RESUMO
Commercialization of aqueous batteries is mainly hampered by their low energy density, owing to the low mass loading of active cathode materials. In this work, a MnO2 cathode structure (MnO2 /CTF) is designed to modify the MnO2 /collector interface for enhanced ion transportation properties. Such a cathode can achieve ultrahigh mass loading of MnO2 , large areal capacity, and high energy density, with excellent cycling stability and rate performance. Specifically, a 0.15 mm thick MnO2 /CTF cathode can realize a mass loading of 20 mg cm-2 with almost 100% electrochemical conversion of MnO2 , providing the maximum areal capacity of 12.08 mA h cm-2 and energy density of 191 W h kg-1 for Zn-MnO2 /CTF batteries when considering both cathode and anode. Besides the conventional low energy demonstrations, such a Zn-MnO2 /CTF battery is capable of realistic applications, such as mobile phones in our daily life, which is a promising alternative for wearable electronics.
Assuntos
Compostos de Manganês , Óxidos , Zinco , Fontes de Energia ElétricaRESUMO
Potassium-ion batteries (PIBs) are recognized as promising alternatives for lithium-ion batteries as the next-generation energy storage systems. However, the larger radius of K+ hinders the K+ insertion into the conventional carbon electrode and results in sluggish potassiation kinetics and poor cycling stability. Here, nitrogen and fluorine dual doping of soft carbon nanotubes (NFSC) anode are synthesized in one pot, achieving extraordinary electrochemical performance for PIBs. It is demonstrated that NFSC with a doping dose of 5.6 at% nitrogen and 1.3 at% fluorine together exhibits the highest reversible capacity of 238 mAh g-1 at 0.2 A g-1 and cycling stability of 186 mAh g-1 after 1000 cycles at 1 A g-1 . The extraordinary electrochemical performance can be attributed to the hollow structure, expanded interlayer distance, nitrogen and fluorine dual doping, and the binding ability of abundant defect sites. Moreover, density functional theory shows that the extra fluorine modification can dramatically enhance the conventional nitrogen doping effect and reduces the formation energy which makes a great contribution to the improvement of electrical conduction and K-ions insert. This work may promote the development of low-cost and sustainable carbon-based materials for PIBs and other advanced energy storage devices.
RESUMO
Imaging techniques through turbid materials have been extensively studied in recent years. The challenge now is to recover objects in a large field of view with depth-resolving ability. We present a method to image through a thin scattering layer automatically with the depth of the object detectable. By revealing the wavelength-depth-matching relation based on the axial memory effect, this method can automatically search the optimal wavelength of the reference light and compute the depth of the object. The no-reference image quality assessment function and rule-based searching algorithm are used in the searching process. The proposed method is promising for dynamic object tracking.
RESUMO
Metal-organic framework-derived NiCo2.5 S4 microrods wrapped in reduced graphene oxide (NCS@RGO) were synthesized for potassium-ion storage. Upon coordination with organic potassium salts, NCS@RGO exhibits an ultrahigh initial reversible specific capacity (602â mAh g-1 at 50â mA g-1 ) and ultralong cycle life (a reversible specific capacity of 495â mAh g-1 at 200â mA g-1 after 1 900 cycles over 314â days). Furthermore, the battery demonstrates a high initial Coulombic efficiency of 78 %, outperforming most sulfides reported previously. Advanced exâ situ characterization techniques, including atomic force microscopy, were used for evaluation and the results indicate that the organic potassium salt-containing electrolyte helps to form thin and robust solid electrolyte interphase layers, which reduce the formation of byproducts during the potassiation-depotassiation process and enhance the mechanical stability of electrodes. The excellent conductivity of the RGO in the composites, and the robust interface between the electrodes and electrolytes, imbue the electrode with useful properties; including, ultrafast potassium-ion storage with a reversible specific capacity of 402â mAh g-1 even at 2â A g-1 .
