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Calcium-oxygen (Ca-O2) batteries can theoretically afford high capacity by the reduction of O2 to calcium oxide compounds (CaOx) at low cost1-5. Yet, a rechargeable Ca-O2 battery that operates at room temperature has not been achieved because the CaOx/O2 chemistry typically involves inert discharge products and few electrolytes can accommodate both a highly reductive Ca metal anode and O2. Here we report a Ca-O2 battery that is rechargeable for 700 cycles at room temperature. Our battery relies on a highly reversible two-electron redox to form chemically reactive calcium peroxide (CaO2) as the discharge product. Using a durable ionic liquid-based electrolyte, this two-electron reaction is enabled by the facilitated Ca plating-stripping in the Ca metal anode at room temperature and improved CaO2/O2 redox in the air cathode. We show the proposed Ca-O2 battery is stable in air and can be made into flexible fibres that are weaved into textile batteries for next-generation wearable systems.
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Radiation-induced fibrosis (RIF) is a severe chronic complication of radiotherapy (RT) manifested by excessive extracellular matrix (ECM) components deposition within the irradiated area. The lung, heart, skin, jaw, pelvic organs and so on may be affected by RIF, which hampers body functions and quality of life. There is accumulating evidence suggesting that the immune microenvironment may play a key regulatory role in RIF. This article discussed the synergetic or antagonistic effects of immune cells and mediators in regulating RIF's development. Several potential preventative and therapeutic strategies for RIF were proposed based on the immunological mechanisms to provide clinicians with improved cognition and clinical treatment guidance.
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Microambiente Celular , Fibrosis , Traumatismos por Radiación , Radioterapia , Humanos , Animales , Traumatismos por Radiación/inmunología , Radioterapia/efectos adversos , Matriz Extracelular/metabolismo , Matriz Extracelular/inmunología , Matriz Extracelular/efectos de la radiaciónRESUMEN
Transition metal oxides (TMOs) are recognized as high-efficiency electrocatalyst systems for restraining the shuttle effect in lithium-sulfur (Li-S) batteries, owing to their robust adsorption capabilities for polysulfides. However, the sluggish catalytic conversion of Li2S redox and severe passivation effect of TMOs exacerbate polysulfide shuttling and reduce the cyclability of Li-S batteries, which significantly hinders the development of TMOs electrocatalysts. Here, through the anion-cation doping approach, dual incorporation of phosphorus and molybdenum into MnO2 (P,Mo-MnO2) was engineered, demonstrating effective mitigation of the passivation effect and allowing for the simultaneous immobilization of polysulfides and rapid redox kinetics of Li2S. Both experimental and theoretical investigations reveal the pivotal role of dopants in fine-tuning the d-band center and optimizing the electronic structure of MnO2. Furthermore, this well-designed configuration processes catalytic selectivity. Specifically, P-doping expedites rapid Li2S nucleation kinetics by minimizing reaction-free energy, while Mo-doping facilitates robust Li2S dissolution kinetics by mitigating decomposition barriers. This dual-doping approach equips P,Mo-MnO2 with robust bi-directional catalytic activity, effectively overcoming passivation effect and suppressing the notorious shuttle effect. Consequently, Li-S batteries incorporating P,Mo-MnO2-based separators demonstrate favorable performance than pristine TMOs. This design offers rational viewpoint for the development of catalytic materials with superior bi-directional sulfur electrocatalytic in Li-S batteries.
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The reaction rate bottleneck during interconversion between insulating S8 (S) and Li2 S fundamentally leads to incomplete conversion and restricted lifespan of Li-S battery, especially under high S loading and lean electrolyte conditions. Herein, we demonstrate a new catalytic chemistry: soluble semiquinone, 2-tertbutyl-semianthraquinone lithium (Li+ TBAQâ - ), as both e- /Li+ donor and acceptor for simultaneous S reduction and Li2 S oxidation. The efficient activation of S and Li2 S by Li+ TBAQâ - in the initial discharging/charging state maximizes the amount of soluble lithium polysulfide, thereby substantially improve the rate of solid-liquid-solid reaction by promoting long-range electron transfer. With in situ Raman spectra and theoretical calculations, we reveal that the activation of S/Li2 S is the rate-limiting step for effective S utilization under high S loading and low E/S ratio. Beyond that, the S activation ratio is firstly proposed as an accurate indicator to quantitatively evaluate the reaction rate. As a result, the Li-S batteries with Li+ TBAQâ - deliver superior cycling performance and over 5 times higher S utilization ratio at high S loading of 7.0â mg cm-2 and a current rate of 1â C compared to those without Li+ TBAQâ - . We hope this study contributes to the fundamental understanding of S redox chemical and inspires the design of efficient catalysis for advanced Li-S batteries.
