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1.
Small ; : e2404879, 2024 Aug 05.
Article in English | MEDLINE | ID: mdl-39101287

ABSTRACT

Traditional ethylene carbonate (EC)-based electrolytes constrain the applications of silicon carbon (Si-C) anodes under fast-charging and low-temperature conditions due to sluggish Li+ migration kinetics and unstable solid electrolyte interphase (SEI). Herein, inspired by the efficient water purification and soil stabilization of aquatic plants, a stable SEI with a 3D desolvation interface is designed with gel polymer electrolyte (GPE), accelerating Li+ desolvation and migration at the interface and within stable SEI. As demonstrated by theoretical simulations and experiment results, the resulting poly(1,3-dioxolane) (PDOL), prepared by in situ ring-opening polymerization of 1,3-dioxolane (DOL), creates a 3D desolvation area, improving the Li+ desolvation at the interface and yielding an amorphous GPE with a high Li+ ionic conductivity (5.73 mS cm-1). Furthermore, more anions participate in the solvated structure, forming an anion-derived stable SEI and improving Li+ transport through SEI. Consequently, the Si-C anode achieves excellent rate performance with GPE at room temperature (RT) and low temperature (-40 °C). The pouch full cell coupled with LiFePO4 cathode obtains 97.42 mAh g-1 after 500 cycles at 5 C/5 C. This innovatively designed 3D desolvation interface and SEI represent significant breakthroughs for developing fast-charging and low-temperature batteries.

2.
Heliyon ; 10(15): e34883, 2024 Aug 15.
Article in English | MEDLINE | ID: mdl-39144935

ABSTRACT

The indoor thermal environment has a direct impact on human thermal comfort and health. In order to assess the status of the indoor thermal environment of typical sports buildings in hot summer and cold winter climate zones in China, 14 badminton halls in 10 cities in Hubei Province (including 5 venues in Wuhan) in this climate zone are chosen as research objects for field testing of indoor thermal environment parameters in 4 seasons. All the tested stadiums are naturally ventilated in non-event conditions. The results reveal that the average indoor temperature of badminton halls in summer is excessively high (i.e., 31.89 °C), which is higher than the regulation specified in JGJ31-2003 or GB-T18883-2022 on the reference interval of the indoor air temperature of venues in summer, (i.e., (26-28 °C) or (22-28 °C), respectively). The average indoor temperature of badminton halls in winter is too low (i.e., 12.95 °C), and it is lower than the recommendations of JGJ31-2003 or GB-T18883-2022 on the reference interval of the indoor air temperature of venues in winter (i.e., (16-18 °C) or (16-24 °C), respectively), relative humidity and air velocity are in the thermal comfort interval for all seasons, and the indoor thermal environment factors of badminton courts in spring and autumn meet the comfort requirements. The indoor and outdoor temperatures and the relative humidity of badminton courts are highly correlated. The indoor temperature and relative humidity vary according to changes in those factors outdoors, whereas the air velocity is not affected by outdoor changes. In the hot summer and cold winter climate zones, some discrepancies in the indoor temperature variation patterns of badminton halls at various altitudes are detectable. The results of this study aim to provide a solid basis for the development of indoor thermal-comfort standards for sports stadiums in China.

