Designing Advanced Electrolytes for High-Safety and Long-Lifetime Sodium-Ion Batteries via Anion-Cation Interaction Modulation.

Safety hazards caused by flammable electrolytes have been major obstacles to the practical application of sodium-ion batteries (SIBs). The adoption of nonflammable all-phosphate electrolytes can effectively improve the safety of SIBs; however, traditional low-concentration phosphate electrolytes are not compatible with carbon-based anodes. Herein, we report an anion-cation interaction modulation strategy to design low-concentration phosphate electrolytes with superior physicochemical properties. Tris(2,2,2-trifluoroethyl) phosphate (TFEP) is introduced as a cosolvent to regulate the ion-solvent-coordinated (ISC) structure through enhancing the anion-cation interactions, forming the stable anion-induced ISC (AI-ISC) structure, even at a low salt concentration (1.22 M). Through spectroscopy analyses and theoretical calculations, we reveal the underlying mechanism responsible for the stabilization of these electrolytes. Impressively, both the hard carbon (HC) anode and Na4Fe2.91(PO4)2(P2O7) (NFPP) cathode work well with the developed electrolytes. The designed phosphate electrolyte enables Ah-level HC//NFPP pouch cells with an average Coulombic efficiency (CE) of over 99.9% and a capacity retention of 84.5% after 2000 cycles. In addition, the pouch cells can operate in a wide temperature range (-20 to 60 °C) and successfully pass rigorous safety testing. This work provides new insight into the design of the electrochemically compatibility electrolyte for high-safety and long-lifetime SIBs.

Cordycepin inhibits kidney injury by regulating GSK-3ß-mediated Nrf2 activation.

We explored the role and mechanism of cordycepin (COR) in inhibiting kidney injury. A mouse model of kidney injury was established using cisplatin (CDDP), and the kidney function, histopathology, and ferroptosis indices in mice were detected after intervening with COR. The targets of COR-ferroptosis-kidney injury were analyzed by network pharmacology, based on which the association between glycogen synthase kinase-3 beta (GSK-3ß) and COR was determined. HK-2 cells were cultured in vitro and treated separately with ferroptosis inducers erastin and CDDP. After the COR intervention, the level of ferroptosis was monitored. In vitro experiments found that COR could inhibit ferroptosis and CDDP-induced kidney injury. Network pharmacological analysis revealed that GSK-3ß was the target of COR. After inhibiting GSK-3ß expression, COR could not further inhibit the occurrence of ferroptosis. In vitro results also indicated that COR could inhibit ferroptosis in HK-2 cells. According to our findings, COR can ameliorate CDDP-induced kidney injury through GSK-3ß-mediated ferroptosis signaling. We identify new pharmacological effect and target for COR, the major component of Cordyceps sinensis.

Cryptotanshinone Inhibits Bladder Cancer Cell Malignant Progression in a Lipopolysaccharide-Induced Inflammatory Microenvironment through NLRP3 Inhibition.

Background: Bladder cancer (BC) is one of the most common malignancies of the urogenital system. This study assessed the nucleotide-binding oligomerization domain and leucine-rich repeat and pyrin domain-containing protein 3 (NLRP3) in BC as well as the effects of cryptotanshinone on changes in BC malignant behaviors and NLRP3 expression under a lipopolysaccharide (LPS)-induced inflammatory microenvironment. Methods: BC tissue specimens from 62 patients were collected for immunohistochemical detection of NLRP3 protein. BC and normal urothelial cell lines were cultured for the detection of NLRP3 mRNA and protein. Then, BC cells were pretreated with LPS to mimic the inflammatory tumor microenvironment. Next, these cells were incubated with a low or high dose of cryptotanshinone to assess its effects on tumor cell malignant behaviors as well as transfected with NLRP3 cDNA to confirm the role of NLRP3 in BC cells in vitro. Results: High NLRP3 expression was associated with larger tumor diameters (>2 cm), muscle invasion, and metastasis. The levels of NLRP3 mRNA and protein were greater in BC cells than in normal urothelial cells. LPS pretreatment significantly promoted NLRP3 and inflammatory cytokine expression in BC cells, and induced cell viability, migration, and invasion. However, cryptotanshinone was able to reduce the LPS-induced increase of NLRP3 and inflammatory cytokine expression as well as the BC cell malignant progression. NLRP3 overexpression using NLRP3 cDNA further promoted BC cell malignant progression after LPS stimulation and reversed cryptotanshinone-reduced LPS-induced BC cell malignant behaviors. Conclusion: NLRP3 might possess oncogenic activity in BC, and the antitumor activity of cryptotanshinone in BC in vitro might be related to its inhibition of NLRP3 expression.