RESUMO
Incoherently illuminated or luminescent objects give rise to a low-contrast speckle-like pattern when observed through a thin diffusive medium, as such a medium effectively convolves their shape with a speckle-like point spread function (PSF). This point spread function can be extracted in the presence of a reference object of known shape. Here it is shown that reference objects that are both spatially and spectrally separated from the object of interest can be used to obtain an approximation of the point spread function. The crucial observation, corroborated by analytical calculations, is that the spectrally shifted point spread function is strongly correlated to a spatially scaled one. With the approximate point spread function thus obtained, the speckle-like pattern is deconvolved to produce a clear and sharp image of the object on a speckle-like background of low intensity.
RESUMO
Creating high-performance host materials for potassium (K) metal anodes remains a significant challenge due to the complex preparation process and poor K reversibility. In our work, we developed a potassiophilicity strategy using an oxygen-modified carbon cloth (O-CC) network as a host for K metal anodes. The O-CC network exhibited superior potassiophilic ability, and this improvement was also observed in other carbon hosts using the same process. The oxygen-induced epoxy group in the carbon network regulates interface electrons and enables strong binding of K adatoms through orbital hybridization, resulting in fewer side reactions with the electrolyte and promoting K-ion desolvation and uniform deposition. These factors result in unprecedented stability of the carbon network host, with a long lifespan of over 5500 hours at 0.5 mA cm-2/0.5 mA h cm-2 and 3500 h at 1 mA cm-2/0.5 mA h cm-2 in symmetric cells for K metal anodes, surpassing the cycle life of all previously reported K metal anodes. Furthermore, a high average coulombic efficiency of over 99.3% is demonstrated in O-CC//K cells during 210 cycles. The O-CC also exhibited a stable electrochemical performance, with a capacity retention of 73.3% in full cells coupled with a perylene-3,4,9,10-tetracarboxylic dianhydride cathode. We believe that this new strategy holds great promise for metal anodes in battery applications.
RESUMO
Potassium (K) metal batteries have attracted great attention owing to their low price, widespread distribution, and comparable energy density. However, the arbitrary dendrite growth and side reactions of K metal are attributed to high environmental sensitivity, which is the Achilles' heel of its commercial development. Interface engineering between the current collector and K metal can tailor the surface properties for K-ion flux accommodation, dendrite growth inhibition, parasitic reaction suppression, etc. We have designed bifunctional layers via prepassivation, which can be recognized as an O/F-rich Sn-K alloy and a preformed solid-electrolyte interphase (SEI) layer. This Sn-K alloy with high substrate-related binding energy and Fermi level demonstrates strong potassiophilicity to homogeneously guide K metal deposition. Simultaneously, the preformed SEI layer can effectually eliminate side reactions initially, which is beneficial for the spatially and temporally KF-rich SEI layer on K metal. K metal deposition and protection can be implemented by the bifunctional layers, delivering great performance with a low nucleation overpotential of 0.066 V, a high average Coulombic efficiency of 99.1%, and durable stability of more than 900 h (1 mA cm-2, 1 mAh cm-2). Furthermore, the high-voltage platform, energy, and power densities of K metal batteries can be realized with a conventional Prussian blue analogue cathode. This work provides a paradigm to passivate fragile interfaces for alkali metal anodes.
RESUMO
Aqueous batteries are promising alternatives to non-aqueous lithium-ion batteries due to their safety, environmental impact, and cost-effectiveness. However, their energy density is limited by the narrow electrochemical stability window (ESW) of water. The "Water-in-salts" (WIS) strategy is an effective method to broaden the ESW by reducing the "free water" in the electrolyte, but the drawbacks (high cost, high viscosity, poor low-temperature performance, etc.) also compromise these inherent superiorities. In this review, electrolyte and interphase engineering of aqueous batteries to overcome the drawbacks of the WIS strategy are summarized, including the developments of electrolytes, electrode-electrolyte interphases, and electrodes. First, the main challenges of aqueous batteries and the problems of the WIS strategy are comprehensively introduced. Second, the electrochemical functions of various electrolyte components (e.g., additives and solvents) are summarized and compared. Gel electrolytes are also investigated as a special form of electrolyte. Third, the formation and modification of the electrolyte-induced interphase on the electrode are discussed. Specifically, the modification and contribution of electrode materials toward improving the WIS strategy are also introduced. Finally, the challenges of aqueous batteries and the prospects of electrolyte and interphase engineering beyond the WIS strategy are outlined for the practical applications of aqueous batteries.
