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Silicon (Si)-based anodes offer high theoretical capacity for lithium-ion batteries but suffer from severe volume changes and continuous solid electrolyte interphase (SEI) degradation. Here, we address these challenges by selective methylation of 1,3-dioxolane (DOL), thus shifting the unstable bulk polymerization to controlled interfacial reactions and resulting in a highly elastic SEI. Comparative studies of 2-methyl-1,3-dioxolane (2MDOL) and 4-methyl-1,3-dioxolane (4MDOL) reveal that 4MDOL, with its larger ring strain and more stable radical intermediates due to hyperconjugation effect, promotes the formation of high-molecular-weight polymeric species at the electrode-electrolyte interface. This elastic, polymer-rich SEI effectively accommodates volume changes of Si and inhibits continuous side reactions. Our designed electrolyte enables Si-based anode to achieve 85.4% capacity retention after 400 cycles at 0.5 C without additives, significantly outperforming conventional carbonate-based electrolytes. Full cells also demonstrate stable long-term cycling. This work provides new insights into molecular-level electrolyte design for high-performance Si anodes, offering a promising pathway toward next-generation lithium-ion batteries with enhanced energy density and longevity.
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Garnet Li7La3Zr2O12 (LLZO)-based solid-state electrolytes (SSEs) hold promise for realizing next-generation lithium metal batteries with high energy density. However, the high stiffness of high-temperature sintered LLZO makes it brittle and susceptible to strain during the fabrication of solid-state batteries. Cold-pressed LLZO exhibits improved ductility but suffers from insufficient Li+ conductivity. Here, we report cold-pressed Ta-doped LLZO (Ta-LZ) particles integrated with ductile Li6PS5Cl (LPSC) via a Li+ conductive Li-containing Ta-Cl structure. This configuration creates a continuous Li+ conduction network by enhancing the Li+ exchange at the Ta-LZ/LPSC interface. The resulting Ta-LZ/LPSC SSE exhibits Li+ conductivity of 4.42×10-4â S cm-1 and a low activation energy of 0.31â eV. Li symmetric cells with Ta-LZ/LPSC SSE demonstrate excellent Li dendrite suppression ability, with an improved critical current density of 5.0â mA cm-2 and a prolonged cycle life exceeding 600â h at 1â mA cm-2. Our finding provides valuable insights into developing cold-pressed ceramic powder electrolytes for high-performance all-solid-state batteries.
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Uncontrollable zinc (Zn) plating and hydrogen evolution greatly undermine Zn anode reversibility. Previous electrolyte designs focus on suppressing H2O reactivity, however, the accumulation of alkaline byproducts during battery calendar aging and cycling still deteriorates the battery performance. Here, we present a direct strategy to tackle such problems using a strong Brønsted acid, bis(trifluoromethanesulfonyl)imide (HTFSI), as the electrolyte additive. This approach reformulates battery interfacial chemistry on both electrodes, suppresses continuous corrosion reactions and promotes uniform Zn deposition. The enrichment of hydrophobic TFSI- anions at the Zn|electrolyte interface creates an H2O-deficient micro-environment, thus inhibiting Zn corrosion reactions and inducing a ZnS-rich interphase. This highly acidic electrolyte demonstrates high Zn plating/stripping Coulombic efficiency up to 99.7% at 1 mA cm-2 ( > 99.8% under higher current density and areal capacity). Additionally, Zn | |ZnV6O9 full cells exhibit a high capacity retention of 76.8% after 2000 cycles.
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Constraining the electrochemical reactivity of free solvent molecules is pivotal for developing high-voltage lithium metal batteries, especially for ether solvents with high Li metal compatibility but low oxidation stability ( <4.0 V vs Li+/Li). The typical high concentration electrolyte approach relies on nearly saturated Li+ coordination to ether molecules, which is confronted with severe side reactions under high voltages ( >4.4 V) and extensive exothermic reactions between Li metal and reactive anions. Herein, we propose a molecular anchoring approach to restrict the interfacial reactivity of free ether solvents in diluted electrolytes. The hydrogen-bonding interactions from the anchoring solvent effectively suppress excessive ether side reactions and enhances the stability of nickel rich cathodes at 4.7 V, despite the extremely low Li+/ether molar ratio (1:9) and the absence of typical anion-derived interphase. Furthermore, the exothermic processes under thermal abuse conditions are mitigated due to the reduced reactivity of anions, which effectively postpones the battery thermal runaway.
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Biothiols such as cysteine, homocysteine, and glutathione play significant roles in important biological activities, and their abnormal concentrations have been found to be closely associated with certain diseases, making their detection a critical task. To this end, fluorescent probes have become increasingly popular due to their numerous advantages, including easy handling, desirable spatiotemporal resolution, high sensitivity, fast response, and favorable biocompatibility. As a result, intensive research has been conducted to create fluorescent probes for the detection and imaging of biothiols. This brief review summarizes recent advances in the field of biothiol-responsive fluorescent probes, with an emphasis on rational probe design, including the reaction mechanism, discriminating detection, reversible detection, and specific detection. Furthermore, the challenges and prospects of fluorescence probes for biothiols are also outlined.