3.
BMC Complement Med Ther ; 24(1): 304, 2024 Aug 14.
Article in English | MEDLINE | ID: mdl-39143580

ABSTRACT

OBJECTIVE: Traditional Chinese exercises (Taichi, Wuqinxi, Liuzijue, and Baduanjin) are considered effective alternative treatments for improving symptoms in the stable phase of COPD. However, the most effective exercise remains unknown. This study compared the effectiveness of different traditional Chinese exercises on pulmonary function in patients with stable chronic obstructive pulmonary disease (COPD) using a network meta-analysis. METHODS: From database establishment until September 2023, eligible randomized controlled trials (RCTs) were searched. Two reviewers performed the risk of bias assessment of the included studies using the Cochrane Collaboration tool, and the evidence level was suggested using the GRADE system. RESULTS: Fifty-seven studies comprising 4294 patients were included. The results of the network meta-analysis show that Baduanjin was most effective in improving the forced expiratory volume in the first second (FEV1). However, Liuzijue significantly improved the first-second forced vital capacity percentage of expected value (FEV1%) and the ratio of the forced expiratory volume in the first second to the forced vital capacity (FEV1/FVC). The probability ranking results indicated that Liuzijue was the most effective, followed by Baduanjin, Wuqinxi, and Taichi. Subgroup analysis in conjunction with intervention duration revealed that Liuzijue had a significant advantage over other interventions for improving FEV1, FEV1%, and FEV1/FVC within 6 months and improved FEV1% and FEV1/FVC for ≥ 6 months. Moreover, Subgroup analysis based on baseline pulmonary function revealed that Liuzijue had a significant advantage over other interventions for improving FEV1% within severe and moderate groups. Finally, Subgroup analysis based on the frequency of interventions showed that Liuzijue was still more effective in improving FEV1, FEV1%, and FEV1/FVC in the ≥ three times one week. CONCLUSION: Liuzijue was more effective than Taichi, Wuqinxi, Liuzijue, and Baduanjin in improving pulmonary function in patients with stable COPD.


Subject(s)
Network Meta-Analysis , Pulmonary Disease, Chronic Obstructive , Pulmonary Disease, Chronic Obstructive/therapy , Pulmonary Disease, Chronic Obstructive/physiopathology , Humans , Exercise Therapy/methods , Randomized Controlled Trials as Topic , Medicine, Chinese Traditional/methods , Respiratory Function Tests , Forced Expiratory Volume , East Asian People
4.
Nanotechnology ; 35(43)2024 Aug 09.
Article in English | MEDLINE | ID: mdl-39074485

ABSTRACT

Solution-processed perovskite solar cells (PSCs) have demonstrated a tremendous growth in power conversion efficiency (PCE). A high-quality, defect-free perovskite-based active layer is a key point to enhance PSC performance. Introduction of additives and interlayers have proved to be an effective tool to passivate surface defects, control crystal growth, and improve PSC stability. Antisolvent engineering has emerged recently as a new approach, which aims to adjust perovskite layer properties and enhance the PCE and stability of PSC devices. Here, we demonstrate that carbon dots (CDs) may serve as a prospective additive for antisolvent engineering. Nitrogen-rich amphiphilic CDs were synthesized from amines by a solvothermal method and used as an additive to chlorobenzene for a perovskite layer fabrication. The interaction between perovskite and functional groups in CDs promotes improved crystallization of an active perovskite layer and defects passivation, bringing higher PSCs efficiency, stability, and suppressed hysteresis. Under optimized CD concentration, the maximum PCE increased by 34% due to the improved short-circuit current and fill factor, and the device maintains 87% of its initial efficiency after 6 d of storage under ambient conditions.

5.
J Am Chem Soc ; 146(29): 20291-20299, 2024 Jul 24.
Article in English | MEDLINE | ID: mdl-39011658

ABSTRACT

Carbon is commonly used as an electrode material for supercapacitors operating on an electrical double-layer energy storage mechanism. However, the low specific capacitance limits its application. Increasing the specific surface area is by far the most common expansion method, and surprisingly, they are not always positively correlated. The overmuch specific surface will show the characteristics of nanoconfinement, and the potential synergistic enhancement mechanism of various key parameters is still controversial. In this work, carbon fiber electrodes with different ultramicropore structures were designed in order to improve the utilization rate and the discharge capacitance. It has been found that when the ultramicropore entrance's surface is too small, it will lead to the decrease of the external charge of the pore transport channel, and then, the selectivity of the opposite ions will decrease. The numerical simulation based on Poisson and Nernst-Planck equations also indicates that ions have difficulty diffusing into the micropores when their entrance surface decreases. Surface properties within the nanocontainment space become critical factors influencing ion transport and adsorption. The specific discharge capacitance of carbon fiber is increased from 3 to 1430 mF cm-2.