RESUMO
Introduction: The treatment response to neoadjuvant immunochemotherapy varies among patients with potentially resectable non-small cell lung cancers (NSCLC) and may have severe immune-related adverse effects. We are currently unable to accurately predict therapeutic response. We aimed to develop a radiomics-based nomogram to predict a major pathological response (MPR) of potentially resectable NSCLC to neoadjuvant immunochemotherapy using pretreatment computed tomography (CT) images and clinical characteristics. Methods: A total of 89 eligible participants were included and randomly divided into training (N=64) and validation (N=25) sets. Radiomic features were extracted from tumor volumes of interest in pretreatment CT images. Following data dimension reduction, feature selection, and radiomic signature building, a radiomics-clinical combined nomogram was developed using logistic regression analysis. Results: The radiomics-clinical combined model achieved excellent discriminative performance, with AUCs of 0.84 (95% CI, 0.74-0.93) and 0.81(95% CI, 0.63-0.98) and accuracies of 80% and 80% in the training and validation sets, respectively. Decision curves analysis (DCA) indicated that the radiomics-clinical combined nomogram was clinically valuable. Discussion: The constructed nomogram was able to predict MPR to neoadjuvant immunochemotherapy with a high degree of accuracy and robustness, suggesting that it is a convenient tool for assisting with the individualized management of patients with potentially resectable NSCLC.
Assuntos
Carcinoma Pulmonar de Células não Pequenas , Neoplasias Pulmonares , Humanos , Terapia Neoadjuvante , Nomogramas , ImunoterapiaRESUMO
Aqueous zinc-ion batteries (ZIBs) are promising candidates for next-generation energy storage systems due to their intrinsic safety, environmental friendliness, and low cost. However, the uncontrollable Zn dendrite growth during cycling is still a critical challenge for the long-term operation of ZIBs, especially under harsh lean-Zn conditions. Herein, we report nitrogen and sulfur-codoped carbon quantum dots (N,S-CDs) as zincophilic electrolyte additives to regulate the Zn deposition behaviors. The N,S-CDs with abundant electronegative groups can attract Zn2+ ions and co-deposit with Zn2+ ions on the anode surface, inducing a parallel orientation of the (002) crystal plane. The deposition of Zn preferentially along the (002) crystal direction fundamentally avoids the formation of Zn dendrites. Moreover, the co-depositing/stripping feature of N,S-CDs under an electric field force ensures the reproducible and long-lasting modulation of the Zn anode stability. Benefiting from these two unique modulation mechanisms, stable cyclability of the thin Zn anodes (10 and 20 µm) at a high depth of discharge (DOD) of 67% and high Zn||Na2V6O16·3H2O (NVO, 11.52 mg cm-2) full-cell energy density (144.98 W h Kg-1) at a record-low negative/positive (N/P) capacity ratio of 1.05 are achieved using the N,S-CDs as an additive in ZnSO4 electrolyte. Our findings not only offer a feasible solution for developing actual high-energy density ZIBs but also provide in-depth insights into the working mechanism of CDs in regulating Zn deposition behaviors.
RESUMO
Vertical and lateral heterostructures consisting of atomically layered two-dimensional (2D) materials exhibit intriguing properties, such as efficient charge/energy transfer, high photoresponsivity, and enhanced photocatalytic activities. However, the controlled fabrication of vertical or lateral heterojunctions on metal substrates remains challenging. Herein, we report a facile and controllable method for selective growth of WS2/MoS2 vertical or lateral heterojunctions on polycrystalline gold (Au) foil by tuning the gas flow rate of hydrogen (H2). We find that lateral growth is favored without H2, whereas vertical growth mode can be switched on by introducing 8-10 sccm H2. In addition, the areal coverage of the WS2/MoS2 vertical heterostructures is tunable in the range of 12-25%. Transmission electron microscopy (TEM) and selected area electron diffraction (SAED) results demonstrate the quality and absence of cross-contamination of the as-grown heterostructures. Furthermore, we investigate the effects of the H2 flow rate on the morphology of the heterostructures. These pave the way to develop unprecedented 2D heterostructures towards applications in (opto)electronic devices.