Linkage Engineering in Covalent Organic Frameworks for Metal-Free Electrocatalytic C2H4 Production from CO2.

Electrocatalytic carbon dioxide reduction reaction (CO2RR) to produce ethylene (C2H4) is conducive to sustainable development of energy and environment. At present, most electrocatalysts for C2H4 production are limited to the heavy metal copper, meanwhile, achieving metal-free catalysis remains a challenge. Noted piperazine with sp3 N hybridization is beneficial to CO2 capture, but CO2RR performance and mechanism have been lacking. Herein, based on linkage engineering, we construct a novel high-density sp3 N catalytic array via introducing piperazine into the crystalline and microporous aminal-linked covalent organic frameworks (COFs). Thanks to its high sp3 N density, strong CO2 capture capacity and great hydrophilicity, aminal-linked COF successfully achieves the conversion of CO2 to C2H4 with a Faraday efficiency up to 19.1 %, which is stand out in all reported metal-free COF electrocatalysts. In addition, a series of imine-linked COFs are synthesized and combined with DFT calculations to demonstrate the critical role of sp3 N in enhancing the kinetics of CO2RR. Therefore, this work reveals the extraordinary potential of linkage engineering in COFs to break through some catalytic bottlenecks.

LiNO3 -Based Electrolytes via Electron-Donation Modulation for Sustainable Nonaqueous Lithium Rechargeable Batteries.

LiPF6 as a dominant lithium salt of electrolyte is widely used in commercial rechargeable lithium-ion batteries due to its well-balanced properties, including high solubility in organic solvents, good electrochemical stability, and high ionic conductivity. However, it suffers from several undesirable properties, such as high moisture sensitivity, thermal instability, and high cost. To address these issues, herein, we propose an electron-donation modulation (EDM) rule for the development of low-cost, sustainable, and electrochemically compatible LiNO3 -based electrolytes. We employ high donor-number solvents (HDNSs) with strong electron-donation ability to dissolve LiNO3 , while low donor-number solvents (LDNSs) with weak electron-donation ability are used to regulate the solvation structure to stabilize the electrolytes. As an example, we design the LiNO3 -DMSO@PC electrolyte, where DMSO acts as an HDNS and PC serves as an LDNS. This electrolyte exhibits excellent electrochemical compatibility with graphite anodes, as well as the LiFePO4 and LiCoO2 cathodes, leading to stable cycling over 200 cycles. Through spectroscopy analyses and theoretical calculation, we uncover the underlying mechanism responsible for the stabilization of these electrolytes. Our findings provide valuable insights into the preparation of LiNO3 -based electrolytes using the EDM rule, opening new avenues for the development of advanced electrolytes with versatile functions for sustainable rechargeable batteries.

Aromatic Ketones as Mild Presodiating Reagents toward Cathodes for High-Performance Sodium-Ion Batteries.