6.
Int J Surg ; 110(8): 5007-5021, 2024 Aug 01.
Article in English | MEDLINE | ID: mdl-38978471

ABSTRACT

The presence of tertiary lymphoid structures (TLSs) associated with distinct treatment efficacy and clinical prognosis has been identified in various cancer types. However, the mechanistic roles and clinical implications of TLSs in genitourinary (GU) cancers remain incompletely explored. Despite their potential role as predictive markers described in numerous studies, it is essential to comprehensively evaluate the characteristics of TLSs, including drivers of formation, structural foundation, cellular compositions, maturation stages, molecular features, and specific functionality to maximize their positive impacts on tumor-specific immunity. The unique contributions of these structures to cancer progression and biology have fueled interest in these structures as mediators of antitumor immunity. Emerging data are trying to explore the effects of therapeutic interventions targeting TLSs. Therefore, a better understanding of the molecular and phenotypic heterogeneity of TLSs may facilitate the development of TLSs-targeting therapeutic strategies to obtain optimal clinical benefits for GU cancers in the setting of immunotherapy. In this review, the authors focus on the phenotypic and functional heterogeneity of TLSs in cancer progression, current therapeutic interventions targeting TLSs and the clinical implications and therapeutic potential of TLSs in GU cancers.


Subject(s)
Tertiary Lymphoid Structures , Urogenital Neoplasms , Humans , Tertiary Lymphoid Structures/immunology , Urogenital Neoplasms/therapy , Urogenital Neoplasms/immunology , Urogenital Neoplasms/pathology , Immunotherapy/methods
7.
Front Bioeng Biotechnol ; 12: 1364095, 2024.
Article in English | MEDLINE | ID: mdl-38974657

ABSTRACT

Objective: The purpose of this study is to analyze the inherent relationship between the score values and the biomechanical characteristics of the forward kicking motion, we aim to identify the fundamental variables influencing the score values of the forward kicking motion and establish the key biomechanical factors that effectively trigger scoring in the forward kicking motion. Methods: The DaeDo electronic scoring system was used with the Vicon optical motion capture system and the Kistler 3D force platform to obtain kinematic and kinetic variables of the front roundhouse kick motion. Linear bivariate correlation analysis and principal component analysis were used to analyze the associations between kinematic, kinetic variables, and scoring values, and summarize key biomechanical factors for effectively scoring. Results: The peak ankle plantar flexion angle and knee extension torque of the kicking leg showed a significant negative correlation with scoring values (r < 0, p < 0.05), while other variables showed no statistical significance. The peak knee flexion angle and hip extension angular velocity of the supporting leg showed a significant positive correlation with scoring values (r > 0, p < 0.01), while the peak ankle plantar flexion torque showed a significant negative correlation with scoring values (r < 0, p < 0.05), and other variables showed no statistically significant correlation. The absolute values of eigenvectors of the first and second principal components, which included hip angular velocity, ankle angle, knee torque, and hip torque, were relatively large, indicating their strong influence on effective scoring triggering. Conclusion: Maintaining ankle dorsiflexion and a larger knee flexion angle in the kicking leg is favorable for triggering scoring. Higher knee flexion angle and hip extension angular velocity in the supporting leg are also advantageous for triggering scoring. "Body posture" and "Strength" are key factors that effectively trigger scoring.

8.
J Colloid Interface Sci ; 676: 177-185, 2024 Jul 15.
Article in English | MEDLINE | ID: mdl-39024818

ABSTRACT

The pentlandite Fe5Ni4S8(abbreviated as FNS) is not efficient for water splitting because of its inferior performance for the oxygen evolution reaction (OER). This issue originates from the low activity and instability of FNS during the OER process but can be solved through appropriate doping. Herein, a P-doping strategy based on annealing in the presence of NaH2PO2as a phosphorus source upstream was employed on FNS to enhance its activity and stability toward OER. The results demonstrated fine-tuned electronic structures of Fe and Ni in FNS through P-doping, resulting in suppressed Fe leaching,improved electrical conductivity of FNS, and easier formation of NiOOH on the surface of the catalyst. In turn, these features enhanced the OER activity and stability. The optimal P-doped FNS catalyst FNSP-40 exhibited a 4-fold greater electrochemical surface area compared to that of FNS, accompanied by an overpotential of 235 mV at 10 mA cm-2. The optimized FNSP-40 catalyst was used as an anode, and platinum-decorated FNS was used as a cathode. This combination demonstrated an electrolysis performance with a cell voltage of 1.57 V, reaching a current density of 100 mA cm-2,which indicates efficient operation. The advantages of P-doping engineering were also verified in simulated seawater with enhanced OER performance. Overall, the proposed strategy looks promising for the fabrication of pentlandite-structured catalysts for efficient alkaline water and seawater oxidation.