Asunto(s)
Cisteína , Colorantes Fluorescentes , Glutatión , Homocisteína , Espectrometría de Fluorescencia/métodosRESUMEN
Albeit ethers are favorable electrolyte solvents for lithium (Li) metal anode, their inferior oxidation stability (<4.0â V vs. Li/Li+ ) is problematic for high-voltage cathodes. Studies of ether electrolytes have been focusing on the archetype glyme structure with ethylene oxide moieties. Herein, we unveil the crucial effect of ion coordination configuration on oxidation stability by varying the ether backbone structure. The designed 1,3-dimethoxypropane (DMP, C3) forms a unique six-membered chelating complex with Li+ , whose stronger solvating ability suppresses oxidation side reactions. In addition, the favored hydrogen transfer reaction between C3 and anion induces a dramatic enrichment of LiF (a total atomic ratio of 76.7 %) on the cathode surface. As a result, the C3-based electrolyte enables greatly improved cycling of nickel-rich cathodes under 4.7â V. This study offers fundamental insights into rational electrolyte design for developing high-energy-density batteries.
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Ethers are promising electrolytes for lithium (Li) metal batteries (LMBs) because of their unique stability with Li metal. Although intensive research on designing anion-enriched electrolyte solvation structures has greatly improved their electrochemical stabilities, ether electrolytes are approaching an anodic bottleneck. Herein, we reveal the strong correlation between electrolyte solvation structure and oxidation stability. In contrast to previous designs of weakly solvating solvents for enhanced anion reactivities, the triglyme (G3)-based electrolyte with the largest Li+ solvation energy among different linear ethers demonstrates greatly improved stability on Ni-rich cathodes under an ultrahigh voltage of 4.7 V (93% capacity retention after 100 cycles). Ether electrolytes with a stronger Li+ solvating ability could greatly suppress deleterious oxidation side reactions by decreasing the lifetime of free labile ether molecules. This study provides critical insights into the dynamics of the solvation structure and its significant influence on the interfacial stability for future development of high-efficiency electrolytes for high-energy-density LMBs.
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Rechargeable potassium-oxygen batteries (KOB) are promising next-generation energy storage devices because of the highly reversible O2/O2- redox reactions during battery charge and discharge. However, the complicated cathode reaction processes seriously jeopardize the battery reaction kinetics and discharge capacity. Herein, we propose a hybrid-solvent strategy to effectively tune the K+ solvation structure, which demonstrates a critical influence on the charge-transfer kinetics and cathode reaction mechanism. The cosolvation of K+ by 1,2-dimethoxyethane (DME) and dimethyl sulfoxide (DMSO) could greatly decrease overpotentials for the cathode processes and increase the cathode discharge capacity. Furthermore, the Coulombic efficiency for the cathode could be significantly improved with the enhanced solution-mediated KO2 growth and stripping during cycling. This work provides a promising electrolyte design approach to improve the electrochemical performance of the KOB.
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OBJECTIVE: This research was designed to investigate the changes of inflammatory factors in patients after resection of lung adenocarcinoma with propofol versus etomidate. METHODS: A total of 104 patients who underwent resection of lung adenocarcinoma in our hospital were divided into a propofol group (group A, n=50) and an etomidate group (group B, n=54). The levels of CRP and IL-6 at different time points and the changes of blood gas indexes at 10 min before and after operation were observed in both groups. Their pain score and quality of life score were compared. Besides, we observed the wake-up time, tracheal extubation time and the incidence of adverse reactions. RESULTS: The anesthesia recovery and tracheal extubation time in group B were shorter than those in group A (P<0.05). After 10-minutes of spontaneous breathing, PaO2 and SaO2 in group B were higher than those in group A (P<0.05), and PaCO2 was lower (P<0.05); compared with group A. The incidence of adverse reactions and the levels of inflammatory factors in group B were lower than those in group A after operation (both P<0.05). The quality of life of patients in group B after operation was better than that in group A (P<0.05). There was no marked difference in VAS scores between groups. CONCLUSION: Etomidate has better anesthetic effect than propofol in lung adenocarcinoma resection, leading to better stabilization of the vital signs of patients and it also has higher safety.
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OBJECTIVE: To study the effect of hBcl-2 gene transfer on rat liver against ischemia-reperfusion injury, and explore the feasibility of this approach to reduce ischemia-reperfusion injury in liver transplantation. METHODS: We constructed the replication-deficient recombinant adenoviruses Adv-EGFP and Adv-Bcl-2 and transfected them into 293 cells and packaged into adenovirus particles for amplification and purification. The empty plasmid vector virus was constructed similarly. Male SD rats were randomized into Adv-Bcl-2-transfected group, Adv-EGFP-transfected group, ischemia-reperfusion group, and sham-operated group, and liver allograft transplantation model was established by sleeve method. In the transfected groups, the recombinant viruses were administered by perfusion through the portal vein, and the ischemia-reperfusion and sham-operated groups received no treatment. Real-time quantitative PCR and Western blotting were used to detect the mRNA and protein expressions of bcl-2 in the liver tissue of each group, and at 0, 60 and 180 min after reperfusion, serum AST, LDH, and MDA levels were measured. Histological changes of the liver cells were evaluated by HE staining. RESULTS: Bcl-2 mRNA and protein expressions in Adv-Bcl-2-transfected group, as compared with those in Adv-EGFP-transfected group and control group, were significantly increased (P<0.01); the serum levels of AST, LDH and MDA in Adv-Bcl-2-transfected group were significantly lower than those of Adv-EGFP-transfected group and ischemia-reperfusion group (P<0.05 or 0.01). Compared with the sham-operated group, Adv-Bcl-2 treatment group showed lessened edema and vacuolar degeneration of the liver cells without patches or spots of necrosis. In ischemia-reperfusion and Adv-EGFP group, HE staining revealed hepatic lobular destruction and extensive liver cell swelling, enlargement, vacuolar degeneration, edema and occasional focal necrosis. CONCLUSION: Adv-Bcl-2 transfection can induce the expression of bcl-2 gene to reduce ischemia-reperfusion injury of the liver graft in rats.