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Angewandte Chemie (International Ed. in... Jul 2024Graphite (Gr)-based lithium-ion batteries with admirable electrochemical performance below -20 °C are desired but are hindered by sluggish interfacial charge transport...
Graphite (Gr)-based lithium-ion batteries with admirable electrochemical performance below -20 °C are desired but are hindered by sluggish interfacial charge transport and desolvation process. Li salt dissociation via Li+-solvent interaction enables mobile Li+ liberation and contributes to bulk ion transport, while is contradictory to fast interfacial desolvation. Designing kinetically-stable solid electrolyte interphase (SEI) without compromising strong Li+-solvent interaction is expected to compatibly improve interfacial charge transport and desolvation kinetics. However, the relationship between physicochemical features and temperature-dependent kinetics properties of SEI remains vague. Herein, we propose four key thermodynamics parameters of SEI potentially influencing low-temperature electrochemistry, including electron work function, Li+ transfer barrier, surface energy, and desolvation energy. Based on the above parameters, we further define a novel descriptor, separation factor of SEI (SSEI), to quantitatively depict charge (Li+/e-) transport and solvent deprivation processes at Gr/electrolyte interface. A Li3PO4-based, inorganics-enriched SEI derived by Li difluorophosphate (LiDFP) additive exhibits the highest SSEI (4.89×103) to enable efficient Li+ conduction, e- blocking and rapid desolvation, and as a result, much suppressed Li-metal precipitation, electrolyte decomposition and Gr sheets exfoliation, thus improving low-temperature battery performances. Overall, our work originally provides visualized guides to improve low-temperature reaction kinetics/thermodynamics by constructing desirable SEI chemistry.
PubMed: 38955769
DOI: 10.1002/anie.202411029 -
Journal of Colloid and Interface Science Jun 2024Lithium-sulfur batteries (LSBs) hold promise as the next-generation lithium-ion batteries (LIBs) due to their ultra-high theoretical capacity and remarkable...
A multifunctional solution to enhance capacity and stability in lithium-sulfur batteries: Incorporating hollow CeO nanorods into carbonized non-woven fabric as an interlayer.
Lithium-sulfur batteries (LSBs) hold promise as the next-generation lithium-ion batteries (LIBs) due to their ultra-high theoretical capacity and remarkable cost-efficiency. However, these batteries suffer from the serious shuttle effect, challenging their practical application. To address this challenge, we have developed a unique interlayer (HCON@CNWF) composed of hollow cerium oxide nanorods (CeO) anchored to carbonized non-woven viscose fabric (CNWF), utilizing a straightforward template method. The prepared interlayer features a three-dimensional (3D) conductive network that serves as a protective barrier and enhances electron/ion transport. Additionally, the CeO component effectively chemisorbs and catalytically transforms lithium polysulfides (LiPSs), offering robust chemisorption and activation sites. Moreover, the unique porous structure of the HCON@CNWF not only physically adsorbs LiPSs but also provides ample space for sulfur's volume expansion, thus mitigating the shuttle effect and safeguarding the electrode against damage. These advantages collectively contribute to the battery's outstanding electrochemical performance, notably in retaining a reversible capacity of 80.82 % (792 ± 5.60 mAh g) of the initial value after 200 charge/discharge cycles at 0.5C. In addition, the battery with HCON@CNWF interlayer has excellent electrochemical performance at high sulfur loading (4 mg cm) and low liquid/sulfur ratio (7.5 µL mg). This study, thus, offers a novel approach to designing advanced interlayers that can enhance the performance of LSBs.
PubMed: 38955018
DOI: 10.1016/j.jcis.2024.06.228 -
ACS Nano Jul 2024Graphite exhibits crystal anisotropy, which impedes the mass transfer of ion intercalation and extraction processes in Li-ion batteries. Herein, a dual-shock chemical...