RESUMO
Background: Neoadjuvant chemoimmunotherapy (NCIO) is more effective than neoadjuvant immunotherapy alone for pathological response in non-small cell lung cancer (NSCLC) patients, but the processes for determining patient suitability for its implementation are not clear. We aimed to identify the most relevant factors and build a convenient model to select NSCLC patients who would benefit most from NCIO. Methods: We retrospectively collected the clinical data of patients with locally advanced NSCLC who received NCIO followed by surgery at our institution between January 2019 and July 2022. Results: A total of 101 eligible stage IIB-IIIC NSCLC patients were included. After NCIO, all patients successfully underwent surgical resection. A total of 46.53% (47/101) of patients achieved pathological complete response (pCR), and 70.30% (71/101) achieved major pathologic response (MPR). Tumor regression rate (adjusted odds ratio OR = 12.33), PD-L1 expression (adjusted odds ratio (OR) = 9.66), pembrolizumab/nab-paclitaxel-based regimens (adjusted OR = 4.92), and comorbidities (adjusted OR = 0.16) were independently associated with pCR rate (all P < 0.05). Tumor regression rate (adjusted OR = 8.45), PD-L1 expression (adjusted OR = 5.35), and presence of squamous cell carcinoma (adjusted OR = 7.02) were independently associated with MPR rate (all P < 0.05). We established and validated an easy-to-use clinical model to predict pCR (with an area under the curve [AUC] of 0.848) and MPR (with an AUC of 0.847). Of note, the present study showed that CD4+ T-cell count/rate and total cholesterol (TC) and high-density lipoprotein cholesterol (HDL-C) levels in the peripheral blood of pre-NCIO patients were also significantly correlated with pathological response in univariate analyses. Conclusions: The tumor regression rate, PD-L1 expression, pembrolizumab/nab-paclitaxel-based regimens, presence of squamous cell carcinoma, and comorbidities were the main influential factors for incidence of pCR/MPR in patients with stage IIB-IIIC NSCLC in the present study. Through predictive models, we can predict who will benefit most from NCIO prior to the emergence of clinical outcomes in locally advanced NSCLC.
RESUMO
Maintaining the morphology of electrode materials with high invertibility contributes to the prolonged cyclic stability of battery systems. However, the majority of electrode materials tend to degrade during the charge-discharge process owing to the inevitable increase in entropy. Herein, a self-healing strategy is designed to promote morphology rejuvenation in Prussian blue analogue (PBA) cathodes by cobalt doping. Experimental characterization and theoretical calculations demonstrate that a trace amount of cobalt can decelerate the crystallization process and restore the cracked areas to ensure perfect cubic structures of PBA cathodes. The electric field controls the kinetic dynamics, rather than the conventional thermodynamics, to realize the "electrochemically driven dissolution-recrystallization process" for the periodic self-healing phenomenon. The properties of electron transportation and ion diffusion in bulk PBA are also improved by the doping strategy, thus boosting the cyclability with 4000 cycles in a diluent electrolyte. This discovery provides a new paradigm for the construction of self-healing electrodes for cathodes.
RESUMO
Novel monomer, N, N'-bis(acryloyl) cystinamide (NBACA), was designed and synthesized with L-cystine as row material. By using this NBACA both as the monomer and crosslinker, reduction-sensitive nanohydrogel was prepared in ethanol via distillation-precipitation polymerization. The obtained nanohydrogel can provide a relatively hydrophobic environment and hydrogen-bonding sites inside the gel; therefore, it is suitable for loading hydrophobic drug. When paclitaxel that possess poor water-solubility was used as a model drug, the nanohydrogel represented a high drug-loading capacity, and dispersed well in aqueous solutions. Furthermore, the disulfide-group-containing nanohydrogel exhibited good reduction-sensitive drug-release behavior. The nanohydrogel biodegraded rapidly in a reducing environment, and released approximately 80% of the PTX within 24 h. Cytotoxicity assays showed that the PTX-loaded nanohydrogel exhibited high cytotoxicity against MCF-7 breast cancer cells, while blank nanohydrogels displayed a negligible cytotoxicity.