9.
PLoS One ; 19(7): e0307478, 2024.
Article in English | MEDLINE | ID: mdl-39042660

ABSTRACT

This study investigated the application of artificial intelligence in real-time prediction of professional basketball games, identifying the variations within performance indicators that are critical in determining the outcomes of the games. Utilizing games data from the NBA seasons 2021 to 2023 as the sample, the study constructed a real-time predictive model for NBA game outcomes, integrating the machine learning XGBoost and SHAP algorithms. The model simulated the prediction of game outcomes at different time of games and effectively quantified the analysis of key factors that influenced game outcomes. The study's results demonstrated that the XGBoost algorithm was highly effective in predicting NBA game outcomes. Key performance indicators such as field goal percentage, defensive rebounds, and turnovers were consistently related to the outcomes at all times during the game. In the first half of the game, assists were a key indicator affecting the outcome of the game. In the second half of the games, offensive rebounds and three-point shooting percentage were key indicators affecting the outcome of the games. The performance of the real-time prediction model for NBA game outcomes, which integrates machine learning XGBoost and SHAP algorithms, is found to be excellent and highly interpretable. By quantifying the factors that determine victory, it is able to provide significant decision support for coaches in arranging tactical strategies on the court. Moreover, the study provides reliable data references for sports bettors, athletes, club managers, and sponsors.


Subject(s)
Algorithms , Athletic Performance , Basketball , Machine Learning , Humans
10.
BMC Cancer ; 24(1): 732, 2024 Jun 14.
Article in English | MEDLINE | ID: mdl-38877472

ABSTRACT

BACKGROUND: Considering the age relevance of prostate cancer (PCa) and the involvement of the cGAS-STING pathway in aging and cancer, we aim to classify PCa into distinct molecular subtypes and identify key genes from the novel perspective of the cGAS-STING pathway. It is of significance to guide personalized intervention of cancer-targeting therapy based on genetic evidence. METHODS: The 430 patients with PCa from the TCGA database were included. We integrated 29 key genes involved in cGAS-STING pathway and analyzed differentially expressed genes and biochemical recurrence (BCR)-free survival-related genes. The assessments of tumor stemness and heterogeneity and tumor microenvironment (TME) were conducted to reveal potential mechanisms. RESULTS: PCa patients were classified into two distinct subtypes using AURKB, TREX1, and STAT6, and subtype 1 had a worse prognosis than subtype 2 (HR: 21.19, p < 0.001). The findings were validated in the MSKCC2010 cohort. Among subtype 1 and subtype 2, the top ten mutation genes were MUC5B, DNAH9, SLC5A10, ZNF462, USP31, SIPA1L3, PLEC, HRAS, MYOM1, and ITGB6. Gene set variation analysis revealed a high enrichment of the E2F target in subtype 1, and gene set enrichment analysis showed significant enrichment of base excision repair, cell cycle, and DNA replication in subtype 1. TME evaluation indicated that subtype 1 had a significantly higher level of T cells follicular helper and a lower level of plasma cells than subtype 2. CONCLUSIONS: The molecular subtypes mediated by the cGAS-STING pathway and the genetic risk score may aid in identifying potentially high-risk PCa patients who may benefit from pharmacologic therapies targeting the cGAS-STING pathway.