Graphite exhibits crystal anisotropy, which impedes the mass transfer of ion intercalation and extraction processes in Li-ion batteries. Herein, a dual-shock chemical strategy has been developed to synthesize the carbon anode. This approach comprised two key phases: (1) a thermal shock utilizing ultrahigh temperature (3228 K) can thermodynamically facilitate graphitization; (2) a mechanical shock (21.64 MPa) disrupting the π-π interactions in the aromatic chains of carbon can result in hybrid-structured carbon composed of crystalline and amorphous carbon. The optimized carbon (DSC-200-0.3) demonstrates a capacity of 208.61 mAh/g at a 10C rate, with a significant enhancement comparing with 15 mAh/g of the original graphite. Impressively, it maintains 81.06% capacity even after 3000 charge-discharge cycles. Dynamic process analysis reveals that this superior rate performance is attributed to a larger interlayer spacing facilitating ion transport comparing with the original graphite, disordered amorphous carbon for additional lithium storage sites, and crystallized carbon for enhanced charge transfer. The dual-shock chemical approach offers a cost-effective and efficient method to rapidly produce hybrid-structured carbon anodes, enabling 10C fast charging capabilities in lithium-ion batteries.
PubMed: 38954797
DOI: 10.1021/acsnano.4c02300 -
Environmental Science and Pollution... Jul 2024As a widely used pesticide, abamectin could be a threat to nontarget organisms. In this study, the toxic mechanism of abamectin on osmoregulation in Procambarus clarkii...
As a widely used pesticide, abamectin could be a threat to nontarget organisms. In this study, the toxic mechanism of abamectin on osmoregulation in Procambarus clarkii was explored for the first time. The results of this study showed that with increasing abamectin concentration, the membrane structures of gill filaments were damaged, with changes in ATPase activities, transporter contents, biogenic amine contents, and gene expression levels. The results of this study indicated that at 0.2 mg/L abamectin, ion diffusion could maintain osmoregulation. At 0.4 mg/L abamectin, passive transport was inhibited due to damage to the membrane structures of gill filaments, and active transport needed to be enhanced for osmoregulation. At 0.6 mg/L abamectin, the membrane structures of gill filaments were seriously damaged, and the expression level of osmoregulation-related genes decreased, but the organisms were still mobilizing various transporters, ATPases, and biogenic amines to address abamectin stress. This study provided a theoretical basis for further study of the effects of contaminations in aquatic environment on the health of crustaceans.
PubMed: 38954342
DOI: 10.1007/s11356-024-34056-5 -
Nano-micro Letters Jul 2024The rapid development of organic electrochemical transistors (OECTs) has ushered in a new era in organic electronics, distinguishing itself through its application in a... (Review)
Review
The rapid development of organic electrochemical transistors (OECTs) has ushered in a new era in organic electronics, distinguishing itself through its application in a variety of domains, from high-speed logic circuits to sensitive biosensors, and neuromorphic devices like artificial synapses and organic electrochemical random-access memories. Despite recent strides in enhancing OECT performance, driven by the demand for superior transient response capabilities, a comprehensive understanding of the complex interplay between charge and ion transport, alongside electron-ion interactions, as well as the optimization strategies, remains elusive. This review aims to bridge this gap by providing a systematic overview on the fundamental working principles of OECT transient responses, emphasizing advancements in device physics and optimization approaches. We review the critical aspect of transient ion dynamics in both volatile and non-volatile applications, as well as the impact of materials, morphology, device structure strategies on optimizing transient responses. This paper not only offers a detailed overview of the current state of the art, but also identifies promising avenues for future research, aiming to drive future performance advancements in diversified applications.
PubMed: 38954272
DOI: 10.1007/s40820-024-01452-y -
Microbial Cell Factories Jul 2024Advancing the engineering of photosynthesis-based prokaryotic cell factories is important for sustainable chemical production and requires a deep understanding of the...
BACKGROUND
Advancing the engineering of photosynthesis-based prokaryotic cell factories is important for sustainable chemical production and requires a deep understanding of the interplay between bioenergetic and metabolic pathways. Rearrangements in photosynthetic electron flow to increase the efficient use of the light energy for carbon fixation must be balanced with a strong carbon sink to avoid photoinhibition. In the cyanobacterium Synechocystis sp. PCC 6803, the flavodiiron protein Flv3 functions as an alternative electron acceptor of photosystem I and represents an interesting engineering target for reorganizing electron flow in attempts to enhance photosynthetic CO fixation and increase production yield.
