MUFA) and polyunsaturated fatty acids (PUFA) decreased by 13.77% and 9.16%, respectively. Our study establishes a foundation for the lipid oxidation mechanism of ASB following DBD treatment.

Optimization of cold plasma combined treatment process and its effect on the quality of Asian sea bass (Lates calcarifer) during refrigerated storage.

BACKGROUND: Cold plasma exhibits broad applicability in the realm of fish sterilization and preservation. The combination process of plasma-activated water and dielectric barrier discharge (PAW-DBD) was optimized, and its disinfection effects on bass fillets were studied. RESULTS: The best conditions for disinfection of PAW-DBD were as follows. Bass fillets were soaked in PAW for 150 s, and then treated by DBD system at 160 kV for 180 s. The total viable count (TVC) reduced by 1.68 log CFU g-1 . On the 15th day of refrigerated storage, TVC of PAW-DBD group was 7.01 log CFU g-1 , while the PAW and DBD group exhibited a TVC of 7.02 and 7.01 log CFU g-1 on day 12; the TVC of the control group was 7.13 log CFU g-1 on day 6. The sensory score, water-holding capacity, and 2-thiobarbituric acid reactive substance values of the PAW-DBD group were significantly higher than those of PAW and DBD group (P < 0.05), whereas the TVC, Pseudomonas spp. count, and pH of the group were significantly lower (P < 0.05) during refrigerated storage. CONCLUSION: PAW-DBD treatment can enhance the disinfection effect, maintain good quality, and extend the storage period of bass fillets. © 2023 Society of Chemical Industry.

High Voltage Ga-Doped P2-Type Na2/3 Ni0.2 Mn0.8 O2 Cathode for Sodium-Ion Batteries.

Ni/Mn-based oxide cathode materials have drawn great attention due to their high discharge voltage and large capacity, but structural instability at high potential causes rapid capacity decay. How to moderate the capacity loss while maintaining the advantages of high discharge voltage remains challenging. Herein, the replacement of Mn ions by Ga ions is proposed in the P2-Na2/3 Ni0.2 Mn0.8 O2 cathode for improving their cycling performances without sacrificing the high discharge voltage. With the introduction of Ga ions, the relative movement between the transition metal ions is restricted and more Na ions are retained in the lattice at high voltage, leading to an enhanced redox activity of Ni ions, validated by ex situ synchrotron X-ray absorption spectrum and X-ray photoelectron spectroscopy. Additionally, the P2-O2 phase transition is replaced by a P2-OP4 phase transition with a smaller volume change, reducing the lattice strain in the c-axis direction, as detected by operando/ex situ X-ray diffraction. Consequently, the Na2/3 Ni0.21 Mn0.74 Ga0.05 O2 electrode exhibits a high discharge voltage close to that of the undoped materials, while increasing voltage retention from 79% to 93% after 50 cycles. This work offers a new avenue for designing high-energy density Ni/Mn-based oxide cathodes for sodium-ion batteries.

Head-to-Head Comparison of CCN4, DNMT3A, PTPN11, and SPARC as Suppressors of Anti-tumor Immunity.

Purpose: Emergent cancer cells likely secrete factors that inhibit anti-tumor immunity. To identify such factors, we applied a functional assay with proteomics to an immunotherapy resistant syngeneic mouse melanoma model. Four secreted factors were identified that potentially mediate immunosuppression and could become targets for novel immunotherapies. We tested for consistent clinical correlates in existing human data and verified in vivo whether knocking out tumor cell production of these factors improved immune-mediated control of tumor growth. Methods: Existing human data was analyzed for clinical correlates. A CRISPR/Cas9 approach to generate knockout cell lines and a kinetic analysis leveraging a Markov Chain Monte Carlo (MCMC) approach quantified the various knockouts' effect on cells' intrinsic growth rate. Flow cytometry was used to characterize differences in immune infiltration. Results: While all four gene products were produced by malignant melanocytes, only increased CCN4 expression was associated with reduced survival in primary melanoma patients. In immunocompetent C57BL/6 mice the CCN4 knockout increased survival while the other knockouts had no effect. This survival advantage was lost when the CCN4 knockout cells were injected into immunocompromised hosts, indicating that the effect of CCN4 may be immune mediated. Parameter estimation from the MCMC analysis shows that CCN4 was the only knockout tested that decreased the net tumor growth rate in immunocompetent mice. Flow cytometry showed an increase in NK cell infiltration in CCN4 knockout tumors. Conclusions: The results suggest that CCN4 is a mediator of immunosuppression in the melanoma tumor microenvironment and a potential collateral immunotherapy target. Supplementary Information: The online version contains supplementary material available at 10.1007/s12195-023-00787-7.

Boosting the interfacial dynamics and thermodynamics in polyanion cathode by carbon dots for ultrafast-charging sodium ion batteries.

Ultrafast-charging is the focus of next-generation rechargeable batteries for widespread economic success by reducing the time cost. However, the poor ion diffusion rate, intrinsic electronic conductivity and structural stability of cathode materials seriously hinder the development of ultrafast-charging technology. To overcome these challenges, an interfacial dynamics and thermodynamics synergistic strategy is proposed to synchronously enhance the fast-charging capability and structural stability of polyanion cathode materials. As a case study, a Na3V2(PO4)3 composite (NVP/NSC) is successfully obtained by introducing an interface layer derived from N/S co-doped carbon dots. Density functional theory calculations validate that the interfacial bonding effect of V-N/S-C significantly reduces the Na+ transport energy barrier. D-band center theory analysis confirms the downward shift of the V d-band center enhances the strength of the V-O bond and considerably inhibits irreversible phase transformation. Benefitting from this interfacial synergistic strategy, NVP/NSC achieves a high capability and excellent cycling stability with a surprisingly low carbon content (2.23%) at an extremely high rate of 100C for 10 000 cycles (87.2 mA h g-1, 0.0028% capacity decay per cycle). Furthermore, a superior performance at 5C (115.3 mA h g-1, 92.1% capacity retention after 800 cycles) is exhibited by the NVP/NSC‖HC full cell. These findings provide timely new insights for the systematic design of ultrafast-charging cathode materials.

Carbon dots from alcohol molecules: principles and the reaction mechanism.

Carbon dots (CDs) have attracted significant attention in the energy, environment, and biology fields due to their exceptional physicochemical properties. However, owing to the multifarious precursors and complex reaction mechanisms, the production of carbon dots from organic molecules is still a mysterious process. Inspired by the color change of sodium hydroxide ethanol solution after standing for some time, in this work, we thoroughly investigated the reaction mechanism from alcohol molecules to carbon dots through a lot of experiments and theoretical calculations, and it was found that the rate-controlling reaction is the formation of aldehydes, and it is also confirmed that there is a self-catalysis reaction, which can accelerate the conversion from alcohol to aldehyde, further facilitating the final formation of CDs. After the rate-controlling reaction of alcohol to aldehyde, under strongly alkaline conditions, an aldol reaction occurs to form unsaturated aldehydes, followed by further condensation and polymerization reactions to form long carbon chains, which are cross-linked and dehydrated to form carbon dots with a carbon core and surface functional groups. Additionally, it is found that the reaction can be largely accelerated with the assistance of electricity, which indicates the great prospect of industrial production. Furthermore, the obtained CDs with rich functional groups can be utilized as electrolyte additives to optimize the deposition behavior of Na metal, manifesting great potential towards safe and stable Na metal batteries.