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Lithium iron phosphate (LFP)/graphite batteries have long dominated the energy storage battery market and are anticipated to become the dominant technology in the global power battery market. However, the poor fast-charging capability and low-temperature performance of LFP/graphite batteries seriously hinder their further spread. These limitations are strongly associated with the interfacial Li-ion transport. Here we report a wide-temperature-range ester-based electrolyte that exhibits high ionic conductivity, fast interfacial kinetics and excellent film-forming ability by regulating the anion chemistry of Li salt. The interfacial barrier of the battery is quantitatively unraveled by employing three-electrode system and distribution of relaxation time technique. The superior role of the proposed electrolyte in preventing Li0 plating and sustaining homogeneous and stable interphases are also systematically investigated. The LFP/graphite cells exhibit rechargeability in an ultrawide temperature range of -80°C to 80°C and outstanding fast-charging capability without compromising lifespan. Specially, the practical LFP/graphite pouch cells achieve 80.2% capacity retention after 1200 cycles (2 C) and 10-min charge to 89% (5 C) at 25°C and provides reliable power even at -80°C.
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Organic electrode materials (OEMs), valued for their sustainability and structural tunability, have been attracting increasing attention for wide application in sodium-ion batteries (SIBs) and other rechargeable batteries. However, most OEMs are plagued with insufficient specific capacity or poor cycling stability. Therefore, it's imperative to enhance their specific capacity and cycling stability through molecular design. Herein, we designed and synthesized a heteroaromatic molecule 2,3,8,9,14,15-hexanol hexaazatrinaphthalene (HATN-6OH) by the synergetic coupling of catechol (the precursor of ortho-quinone)/ortho-quinone functional groups and HATN conjugated core structures. The abundance of catechol/ortho-quinone and imine redox-active moieties delivers a high specific capacity of nine-electron transfer for SIBs. Most notably, the π-π interactions and intermolecular hydrogen bond forces among HATN-6OH molecules secure the stable long-term cycling performance of SIBs. Consequently, the as-prepared HATN-6OH electrode exhibited a high specific capacity (554â mAh g-1 at 0.1â A g-1 ), excellent rate capability (202â mAh g-1 at 10â A g-1 ), and stable long-term cycling performance (73 % after 3000 cycles at 10â A g-1 ) in SIBs. Additionally, the nine-electron transfer mechanism is confirmed by systematic density functional theory (DFT) calculation, attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), and Raman analysis. The achievement of the synergetic coupling of the redox-active sites on OEMs could be an important key to the enhancement of SIBs and other metal-ion batteries.
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In-line X-ray phase-contrast computed tomography typically contains two independent procedures: phase retrieval and computed tomography reconstruction, in which multi-material and streak artifacts are two important problems. To address these problems simultaneously, an accelerated 3D iterative image reconstruction algorithm is proposed. It merges the above-mentioned two procedures into one step, and establishes the data fidelity term in raw projection domain while introducing 3D total variation regularization term in image domain. Specifically, a transport-of-intensity equation (TIE)-based phase retrieval method is updated alternately for different areas of the multi-material sample. Simulation and experimental results validate the effectiveness and efficiency of the proposed algorithm.