RESUMO
As an emerging group of two-dimensional (2D) layered material, MXenes have received significant attention in the direction of energy storage. However, the restacking of MXene flakes severely hinders the ion transport within electrodes, which limits their application for lithium-ion batteries (LIBs). To address this issue, herein, we rationally designed and optimized the structure of N, S co-doped V2CTx MXene, which exhibits excellent electrochemical performance with a high reversible capacity of 590 mAh g-1 after 100 cycles at 0.1 A g-1 when used as anode of LIBs. Even at a high current density of 2 A g-1, a reversible capacity of 298 mAh g-1 is obtained after 300 cycles, which outperforms most of the V2CTx-based anode materials reported so far. The lithium-ion storage mechanism of N, S co-doped V2CTx MXene was studied by a series of characterizations. The results show that the significant improvement of electrochemical performance should be attributed to the facilitated charge transfer after N and S co-doping in V2CTx MXene, which can effectively improve the ion transfer kinetics during the lithiation-delithiation process. Furthermore, the expanded interlayer spacing of N, S co-doped V2CTx provides more active sites for the adsorption of lithium ions, promoting the insertion capacity of lithium ions. This work indicates that the N, S co-doped 2D V2CTx MXene should be a promising anode material for high-performance LIBs.
RESUMO
Doping is regarded as a prominent strategy to optimize the crystal structure and composition of battery materials to withstand the anisotropic expansion induced by the repeated insertion and extraction of guest ions. The well-known knowledge and experience obtained from doping engineering predominate in cathode materials but have not been fully explored for anodes yet. Here, we propose the practical doping of fluorine ions into the host lattice of nickel oxide to unveil the correlation between the crystal structure and electrochemical properties. Multiple ion transmission pathways are created by the orderly two-dimensional nanosheets, and thus the stress/strain can be significantly relieved with trace fluorine doping, ensuring the mechanical integrity of the active particle and superior electrochemical properties. Density functional theory calculations manifest that the F doping in NiO could improve crystal structural stability, modulate the charge distribution, and enhance the conductivity, which promotes the performance of lithium-ion storage.
RESUMO
The coordinated utilization of nitrogen (N) and phosphorus (P) is vital for plants to maintain nutrient balance and achieve optimal growth. Previously, we revealed a mechanism by which nitrate induces genes for phosphate utilization; this mechanism depends on NRT1.1B-facilitated degradation of cytoplasmic SPX4, which in turn promotes cytoplasmic-nuclear shuttling of PHR2, the central transcription factor of phosphate signaling, and triggers the nitrate-induced phosphate response (NIPR) and N-P coordinated utilization in rice. In this study, we unveiled a fine-tuning mechanism of NIPR in the nucleus regulated by Highly Induced by Nitrate Gene 1 (HINGE1, also known as RLI1), a MYB-transcription factor closely related to PHR2. RLI1/HINGE1, which is transcriptionally activated by PHR2 under nitrate induction, can directly activate the expression of phosphate starvation-induced genes. More importantly, RLI1/HINGE1 competes with PHR2 for binding to its repressor proteins in the nucleus (SPX proteins), and consequently releases PHR2 to further enhance phosphate response. Therefore, RLI1/HINGE1 amplifies the phosphate response in the nucleus downstream of the cytoplasmic SPX4-PHR2 cascade, thereby enabling fine-tuning of N-P balance when nitrate supply is sufficient.