RESULTS
We have shown that inactivation of Flv3 in engineered sucrose-excreting Synechocystis (S02:Δflv3) induces a transition from photoautotrophic sucrose production to mixotrophic growth sustained by sucrose re-uptake and the formation of intracellular carbon sinks such as glycogen and polyhydroxybutyrate. The growth of S02:Δflv3 exceeds that of the sucrose-producing strain (S02) and demonstrates unforeseen proteomic and metabolomic changes over the course of the nine-day cultivation. In the absence of Flv3, a down-regulation of proteins related to photosynthetic light reactions and CO assimilation occurred concomitantly with up-regulation of those related to glycolytic pathways, before any differences in sucrose production between S02 and S02:Δflv3 strains were observed. Over time, increased sucrose degradation in S02:Δflv3 led to the upregulation of respiratory pathway components, such as the plastoquinone reductase complexes NDH-1 and NDH-2 and the terminal respiratory oxidases Cyd and Cox, which transfer electrons to O. While glycolytic metabolism is significantly up-regulated in S02:Δflv3 to provide energy for the cell, the accumulation of intracellular storage compounds and the increase in respiration serve as indirect sinks for photosynthetic electrons.
CONCLUSIONS
Our results show that the presence of strong carbon sink in the engineered sucrose-producing Synechocystis S02 strain, operating under high light, high CO and salt stress, cannot compensate for the lack of Flv3 by directly balancing the light transducing source and carbon fixing sink reactions. Instead, the cells immediately sense the imbalance, leading to extensive reprogramming of cellular bioenergetic, metabolic and ion transport pathways that favor mixotrophic growth rather than enhancing photoautotrophic sucrose production.
Topics: Synechocystis; Photosynthesis; Sucrose; Bacterial Proteins; Carbon; Electron Transport; Proteomics; Carbon Dioxide
PubMed: 38951789
DOI: 10.1186/s12934-024-02462-6 -
Nature Communications Jun 2024The microgeometry of the cellular microenvironment profoundly impacts cellular behaviors, yet the link between it and the ubiquitously expressed mechanosensitive ion...
The microgeometry of the cellular microenvironment profoundly impacts cellular behaviors, yet the link between it and the ubiquitously expressed mechanosensitive ion channel PIEZO1 remains unclear. Herein, we describe a fluorescent micropipette aspiration assay that allows for simultaneous visualization of intracellular calcium dynamics and cytoskeletal architecture in real-time, under varied micropipette geometries. By integrating elastic shell finite element analysis with fluorescent lifetime imaging microscopy and employing PIEZO1-specific transgenic red blood cells and HEK cell lines, we demonstrate a direct correlation between the microscale geometry of aspiration and PIEZO1-mediated calcium signaling. We reveal that increased micropipette tip angles and physical constrictions lead to a significant reorganization of F-actin, accumulation at the aspirated cell neck, and subsequently amplify the tension stress at the dome of the cell to induce more PIEZO1's activity. Disruption of the F-actin network or inhibition of its mobility leads to a notable decline in PIEZO1 mediated calcium influx, underscoring its critical role in cellular mechanosensing amidst geometrical constraints.
Topics: Humans; Ion Channels; Mechanotransduction, Cellular; Actins; HEK293 Cells; Cytoskeleton; Calcium; Calcium Signaling; Finite Element Analysis; Animals; Microscopy, Fluorescence
PubMed: 38951553
DOI: 10.1038/s41467-024-49833-6 -
Planta Jul 2024Nitrogen stress altered important lipid parameters and related genes in Chlorella pyrenoidosa via ROS and Ca signaling. The mutual interference between ROS and Ca...