Chemical presodiation (CP) is an effective strategy to enhance energy density of sodium ion batteries. However, the sodiation reagents reported so far are basically polycyclic aromatic hydrocarbons (PAHs) wth low reductive potential (~0.1 V vs. Na+ /Na), which could easily cause over-sodiation and structural deterioration of the presodiated cathodes. In this work, Aromatic ketones (AKs) are rationally designed as mild presodiating reagents by introducing a carbonyl group (C=O) into PAHs to balance the conjugated and inductive effect. As the representatives, two compounds 9-Fluorenoneb (9-FN) and Benzophenone (BP) manifest favorable equilibrium potential of 1.55 V and 1.07 V (vs. Na+ /Na), respectively. Note that 9-FN demonstrates versatile presodiating capability toward multiple Na uptake hosts (tunneled Na0.44 MnO2 , layered Na0.67 Ni0.33 Mn0.67 O2 , polyanionic Na4 Fe2.91 (PO4 )2 P2 O7 , Na3 V2 (PO4 )3 and Na3 V2 (PO4 )2 F3 ), enabling greatly improved initial charging capacity of the cathode to balance the irrevisible capacity of the anode. Our results indicate that the Aromatic ketones are competitive presodiating cathodic reagents for high-performance sodium-ion batteries, and will inspire more studies and application attempts in the future.

Correlating the Solvating Power of Solvents with the Strength of Ion-Dipole Interaction in Electrolytes of Lithium-ion Batteries.

The solvation structure of Li+ plays a significant role in determining the physicochemical properties of electrolytes. However, to date, there is still no clear definition of the solvating power of different electrolyte solvents, and even the solvents that preferentially participate in the solvation structure remain controversial. In this study, we comprehensively discuss the solvating power and solvation process of Li+ ions using both experimental characterizations and theoretical calculations. Our findings reveal that the solvating power is dependent on the strength of the Li+ -solvent (ion-dipole) interaction. Additionally, we uncover that the anions tend to enter the solvation sheath in most electrolyte systems through Li+ -anion (ion-ion) interaction, which is weakened by the shielding effect of solvents. The competition between the Li+ -solvent and Li+ -anion interactions ultimately determines the final solvation structures. This insight into the fundamental understanding of the solvation structure of Li+ provides inspiration for the design of multifunctional mixed-solvent electrolytes for advanced batteries.

A light-weight periodic plate with embedded acoustic black holes and bandgaps for broadband sound radiation reduction.

Conceiving lightweight structures with low vibration and sound radiation properties is an important topic. The concept of Acoustic Black Hole (ABH) offers new impetus to tackle this problem. Most existing ABH structures are based on simple ABH cells. Apart from the reduced structural strength, systematic ABH effects occur typically above the cut-on frequency of the ABH element, which is perceived as a bottlenecking problem. To tackle the problem, this paper examines the sound radiation properties of a plate comprising periodically tangled ABH cells. Through combining ABH effects with sub-wavelength bandgaps (BGs), numerical and experimental studies show that the plate exhibits reduced sound radiation properties in an ultra-broad frequency range, far below the cut-on frequency of an ABH element. This is owing to the tangled nature of the ABH elements, which extends the actual dimension of the ABH, lowers its onset frequency and reduces the sound radiation efficiency through creating slow waves. Inside the BGs, the reduced sound radiation is mainly due to the redistribution of the vibration energy, basically confined to the excitation area. Capitalizing on the combined ABH and BG features alongside improved mechanical properties, the proposed structure shows promise as a light-weight solution for broadband noise reduction.

Short-term mortality risks among patients with non-metastatic bladder cancer.

BACKGROUND: Population-based analysis for the short-term non-bladder cancer related mortality among patients with non-metastatic bladder cancer is currently lacking. The objective of the current study was to assess and quantify cause of death after bladder cancer diagnosis. METHODS: The custom Surveillance, Epidemiology, and End Results (SEER) dataset for standardized mortality ratios (SMRs) was utilized to identify 24,074 patients who were diagnosed with nonmetastatic (M0) bladder cancer from 2014 to 2015. SMRs for causes of death were calculated. Risk factors for bladder cancer-specific mortality, competing mortality, second-cancer mortality, and noncancer mortality were determined using either multivariable Cox or competing risk regression models. RESULTS: Among all the 4179 (17.4%) deaths occurred during the follow-up period, almost half of them (44.2%) were attributed to non-bladder cancer cause, including second non-bladder cancer (10%) and other non-cancer causes (34.2%). The most common noncancer causes of death were heart diseases followed by chronic obstructive pulmonary disease. Patients had a higher risk of death from second malignancies (SMR, 1.59; 95% CI, 1.47-1.74) compared with death from first malignancies in the US general population, and also had higher risks of death from heart diseases (SMR, 1.29; 95% CI, 1.18-1.40) and chronic obstructive pulmonary disease (SMR, 1.52; 95% CI, 1.29-1.79) compared with the US general population. Additionally, some risk factors for competing second malignancies or noncancer mortality were determined, such as age, gender, marital status and treatment modalities. CONCLUSIONS: Death from non-bladder cancer cause contributed to almost half of all deaths in bladder cancer survivors during the short-term follow-up period. These findings can inform medical management and assist clinicians in counseling those survivors regarding their short-term health risks.