Subject(s)
Membrane Proteins , Nucleotidyltransferases , Prostatic Neoplasms , Signal Transduction , Humans , Male , Nucleotidyltransferases/genetics , Nucleotidyltransferases/metabolism , Prostatic Neoplasms/genetics , Prostatic Neoplasms/pathology , Prostatic Neoplasms/metabolism , Membrane Proteins/genetics , Membrane Proteins/metabolism , Signal Transduction/genetics , Prognosis , Tumor Microenvironment/genetics , Tumor Microenvironment/immunology , Gene Expression Regulation, Neoplastic , Biomarkers, Tumor/genetics , Mutation , Aged , Gene Expression Profiling , Transcriptome
11.
Nano Lett ; 24(21): 6410-6416, 2024 May 29.
Article in English | MEDLINE | ID: mdl-38767286

ABSTRACT

CsPbI3 perovskite quantum dots (QDs) could achieve pure-red emission by reducing their size, but the increased exciton binding energy (EB) and surface defects for the small-sized QDs (SQDs) cause severe Auger and trap recombinations, thus worsening their electroluminescence (EL) performance. Herein, we utilize the dangling bonds of the SQDs as a driving force to accelerate KI dissolution to solve its low solubility in nonpolar solvents, thereby allowing K+ and I- to bond to the surface of SQDs. The EB of the SQDs was decreased from 305 to 51 meV because of the attraction of K+ to electrons, meanwhile surface vacancies were passivated by K+ and I-. The Auger and trap recombinations were simultaneously suppressed by this difunctional ligand. The SQD-based light-emitting diode showed a stable pure-red EL peak of 639 nm, an external quantum efficiency of 25.1% with low roll-off, and a brightness of 5934 cd m-2.

12.
Nano Lett ; 24(23): 7012-7018, 2024 Jun 12.
Article in English | MEDLINE | ID: mdl-38820129

ABSTRACT

Light management is critical to maximizing the external quantum efficiency of perovskite light-emitting diodes (PeLEDs), but strategies for enhancing light out-coupling are typically complex and expensive. Here, using a facile solvent treatment strategy, we create a layer of lithium fluoride (LiF) nanoislands that serve as a template to reconstruct the light-extracting interfaces for PeLEDs. The nanoisland interface rearranges the near-field light distribution in order to maximize the efficiency of internal light extraction. With the proper adjustment of the nanoisland size and distribution, we have achieved an optimal balance between charge injection and light out-coupling, resulting in bright, pure-red quasi-two-dimensional PeLEDs with a 21.8% peak external quantum efficiency.

13.
J Colloid Interface Sci ; 671: 46-55, 2024 Oct.
Article in English | MEDLINE | ID: mdl-38788423

ABSTRACT

Efficient production of green hydrogen energy is crucial in addressing the energy crisis and environmental concerns. The oxygen evolution reaction (OER) poses a challenge in conventional overall water electrolysis due to its slow thermodynamically process. Urea oxidation reaction (UOR) offers an alternative anodic oxidation method that is highly efficient and cost-effective, with favorable thermodynamics and sustainability. Recently, there has been limited research on bifunctional catalysts that exhibit excellent activity for both OER and UOR reactions. In this study, we developed a selenium and iron co-doped nickel sulfide (SeFe-Ni3S2) catalyst that demonstrated excellent Tafel slopes of 53.9 mV dec-1 and 16.4 mV dec-1 for OER and UOR, respectively. Density Functional Theory (DFT) calculations revealed that the introduction of metal (iron) and nonmetallic elements (selenium) was found to coordinate the d-band center, resulting in improved adsorption/desorption energies of the catalysts and reduced the overpotentials and limiting potentials for OER and UOR, respectively. This activity enhancement can be attributed to the altered electronic coordination structure after the introduction of selenium (Se) and iron (Fe), leading to an increase in the intrinsic activity of the catalyst. This work offers a new strategy for bifunctional catalysts for OER and UOR, presenting new possibilities for the future development of hydrogen production and novel energy conversion technologies. It contributes towards the urgent search for technologies that efficiently produce green hydrogen energy, providing potential solutions to mitigate the energy crisis and protect the environment.