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INTRODUCTION: The zygomaticomaxillary suture (ZMS) maturation evaluation is a reliable method for predicting the optimal timing of maxillary protraction. The objective of this study was to compare age distribution patterns of ZMS maturation stages between cleft lip and palate (CLP) patients and non-cleft lip and palate (non-CLP) patients to aid our comprehension in choosing the optimal timing of maxillary protraction. METHODS: Samples of 216 non-CLP and 220 CLP Asian patients without orthodontic and orthognathic treatment aged 5-25 years were scanned to evaluate the ZMS maturation stage by 2 evaluators blindly. Evaluators' agreements and bilateral ZMS maturation consistency were assessed by weighted kappa tests. Age distribution patterns of each ZMS maturation stage were described. Gender effect and age distribution differences between groups were analyzed using an independent t-test. RESULTS: Evaluators' agreements and bilateral ZMS maturation consistency were satisfying (weighted kappa coefficient >0.90). At stages A and B, patients with CLP were 1.3 and 0.4 years older than patients in the non-CLP group (P <0.001 and P = 0.01). In contrast, at stage C, patients with CLP were approximately 1.2 years younger (P = 0.004). Gender barely played a role in the divergence of ZMS maturation (P >0.05). No statistically significant difference was observed between ZMS maturation of patients with unilateral or bilateral cleft lip and palate (UBCLP) and patients with unilateral or bilateral cleft lip (UBCL) (P >0.05). CONCLUSIONS: The ZMS development of patients with CLP was premature at stage C, whereas delayed at stages A and B.
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Labio Leporino , Fisura del Paladar , Labio Leporino/cirugía , Fisura del Paladar/cirugía , Suturas Craneales , Humanos , SuturasRESUMEN
Bioinspired asymmetric nanofluidic ion channels with ionic diode behavior that can boost the osmotic energy (so-called blue energy) conversion are highly desirable, especially if they can be easily constructed and modified. Two-dimensional (2D) metal carbides and nitrides, known as MXenes, combine hydrophilic surfaces and tunable surface charge properties, providing a shortcut to prepare asymmetric nanofluidic ion channels. Here, we report a mechanically robust, flexible, and scale-up-friendly asymmetric Ti3 C2 Tx MXene-based ionic diode membrane with a highly rectified current and demonstrate its potential use in reverse electrodialysis osmotic energy conversion. Under the salinity gradient of synthetic seawater and river water, our ionic diode membrane-based generator's power density is 8.6â W m-2 and up to 17.8â W m-2 at a 500-fold salinity gradient, outperforming the state-of-the-art membranes. The design of MXene-based ionic diode-type membrane provides a facile and general strategy in developing large-scale 2D nanofluidics and selective ion transport.
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Salinidad , Titanio , Iones , Ósmosis , AguaRESUMEN
Propagation-based X-ray phase-contrast computed tomography (PB-PCCT) can serve as an effective tool for studying organ function and pathologies. However, it usually suffers from a high radiation dose due to the long scan time. To alleviate this problem, we propose a deep learning reconstruction framework for PB-PCCT with sparse-view projections. The framework consists of dual-path deep neural networks, where the edge detection, edge guidance, and artifact removal models are incorporated into two subnetworks. It is worth noting that the framework has the ability to achieve excellent performance by exploiting the data-based knowledge of the sample material characteristics and the model-based knowledge of PB-PCCT. To evaluate the effectiveness and capability of the proposed framework, simulations and real experiments were performed. The results demonstrated that the proposed framework could significantly suppress streaking artifacts and produce high-contrast and high-resolution computed tomography images.
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Clear and complete microstructural imaging of the root canal isthmus is an important part of pathological investigations in research and clinical practice. X-ray micro-computed tomography (µCT) is a widely used non-destructive imaging technique, which allows for distortion-free three-dimensional (3D) visualisation. While absorption µCT typically has poor contrast resolution for observing the root canal isthmus, especially for weak-absorbing tissues, propagation-based X-ray phase-contrast imaging (PBI) is a powerful imaging method, which in its combination with µCT (PB-PCµCT) enables high-resolution and high-contrast microstructural imaging of the weak-absorbing tissues in samples. To investigate the feasibility and ability of PB-PCµCT in microstructural imaging of the root canal isthmus, conventional absorption µCT and PB-PCµCT experiments were performed. The two-dimensional (2D) and 3D comparison results demonstrated that, compared to absorption µCT, PB-PCµCT has the ability to image the root canal isthmus more clearly and completely, and thus, it has great potential to serve as a valuable tool for biomedical and preclinical studies on the root canal isthmus.