Assuntos
Oryza/metabolismo , Proteínas de Plantas/metabolismo , Núcleo Celular/metabolismo , Regulação da Expressão Gênica de Plantas , Oryza/genética , Proteínas de Plantas/genética , Proteínas Proto-Oncogênicas c-myb/metabolismoRESUMO
On account of the large radius of K-ions, the electrodes can suffer huge deformation during K-ion insertion and extraction processes. In our work, we unveil the impact of using carboxymethyl cellulose (CMC) instead of poly(vinylidene fluoride) (PVDF) as binders for K-ion storage. Our porous hollow carbon submicrosphere anodes using the CMC binder exhibit a reversible capacity of 208 mA h g-1 after 50 cycles at 50 mA g-1, and even at a high current density of 1 A g-1, they achieve a reversible capacity of 111 mA h g-1 over 3000 cycles with almost no decay, demonstrating remarkably improved reversibility and cycling stability than those using PVDF (18 mA h g-1 after 3000 cycles at 1 A g-1). It is showed that the CMC binder can result in higher adhesion force and better mechanical performance than the PVDF binder, which can restrain the crack during a potassiation/depotassiation process. According to the test of adhesion force, the hollow carbon submicrospheres using the CMC binder show above three times of average adhesion force than that using the PVDF binder. Furthermore, based on the rational design, our hollow carbon submicrospheres also exhibit 62.3% specific capacity contribution below 0.5 V vs K/K+ region, which is helpful to design the full cell with high energy density. We believe that our work will highlight the binder effect to improve the K-ion storage performance.
RESUMO
BACKGROUND: This study proposed a mediated moderation model based on the cognitive theory and susceptibility phenotype theory for depression to explore the moderating role of cognitive flexibility in the relationship between trait anxiety and depression and the mediating role of rumination in this interactive effect. METHODS: The subjects were selected via the cluster sampling method. A cross-sectional survey of 1619 Chinese adults of Han nationality was recruited from three cities in central and western China. The trait anxiety subscale of the State-Trait Anxiety Inventory (STAI-Trait scale), Short Ruminative Response Scale (SRRS), Cognitive Flexibility Inventory (CFI) and Beck Depression Inventory (BDI-II) were used for a paper-and-pencil evaluation. The data were statistically processed using correlation analysis, multiple linear regression analysis, and a test of mediated moderation. RESULTS: (1) Trait anxiety was significantly positively correlated with rumination and depression. There was a significant negative correlation between cognitive flexibility and trait anxiety, rumination, and depression. (2) The moderating effect of cognition flexibility on the relationship between trait anxiety and depression was mediated by rumination, and the indirect moderating effect accounted for 79.25% of the total variance. LIMITATIONS: Cross-sectional studies do not reveal the causal relationships between observed variables well. Self-report questionnaires lack objective indicators. The applicability of the current results in the clinical depression population requires further experimental tests. CONCLUSIONS: The results support the important role of trait anxiety in the development of depression. Cognitive flexibility moderates the relationship between trait anxiety and depression and has a risk-buffering effect on this relationship. Rumination plays a mediating role in the moderating effects of cognitive flexibility on the relationship between trait anxiety and depression. The findings enrich the research on the relationship between trait anxiety and depression and have important practical implications for the early prevention and intervention of depression, which can increase individual cognitive flexibility and address rumination to regulate depression.
Assuntos
Ansiedade/psicologia , Cognição , Depressão/psicologia , Personalidade , Adolescente , Adulto , China , Estudos Transversais , Feminino , Humanos , Masculino , Pessoa de Meia-Idade , Escalas de Graduação Psiquiátrica , Análise de Regressão , Ruminação Cognitiva , Autorrelato , Inquéritos e Questionários , Adulto JovemRESUMO
This study aimed to explore the potential moderating effect of mindfulness and its facets on the relationships among perceived stress and mental health outcomes (burnout, depression, anxiety, and subjective well-being) among Chinese intensive care nurses. A total of 500 Chinese intensive care nurses completed self-report measures of mindfulness, burnout syndromes, perceived stress, depression, anxiety, and subjective well-being. Correlation and hierarchical multiple regressions were applied for data analysis. Mindfulness moderated the effects of perceived stress on emotional exhaustion (the core component of burnout syndrome), depression, anxiety, positive affect, and negative affect but not on the other two dimensions of burnout and life satisfaction. Further analyses indicated that the ability to act with awareness was particularly crucial in improving the effects of perceived stress on depression. These results further broaden our understanding of the relationships between perceived stress and burnout, depression, anxiety, and subjective well-being by demonstrating that mindfulness may serve as a protective factor that alleviates or eliminates the negative effects of perceived stress on depression, anxiety, burnout syndrome, and subjective well-being and may instigate further research into targeted mindfulness interventions for Chinese intensive care nurses.