14.
Adv Mater ; 36(29): e2401452, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38723848

ABSTRACT

Nickel-cobalt (NiCo) phosphides (NCPs) possess high electrochemical activity, which makes them promising candidates for electrode materials in aqueous energy storage devices, such as supercapacitors and zinc (Zn) batteries. However, the actual specific capacitance and rate capability of NCPs require further improvement, which can be achieved through reasonable heterostructural design and loading conditions of active materials on substrates. Herein, novel hierarchical Bi-NCP heterogeneous structures with built-in electric fields consisting of bismuth (Bi) interlayers (electrodeposited on carbon cloth (CC)) are designed and fabricated to ensure the formation of uniform high-load layered active materials for efficient charge and ion transport. The resulting CC/Bi-NCP electrodes show a uniform, continuous, and high mass loading (>3.5 mg) with a superior capacitance reaching 1200 F g-1 at 1 A g-1 and 4129 mF cm-2 at 1 mA cm-2 combined with high-rate capability and durable cyclic stability. Moreover, assembled hybrid supercapacitors (HSCs), supercapatteries, and alkaline Zn-ion (AZBs) batteries constructed using these electrodes deliver high energy densities of 64.4, 81.8, and 319.1 Wh kg-1, respectively. Overall, the constructed NCPs with excellent aqueous energy storage performance have the potential for the development of novel transition metal-based heterostructure electrodes for advanced energy devices.

15.
Angew Chem Int Ed Engl ; 63(26): e202403996, 2024 Jun 21.
Article in English | MEDLINE | ID: mdl-38679568

ABSTRACT

Decreasing perovskite nanocrystal size increases radiative recombination due to the quantum confinement effect, but also increases the Auger recombination rate which leads to carrier imbalance in the emitting layers of electroluminescent devices. Here, we overcome this trade-off by increasing the exciton effective mass without affecting the size, which is realized through the trace Cd2+ doping of formamidinium lead bromide perovskite nanocrystals. We observe an ~2.7 times increase in the exciton binding energy benefiting from a slight distortion of the [BX6]4- octahedra caused by doping in the case of that the Auger recombination rate is almost unchanged. As a result, bright color-saturated green emitting perovskite nanocrystals with a photoluminescence quantum yield of 96 % are obtained. Cd2+ doping also shifts up the energy levels of the nanocrystals, relative to the Fermi level so that heavily n-doped emitters convert into only slightly n-doped ones; this boosts the charge injection efficiency of the corresponding light-emitting diodes. The light-emitting devices based on those nanocrystals reached a high external quantum efficiency of 29.4 % corresponding to a current efficiency of 123 cd A-1, and showed dramatically improved device lifetime, with a narrow bandwidth of 22 nm and Commission Internationale de I'Eclairage coordinates of (0.20, 0.76) for color-saturated green emission for the electroluminescence peak centered at 534 nm, thus being fully compliant with the latest standard for wide color gamut displays.

16.
MedComm (2020) ; 5(5): e544, 2024 May.
Article in English | MEDLINE | ID: mdl-38660686

ABSTRACT

There is considerable interest in the potential of stereotactic body radiation therapy (SBRT) combined with systemic therapy such as tyrosine kinase inhibitors (TKIs) or immune checkpoint inhibitors (ICIs). However, its efficacy and safety remain unclear. The purpose of this study was to evaluate the efficacy and safety of conducting SBRT during ICI or TKI treatment in different disease settings for patients with metastatic renal cell carcinoma (mRCC). A total of 16 studies were ultimately included. Under the random effects model, the pooled 1-year local control rate (1-yr LCR) and objective response rate (ORR) were 90% (95% confidence interval [CI]: 80%-95%, I 2 = 67%) and 52% (95% CI: 37%-67%, I 2 = 90%), respectively. SBRT concomitant with different systemic therapy yield significant different 1-yr LCR (p < 0.01) and ORR (p = 0.02). Regarding survival benefits, the pooled 1-year progression-free survival (1-yr PFS) and 1-year overall survival (1-yr OS) rates were 45% (95% CI: 29%-62%, I 2 = 91%) and 85% (95% CI: 76%-91%, I 2 = 66%), respectively. 1-yr PFS and 1-yr OS in different disease settings demonstrated significant difference (p < 0.01). As for toxicity, the pooled incidence of grade 3-4 adverse events was 14% (95% CI: 5%-26%, I 2 = 90%). This study highlights the feasibility of utilizing these strategies in mRCC patients, especially those with a low metastatic tumor burden.