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Cavidad Pulpar , Imagenología Tridimensional , Microscopía de Contraste de Fase , Microtomografía por Rayos X , Rayos XRESUMEN
Ustilaginoidea virens is the causal agent of rice false smut disease resulting in quantitative and qualitative losses in rice. To gain insights into the pathogenic mechanisms of U. virens, we established a T-DNA insertion mutant library of U. virens through Agrobacterium tumefaciens-mediated transformation and selected an enhanced pathogenicity mutant (i.e., B3277). We analyzed the biological characteristics of the wild-type P1 and B3277. The growth rate and sporulation of B3277 were decreased compared with those of P1; the ferrous iron could be utilized by B3277, but inhibited the growth of P1. Southern blot analysis was performed to verify the copy number of the foreign gene inserted in the genomic DNA and only one copy of the T-DNA was found. The combined hiTAIL-PCR with RACE-PCR analysis showed the successful cloning of full length of the T-DNA flanking gene associated with pathogenicity, named Uvt3277. Gene expression was analyzed using real-time PCR. Results revealed that Uvt3277 was expressed at lower levels in B3277 than in P1. This gene was then subjected to bioinformatics analysis. The encoded protein of Uvt3277 exhibited high homology with low-affinity iron transporter proteins in some fungi. Transformation of the RNAi vector by constructing the hairpin RNA of the target gene was confirmed as successful. The pathogenicity of the transformant also increased. These results suggested that Uvt3277 may have an important function associated with the pathogenesis of U. virens. This study provides insights into the pathogenic mechanism of U. virens and a molecular target of disease control.
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Ascomicetos/genética , Ascomicetos/metabolismo , Proteínas Fúngicas/genética , Proteínas Fúngicas/metabolismo , Hierro/metabolismo , Enfermedades de las Plantas/microbiología , Secuencia de Aminoácidos , Transporte Biológico , Clonación Molecular , Análisis por Conglomerados , ADN Bacteriano , Mutación , Oryza/microbiología , Fenotipo , Carácter Cuantitativo Heredable , Interferencia de ARN , Análisis de Secuencia de ADNRESUMEN
The plastic waste issue has posed a series of formidable challenges for the ecological environment and human health. While conventional recycling strategies often lead to plastic down-cycling, the electrochemical strategy of recovering valuable monomers enables an ideal, circular plastic economy. Here a corrosion synthesized single atom Pt1/Ni(OH)2 electrocatalyst with part-per-million noble Pt loading for highly efficient and selective upcycling of polyethylene terephthalate (PET) into valuable chemicals (potassium diformate and terephthalic acid) and green hydrogen is reported. Electro-oxidation of PET hydrolysate, ethylene glycol (EG), to formate is processed with high Faraday efficiency (FE) and selectivity (>90%) at the current density close to 1000 mA cm-2 (1.444 V vs RHE). The in situ spectroscopy and density functional theory calculations provide insights into the mechanism and the understanding of the high efficiency. Remarkably, the electro-oxidation of EG at the ampere-level current density is also successfully illustrated by using a membrane-electrode assembly with high FEs to formate integrated with hydrogen production for 500 h of continuous operation. This process allows valuable chemical production at high space-time yield and is highly profitable (588-700 $ ton-1 PET), showing an industrial perspective on single-atom catalysis of electrochemical plastic upcycling.
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Despite the high energy of LiNi0.8 Co0.1 Mn0.1 O2 (NCM811) cathode, it still suffers serious decay due to the continuous solvents decomposition and unstable cathode electrolyte interphase (CEI) layers, especially under high temperatures. The intense exothermic reaction between delithiated NCM811 and flammable electrolyte, on the other hand, pushes the batteries to their safety limit. Herein, these two issues are tackled via engineering the electrolytes, that is, utilizing salts with higher HOMO levels and nonflammable solvents with lower HOMO levels, to reduce the massive decomposition of solvents and improve battery safety under elevated temperatures. Consequently, a thin and boron-rich CEI is generated, which effectively inhibited the side reactions, thus improving the cycling stability and safety. Deviated from the highly concentrated electrolytes which heavily relies on the usage of massive salts, the electrolyte recipe can introduce a robust inorganic-rich CEI but use much less salt (i.e., dilute electrolyte), and thus, offer an encouraging alternative toward practical applications. As such, the NCM811 cathode exhibits a high-capacity retention of 81.2% after 950 cycles at 25 °C and 75% after 300 cycles at 55 °C. This work provides a universal electrolyte design strategy for designing stable and safe high-temperature electrolytes for the NCM811 cathode.