Translations of spherical harmonics expansion coefficients for a sound field using plane wave expansions.

A translation method for the spherical harmonics expansion coefficients of a sound field using plane wave expansions is proposed. It is based on the decomposition of a plane wave in the spherical harmonics domain and without the use of the spherical harmonics addition theorem, thus is very computationally efficient. Simulations are conducted for validation. The stabilities of the translations are compared with the conventional method in terms of matrix condition numbers. The proposed method is demonstrated to be more robust as the frequency increases and when upscaling the coefficients. Besides, the computation is much faster when high truncated orders are solved.

A perceptual dissimilarities based nonlinear sound quality model for range hood noise.

The application of sound quality in household appliances has gradually increased in recent years. In addition to modeling algorithms, appropriate acoustic metrics that characterize product sounds also play an important role in developing models. In this study, an artificial neural network based sound quality model for range hood noise was established with the combination of prior metric selection by multidimensional scaling (MDS) analysis of perceptual dissimilarities. First, sounds in different environments, speeds, and positions were recorded, and their annoyance was evaluated by grouped anchor semantic differential subjective jury testing. Then, the timbre space underlying dissimilarity judgments were analyzed by CLASCAL, an accurate MDS algorithm. Each dimension of the space was well explained by some metrics through stepwise regression. Finally, a sound quality model was established based on a back propagation neural network (BPNN). Results show that the combination of BPNN and CLASCAL can address the interpretation of the sound quality model and the ability to model nonlinearity for high accuracy. In addition, the application of noise control on range hoods showed that passive and active noise control (ANC) measures improve sound quality, especially ANC systems.

Subwavelength and quasi-perfect underwater sound absorber for multiple and broad frequency bands.

A structure for an underwater sound absorber with subwavelength thickness and a quasi-perfect absorption property at multiple frequency bands is reported. This absorber consists of a viscoelastic coating layer embedded with periodically distributed plate scatterers (PSs). The embedded PSs cannot only slow sound waves in the coating, leading to a down-shifted resonance frequency where the absorption is maximized, but also introduce multiple local bending modes and local longitudinal modes in the coating. Via proper selection of the parameters of the PSs and the PS array, multiple local resonance modes of different types in a coating unit can be excited, resulting in quasi-perfect absorption of incident sound at multiple frequencies whose wavelengths are much longer than the thickness of the coating layer. For example, absorption (89%) of underwater sound at 462.9 Hz is achieved by such a layer with a thickness of 6 cm, which is 1.9% of the wavelength of the incident sound. Broadband quasi-perfect absorption can also be realized by coupling of those multiple local resonant modes. This quasi-perfect absorption property can also be observed for sound waves with different incident angles, because a large number of local intrinsic modes could still be excited.

Sound field reconstruction within an entire cavity by plane wave expansions using a spherical microphone array.

A spherical microphone array has proved effective in reconstructing an enclosed sound field by a superposition of spherical wave functions in Fourier domain. It allows successful reconstructions surrounding the array, but the accuracy will be degraded at a distance. In order to extend the effective reconstruction to the entire cavity, a plane-wave basis in space domain is used owing to its non-decaying propagating characteristic and compared with the conventional spherical wave function method in a low frequency sound field within a cylindrical cavity. The sensitivity to measurement noise, the effects of the numbers of plane waves, and measurement positions are discussed. Simulations show that under the same measurement conditions, the plane wave function method is superior in terms of reconstruction accuracy and data processing efficiency, that is, the entire sound field imaging can be achieved by only one time calculation instead of translations of local sets of coefficients with respect to every measurement position into a global one. An experiment was conducted inside an aircraft cabin mock-up for validation. Additionally, this method provides an alternative possibility to recover the coefficients of high order spherical wave functions in a global coordinate system without coordinate translations with respect to local origins.