17.
Org Lett ; 26(18): 3951-3956, 2024 May 10.
Article in English | MEDLINE | ID: mdl-38678546

ABSTRACT

Herein, we report a chiral boro-phosphate-catalyzed reductive amination for the desymmetrization of 2,2-disubstituted 1,3-cyclopentadiones with pinacolborane as the reducing agent, delivering chiral ß-amino ketones with an all-carbon quaternary stereocenter in good yields (≤94%), high enantioselectivities (≤97% ee), and excellent diastereoselectivities (>20:1 dr). This reaction has a broad substrate scope and high functional group tolerance. The importance of the chiral products was also demonstrated through the preparation of multifunctional building blocks and heterocycles.

18.
Angew Chem Int Ed Engl ; 63(26): e202405592, 2024 Jun 21.
Article in English | MEDLINE | ID: mdl-38647330

ABSTRACT

In aqueous aluminum-ion batteries (AAIBs), the insertion/extraction chemistry of Al3+ often leads to poor kinetics, whereas the rapid diffusion kinetics of hydronium ions (H3O+) may offer the solution. However, the presence of considerable Al3+ in the electrolyte hinders the insertion reaction of H3O+. Herein, we report how oxygen-deficient α-MoO3 nanosheets unlock selective H3O+ insertion in a mild aluminum-ion electrolyte. The abundant oxygen defects impede the insertion of Al3+ due to excessively strong adsorption, while allowing H3O+ to be inserted/diffused through the Grotthuss proton conduction mechanism. This research advances our understanding of the mechanism behind selective H3O+ insertion in mild electrolytes.

19.
Nat Commun ; 15(1): 3231, 2024 Apr 15.
Article in English | MEDLINE | ID: mdl-38622167

ABSTRACT

Engineering atom-scale sites are crucial to the mitigation of polysulfide shuttle, promotion of sulfur redox, and regulation of lithium deposition in lithium-sulfur batteries. Herein, a homonuclear copper dual-atom catalyst with a proximal distance of 3.5 Å is developed for lithium-sulfur batteries, wherein two adjacent copper atoms are linked by a pair of symmetrical chlorine bridge bonds. Benefiting from the proximal copper atoms and their unique coordination, the copper dual-atom catalyst with the increased active interface concentration synchronously guide the evolutions of sulfur and lithium species. Such a delicate design breaks through the activity limitation of mononuclear metal center and represents a catalyst concept for lithium-sulfur battery realm. Therefore, a remarkable areal capacity of 7.8 mA h cm-2 is achieved under the scenario of sulfur content of 60 wt.%, mass loading of 7.7 mg cm-2 and electrolyte dosage of 4.8 µL mg-1.

20.
Nanoscale ; 16(18): 9011-9020, 2024 May 09.
Article in English | MEDLINE | ID: mdl-38623897

ABSTRACT

Nonlinear absorption of metal-halide perovskite nanocrystals (NCs) makes them an ideal candidate for applications which require multiphoton-excited photoluminescence. By doping perovskite NCs with lanthanides, their emission can be extended into the near-infrared (NIR) spectral region. We demonstrate how the combination of Yb3+ doping and bandgap engineering of cesium lead halide perovskite NCs performed by anion exchange (from Cl- to Br-) leads to efficient and tunable emitters that operate under two-photon excitation in the NIR spectral region. By optimizing the anion composition, Yb3+-doped CsPbClxBr3-x NCs exhibited high values of two-photon absorption cross-section reaching 2.3 × 105 GM, and displayed dual-band emission located both in the visible (407-493 nm) and NIR (985 nm). With a view of practical applications of bio-visualisation in the NIR spectral range, these NCs were embedded into silica microspheres which were further wrapped with amphiphilic polymer shells to ensure their water-compatibility. The resulting microspheres with embedded NCs could be easily dispersed in both toluene and water, while still exhibiting a dual-band emission in visible and NIR under both one- and two-photon excitation conditions.

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