Nitrogen stress altered important lipid parameters and related genes in Chlorella pyrenoidosa via ROS and Ca signaling. The mutual interference between ROS and Ca signaling was also uncovered. The changed mechanisms of lipid parameters (especially lipid classes and unsaturation of fatty acids) in microalgae are not completely well known under nitrogen stress. Therefore, Chlorella pyrenoidosa was exposed to 0, 0.5, 1 and 1.5 g L NaNO for 4 days. Then, the physiological and biochemical changes were measured. It was shown that the total lipid contents, neutral lipid ratios as well as their related genes (accD and DGAT) increased obviously while the polar lipid ratios, degrees of unsaturation as well as their related genes (PGP and desC) decreased significantly in nitrogen stress groups. The obvious correlations supported that gene expressions should be the necessary pathways to regulate the lipid changes in C. pyrenoidosa under nitrogen stress. The changes in ROS and Ca signaling as well as their significant correlations with corresponding genes and lipid parameters were analyzed. The results suggested that ROS and Ca may regulate these gene expressions and lipid changes in C. pyrenoidosa under nitrogen stress conditions. This was verified by the subordinate tests with an ROS inhibitor and calcium reagents. It also uncovered the clues of mutual interference between ROS and Ca signaling. To summarize, this study revealed the signaling pathways of important lipid changes in microalgae under N stress.
Topics: Chlorella; Reactive Oxygen Species; Nitrogen; Stress, Physiological; Lipid Metabolism; Calcium; Lipids; Calcium Signaling; Signal Transduction; Microalgae
PubMed: 38951320
DOI: 10.1007/s00425-024-04471-6 -
Scientific Reports Jul 2024Polyethylene glycols (PEGs) are used in industrial, medical, health care, and personal care applications. The cycling and disposal of synthetic polymers like PEGs pose...
Polyethylene glycols (PEGs) are used in industrial, medical, health care, and personal care applications. The cycling and disposal of synthetic polymers like PEGs pose significant environmental concerns. Detecting and monitoring PEGs in the real world calls for immediate attention. This study unveils the efficacy of time-of-flight secondary ion mass spectrometry (ToF-SIMS) as a reliable approach for precise analysis and identification of reference PEGs and PEGs used in cosmetic products. By comparing SIMS spectra, we show remarkable sensitivity in pinpointing distinctive ion peaks inherent to various PEG compounds. Moreover, the employment of principal component analysis effectively discriminates compositions among different samples. Notably, the application of SIMS two-dimensional image analysis visually portrays the spatial distribution of various PEGs as reference materials. The same is observed in authentic cosmetic products. The application of ToF-SIMS underscores its potential in distinguishing PEGs within intricate environmental context. ToF-SIMS provides an effective solution to studying emerging environmental challenges, offering straightforward sample preparation and superior detection of synthetic organics in mass spectral analysis. These features show that SIMS can serve as a promising alternative for evaluation and assessment of PEGs in terms of the source, emission, and transport of anthropogenic organics.
Topics: Cosmetics; Spectrometry, Mass, Secondary Ion; Polyethylene Glycols; Principal Component Analysis
PubMed: 38951137
DOI: 10.1038/s41598-024-65504-4 -
European Journal of Pharmacology Jun 2024Neurodegenerative disorders are diseases characterized by progressive degeneration of neurons and associated structures and are a major global issue growing more... (Review)
Review
Neurodegenerative disorders are diseases characterized by progressive degeneration of neurons and associated structures and are a major global issue growing more widespread as the global population's average age increases. Despite several investigations on their etiology, the specific cause of these disorders remains unknown. However, there are few symptomatic therapies to treat these disorders. Polyamines (PAs) (putrescine, spermidine, and spermine) are being studied for their role in neuroprotection, aging and cognitive impairment. They are ubiquitous polycations which have relatively higher concentrations in the brain and possess pleiotropic biochemical activities, including regulation of gene expression, ion channels, mitochondria Ca transport, autophagy induction, programmed cell death, and many more. Their cellular content is tightly regulated, and substantial evidence indicates that their altered levels and metabolism are strongly implicated in aging, stress, cognitive dysfunction, and neurodegenerative disorders. In addition, dietary polyamine supplementation has been reported to induce anti-aging effects, anti-oxidant effects, and improve locomotor abnormalities, and cognitive dysfunction. Thus, restoring the polyamine level is considered a promising pharmacological strategy to counteract neurodegeneration. This review highlights PAs' physiological role and the molecular mechanism underpinning their proposed neuroprotective effect in aging and neurodegenerative disorders.
PubMed: 38950837
DOI: 10.1016/j.ejphar.2024.176804