Compressive sensing based spherical harmonics decomposition of a low frequency sound field within a cylindrical cavity.

A low frequency sound field within a cylindrical cavity can be well approximated by a sparse set of Fourier-Bessel series in a spherical coordinate system. The approximation accuracy can be guaranteed as long as the series coefficients are well estimated by use of spherical microphone arrays (SMA). Conventional methods like spherical Fourier transform and Helmholtz equation least square require a large number of sensors, and it is difficult to estimate the high order coefficients in the presence of sensor noise. To cope with these issues, compressive sensing (CS) is utilized and compared with the conventional methods. In this study, the estimate of the high order coefficients from contaminated measurements is examined, and the effect of modal behavior is analyzed. Numerical simulations show that sensors can be significantly saved especially for high order cavity modes due to the low sparsity of coefficients which is also stable as the modal frequency increases, and the overall accuracy is also improved. The optimal SMA configuration for the use of CS is studied. A large SMA with omni-microphone deployed by the Fliege sampling scheme is suggested. The CS results are finally validated through the good simulated reconstructions of cylindrical cavity modes.

Low frequency sound spatial encoding within an enclosure using spherical microphone arrays.

In a spherical coordinate system, interior sound field can be expressed in terms of a series of Fourier-Bessel expansions. The process that obtains the expansion coefficients by use of a microphone array (e.g., a spherical microphone array) is called spatial encoding. Until now spatial encoding has mainly been examined in a free field or a diffuse field which can be modeled as a sum of plane waves. For spatial encoding within an enclosure at low frequencies, special challenges would be encountered in two aspects. First, the expansions are influenced by array configurations. Second, an acoustic mode based model instead of a plane wave based one should be considered. This study focuses on these challenges. Different kinds of array configurations were compared specifically at low frequencies, and the spatial encoding for the cylindrical cavity modes was investigated. It was found that the spherical array with cardioid microphones was optimal when kr<1, the cavity modes can be effectively represented by only a sparse subset of expansion coefficients and a good reproduction can be achieved even outside the spherical valid region, which demonstrates an effective alternative way to describe the cylindrical cavity modes and can be implemented efficiently in practice.

Performance and strategy comparisons of human listeners and logistic regression in discriminating underwater targets.

To improve the design of underwater target recognition systems based on auditory perception, this study compared human listeners with automatic classifiers. Performances measures and strategies in three discrimination experiments, including discriminations between man-made and natural targets, between ships and submarines, and among three types of ships, were used. In the experiments, the subjects were asked to assign a score to each sound based on how confident they were about the category to which it belonged, and logistic regression, which represents linear discriminative models, also completed three similar tasks by utilizing many auditory features. The results indicated that the performances of logistic regression improved as the ratio between inter- and intra-class differences became larger, whereas the performances of the human subjects were limited by their unfamiliarity with the targets. Logistic regression performed better than the human subjects in all tasks but the discrimination between man-made and natural targets, and the strategies employed by excellent human subjects were similar to that of logistic regression. Logistic regression and several human subjects demonstrated similar performances when discriminating man-made and natural targets, but in this case, their strategies were not similar. An appropriate fusion of their strategies led to further improvement in recognition accuracy.

Down-film as a new non-frame porous material for sound absorption.

Down-polyethylene film material has been introduced for the first time as an excellent non-frame sound absorber, showing a distinctively outstanding performance. It contains down fiber adjacent to each other without firm connection in between, forming a structure of elastic fiber network. The unique structure has broadband response to sound wave, showing non-synchronous vibration in low and middle frequency and synchronous vibration in middle and high frequency. The broadband resonance in middle and high frequency allows the structure to achieve complete sound absorption in resonance frequency band. Moreover, down-polyethylene film material possesses forced vibration, corresponding sound absorption coefficient has been obtained based on vibration theory. The down-film sound absorption material has the characteristics of light weight, soft, environment-friendly, and has excellent broadband sound absorption performance.