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All-solid-state lithium metal batteries (LMBs) are currently one of the best candidates for realizing the yearning high-energy-density batteries with high safety. However, even polyethylene oxide (PEO), the most popular polymeric solid-state electrolyte (SSE) with the largest ionic conductivity in the category so far, has significant challenges due to the safety issues of lithium dendrites, and the insufficient ionic conductivity. Herein, molecular sieve (MS) is integrated into the PEO as an inert filler with the liquid metal (LM) as a functional module, forming an "LM-MS-PEO" composite as both SSE with enhanced ionic conductivity, and protection layer against lithium dendrites. As demonstrated by theoretical and experimental investigations, LM released from MS can be uniformly and efficiently distributed in PEO, which could avoid agglomeration, enable the effective blocking of lithium dendrites, and regulate the mass transport of Li ions, thus achieving even deposition of lithium during charge/discharge. Moreover, MS could reduce the crystallinity of PEO, improve lithium-ion conductivity, and reduce operating temperature. Benefiting from the introduction of the functional MS/LM, the LM-MS-PEO electrolyte exhibits fourfold higher lithium ionic conductivity than the pristine PEO at 40 °C, while the as-assembled all-solid-state LMBs have four to five times longer stable cycle life.
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Nickel-rich layered oxide cathode material LiNixCoyMnzO2 (NCM) has emerged as a promising candidate for next-generation lithium-ion batteries (LIBs). These cathode materials possess high theoretical specific capacity, fast electron/ion transfer rate, and high output voltage. However, their potential is impeded by interface instability, irreversible phase transition, and the resultant significant capacity loss, limiting their practical application in LIBs. In this work, a simple and scalable approach is proposed to prepare gradient cathode material (M-NCM) with excellent structural stability and rate performance. Taking advantage of the strong coordination of Ni2+ with ammonia and the reduction reaction of KMnO4, the elemental compositions of the Ni-rich cathode are reasonably adjusted. The resulted gradient compositional design plays a crucial role in stabilizing the crystal structure, which effectively mitigates Li/Ni mixing and suppresses unwanted surficial parasitic reactions. As a result, the M-NCM cathode maintains 98.6% capacity after 200 cycles, and a rapid charging ability of 107.5 mAh g-1 at 15 C. Furthermore, a 1.2 Ah pouch cell configurated with graphite anode demonstrates a lifespan of over 500 cycles with only 8% capacity loss. This work provides a simple and scalable approach for the in situ construction of gradient cathode materials via cooperative coordination and deposition reactions.
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The periosteum plays a vital role in repairing bone defects. Researchers have demonstrated the existence of electrical potential in the periosteum and native bone, indicating that electrical signals are essential for functional bone regeneration. However, the clinical use of external electrical treatments has been limited due to their inconvenience and inefficacy. As an alternative, low-intensity pulsed ultrasound (LIPUS) is a noninvasive form of physical therapy that enhances bone regeneration. Furthermore, the wireless activation of piezoelectric biomaterials through ultrasound stimulation would generate electric charges precisely at the defect area, compensating for the insufficiency of external electrical stimulation and potentially promoting bone regeneration through the synergistic effect of mechanical and electrical stimulation. However, the optimal integration of LIPUS with an appropriate piezoelectric periosteum is yet to be explored. Herein, the BaTiO3/multiwalled-carbon nanotubes/collagen (BMC) membranes have been fabricated, possessing physicochemical properties including improved surface hydrophilicity, enhanced mechanical performance, ideal piezoelectricity, and outstanding biocompatibility, all of which are conducive to bone regeneration. When combined with LIPUS, the endogenous electrical microenvironment of native bone was recreated. After that, the wireless-generated electrical signals, along with the mechanical signals induced by LIPUS, were transferred to macrophages and activated Ca2+ influx through Piezo1. Ultimately, the regenerative effect of the BMC membrane with LIPUS stimulation (BMC + L) was confirmed in a mouse cranial defect model. Together, this research presents a co-engineering strategy that involves fabricating a novel biomimetic periosteum and utilizing the synergistic effect of ultrasound to enhance bone regeneration, which is achieved through the reinforcement of the electrical environment and the immunomodulation of macrophage polarization.