Enabling Ultralow-Temperature (-70 °C) Lithium-Ion Batteries: Advanced Electrolytes Utilizing Weak-Solvation and Low-Viscosity Nitrile Cosolvent.

Low-temperature performance of lithium-ion batteries (LIBs) has always posed a significant challenge, limiting their wide application in cold environments. In this work, the high-performance LIBs working under ultralow-temperature conditions, which is achieved by employing the weak-solvation and low-viscosity isobutyronitrile as a cosolvent to tame the affinity between solvents and lithium ions, is reported. The as-prepared electrolytes exhibit a sufficiently high conductivity (1.152 mS cm-1 ) at -70 °C. The electrolytes enable LiCoO2 cathode and graphite anode to achieve high Coulombic efficiency of >99.9% during long-term cycling at room temperature, and to respectively achieve 75.8% and 100.0% of their room-temperature capacities at -40 °C. Even the LiCoO2 //graphite pouch cells can retain 68.7% of the room-temperature capacity when discharged at -70 °C, and present stable cycling performance at -40 and 60 °C. This work provides a solution for the development of advanced electrolytes to enable LIBs working at wide-temperatures range.

Spatio-Temporal Point Process for Multiple Object Tracking.

Multiple object tracking (MOT) focuses on modeling the relationship of detected objects among consecutive frames and merge them into different trajectories. MOT remains a challenging task as noisy and confusing detection results often hinder the final performance. Furthermore, most existing research are focusing on improving detection algorithms and association strategies. As such, we propose a novel framework that can effectively predict and mask-out the noisy and confusing detection results before associating the objects into trajectories. In particular, we formulate such "bad" detection results as a sequence of events and adopt the spatio-temporal point process to model such events. Traditionally, the occurrence rate in a point process is characterized by an explicitly defined intensity function, which depends on the prior knowledge of some specific tasks. Thus, designing a proper model is expensive and time-consuming, with also limited ability to generalize well. To tackle this problem, we adopt the convolutional recurrent neural network (conv-RNN) to instantiate the point process, where its intensity function is automatically modeled by the training data. Furthermore, we show that our method captures both temporal and spatial evolution, which is essential in modeling events for MOT. Experimental results demonstrate notable improvements in addressing noisy and confusing detection results in MOT data sets. An improved state-of-the-art performance is achieved by incorporating our baseline MOT algorithm with the spatio-temporal point process model.

Revealing the structural chemistry in Na6-2xFex(SO4)3 (1.5 ≤ x ≤ 2.0) for low-cost and high-performance sodium-ion batteries.

Fe-based polyanionic sulfate materials are one of the most promising candidates for large-scale applications in sodium-ion batteries due to their low cost and excellent electrochemical performance. Although great achievements have been gained on a series of Na6-2xFex(SO4)3 (NFSO-x, 1.5 ≤ x ≤ 2.0) materials such as Na2Fe2(SO4)3, Na2Fe1.5(SO4)3, and Na2.4Fe1.8(SO4)3 for sodium storage, the phase and structure characteristics on these NFSO-x are still controversial, making it difficult to achieve phase-pure materials with optimal electrochemical properties. Herein, six NFSO-x samples with varied x are investigated via both experimental methods and density functional theory calculations to analyze the phase and structure properties. It reveals that a pure phase exists in the 1.6 ≤ x ≤ 1.7 region of the NFSO-x, and part of Na ions tend to occupy Fe sites to form more stable frameworks. The NFSO-1.7 exhibits the best electrochemical performance among the NFSO-x samples, delivering a high discharge capacity (104.5 mAh g-1 at 0.1 C, close to its theoretical capacity of 105 mAh g-1), excellent rate performance (81.5 mAh g-1 at 30 C), and remarkable cycle stability over 10,000 cycles with high-capacity retention of 72.4%. We believe that the results are useful to clarify the phase and structure characteristics of polyanionic materials to promote their application for large-scale energy storage.