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Background: Liver cancer (LC) is one of the most common malignancies. Currently, nanotechnology has made great progress in LC research, and many studies on LC nanotechnology have been published. This study aims to discuss the current status, hot spots, and research trends in this field through bibliometric analysis. Methods: The Web of Science Core Collection (WoSCC) database was searched for papers related to hepatocellular carcinoma (HCC) included from January 2000 to November 2022, and its research hotspots and trends were visualized and analyzed with the help of VOSviewer. In addition, a search was conducted to find LC papers related to nanotechnology. Then we used the visual analysis software VOSviewer and CiteSpace to evaluate the contributions of countries/regions, authors, and journals related to the topic and analyze keywords to understand the research priorities and hot spots in the field as well as the development direction. Results: There are 1908 papers in the highly cited literature on LC, and its research hotspots are pathogenesis, risk factors, and survival rate. The literature on the application of nanotechnology in LC had 921 papers. Among them, China (n=560, 60.8%) and the United States (n=170, 18.5%) were the countries with the highest number of published papers. Wang Yan (n=11) and Llovet JM (n=131) were the first authors and co-cited authors, respectively. The International Journal of Nanomedicine was the most prolific academic journal (n=41). In addition to "hepatocellular carcinoma" and "nanoparticles", the most frequent keyword was "drug delivery". In recent years, "metastasis" and "diagnosis" appeared in the keyword bursts. This indicates that the application of nanoparticles in the early diagnosis and drug delivery of LC (including liver metastasis) has a good prospect. Conclusion: Nanotechnology has received more and more attention in the medical field in recent years. As nanoparticles are easily localized in organelles and cells, they can increase drug permeability in tumor tissues, improve drug delivery efficiency and reduce drug toxicity. Our research results were the first scientific evaluation of the application of nanotechnology in LC, providing scholars with research hotspots and development trends.
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Pickled eggs enjoy a long processing history with unique flavor and rich nutrition but suffer from long pickling cycle due to the limitations of traditional processing methods. In terms of quality, salted egg whites have the disadvantage of high sodium content, and salted egg yolks have problems such as hard core and black circle around outer layer. Likewise, the quality of preserved eggs is challenged by the black spots (dots) on the eggshells and the high content of heavy metals in the egg contents. The sustainable development of traditional pickled eggs are hindered by these defects and extensive research has been carried out in recent years. Based on the elaboration of the quality formation mechanism of salted eggs and preserved eggs, this paper reviewed the processing principles and applications of rapid pickling technologies like ultrasonic technology, magnetoelectric-assisted technology, water cycle technology, vacuum decompression technology, and pulsed pressure technology, as well as the quality optimization methods such as controlling the sodium content of the salted egg whites, improving the quality of salted egg yolks, promoting the quality of lead-free preserved eggs, and developing heavy metal-free preserved eggs. In the end, the future development trend of traditional pickled eggs was summarized and prospected in order to provide theoretical guidance for the actual production.
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Pollos , Óvulo , Animales , Yema de Huevo , Clara de Huevo , Sodio , HuevosRESUMEN
The practical viability of high-energy-density lithium-sulfur (Li-S) batteries stipulates the use of a high-loading cathode and lean electrolyte. However, under such harsh conditions, the liquid-solid sulfur redox reaction is much retarded due to the poor sulfur and polysulfides utilization, leading to low capacity and fast fading. Herein, a self-assembled macrocyclic Cu(II) complex (CuL) is designed as an effective catalyst to homogenize and maximize the liquid-involving reaction. The Cu(II) ion coordinated with four N atoms features a planar d sp 2 ${\mathrm{d}}_{{\mathrm{sp}}^{2}}$ hybridization, showing a strong bonding affinity toward lithium polysulfides (LiPSs) along the d z 2 ${\mathrm{d}}_{{z}^{2}}$ orbital via steric effects. Such a structure not only lowers the energy barrier of the liquid-solid conversion (Li2 S4 to Li2 S2 ) but also guides a 3D deposition of Li2 S2 /Li2 S. As such, with a 1 wt% electrolyte additive of CuL, a high initial capacity of 925 mAh g-1 and areal capacity of 9.62 mAh cm-2 with a low decay of 0.3%/cycle can be achieved under a high sulfur loading of 10.4 mg cm-2 and low electrolyte/sulfur ratio of 6 µL mgs -1 . This work is expected to inspire the design of homogenous catalysts and accelerate the uptake of high-energy-density Li-S batteries.