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1.
Nano Lett ; 24(5): 1587-1593, 2024 Feb 07.
Article in English | MEDLINE | ID: mdl-38259044

ABSTRACT

Magnetic skyrmions in bulk materials are typically regarded as two-dimensional structures. However, they also exhibit three-dimensional configurations, known as skyrmion tubes, that elongate and extend in-depth. Understanding the configurations and stabilization mechanism of skyrmion tubes is crucial for the development of advanced spintronic devices. However, the generation and annihilation of skyrmion tubes in confined geometries are still rarely reported. Here, we present direct imaging of skyrmion tubes in nanostructured cuboids of a chiral magnet FeGe using Lorentz transmission electron microscopy (TEM), while applying an in-plane magnetic field. It is observed that skyrmion tubes stabilize in a narrow field-temperature region near the Curie temperature (Tc). Through a field cooling process, metastable skyrmion tubes can exist in a larger region of the field-temperature diagram. Combining these experimental findings with micromagnetic simulations, we attribute these phenomena to energy differences and thermal fluctuations. Our results could promote topological spintronic devices based on skyrmion tubes.

2.
Small ; : e2311650, 2024 May 19.
Article in English | MEDLINE | ID: mdl-38764187

ABSTRACT

Current lithium-ion batteries cannot meet the requirement of higher energy density with further large-scale application of electrical vehicles. Lithium metal batteries combined with Ni-rich layered oxides cathode are expected as the one of promising solutions, while the poor electrode and electrolyte interface impedes the commercial development of lithium metal batteries. A new double-salts super concentrated (DSSC) carbonate electrolyte is proposed to improve the electrochemical performance of LiNi0.90Co0.05Mn0.05O2 (NCM9055)||Li metal battery which exhibits stable cycling performance with the capacity retention of 93.04% and reversible capacity of 173.8 mAh g-1 after 100 cycles at 1 C, while cells with conventional 1 m diluted electrolyte remains only 60.55% and capacity of 114.2 mAh g-1. The double salts synergistic effect in super concentrated electrolyte promotes the formation for more balanced stable cathode electrolyte interface (CEI) inorganic compounds of CFx, LiNOx, SOF2, Li2SO4, and less LiF by X-ray photoelectron spectroscopy (XPS) test, and the uniform 2-3 nm rock-salt phase protection layer on the cathode surface by transmission electron microscope (TEM) characterization, improving the cycling performance of the Ni-rich NCM9055 layered oxide cathode. The DSSC electrolyte also can relief the Li dendrite growth on Li metal anode, as well as exhibit better flame retardance, promoting the application of more safety Ni-rich NCM9055||Li metal batteries.

3.
Small ; 20(1): e2305030, 2024 Jan.
Article in English | MEDLINE | ID: mdl-37649169

ABSTRACT

Vanadium-based oxides have attracted much attention because of their rich valences and adjustable structures. The high theoretical specific capacity contributed by the two-electron-transfer process (V5+ /V3+ ) makes it an ideal cathode material for aqueous zinc-ion batteries. However, slow diffusion kinetics and poor structural stability limit the application of vanadium-based oxides. Herein, a strategy for intercalating organic matter between vanadium-based oxide layers is proposed to attain high rate performance and long cycling life. The V3 O7 ·H2 O is synthesized in situ on the carbon cloth to form an open porous structure, which provides sufficient contact areas with electrolyte and facilitates zinc ion transport. On the molecular level, the added organic matter p-aminophenol (pAP) not only plays a supporting role in the V3 O7 ·H2 O layer, but also shows a regulatory effect on the V5+ /V4+ redox process due to the reducing functional group on pAP. The novel composite electrode with porous structure exhibits outstanding reversible specific capacity (386.7 mAh g-1 , 0.1 A g-1 ) at a high load of 6.5 mg cm-2 , and superior capacity retention of 80% at 3 A g-1 for 2100 cycles.

4.
Small ; 20(5): e2306595, 2024 Feb.
Article in English | MEDLINE | ID: mdl-37732373

ABSTRACT

Iron-based sulfate cathodes of alluaudite Na2+2 δ Fe2- δ (SO4 )3 (NFS) in sodium-ion batteries with low cost, steady cycling performance, and high voltage are promising for grid-scale energy storage systems. However, the poor electronic conductivity and the limited understanding of the phase-evolution of precursors hinder obtaining high-rate capacity and the pure phase. Distinctive NFS@C@n%CNTs (n = 1, 2, 5, 10) sphere-shell conductive networks composite cathode materials are constructed creatively, which exhibit superior reversible capacity and rate performance. In detail, the designed NFS@C@2%CNTs cathode delivers an initial discharge capacity of 95.9 mAh g-1 at 0.05 C and up to 60 mAh g-1 at a high rate of 10 C. The full NFS@C@2%CNTs//HC cell delivers a practical operating voltage of 3.5 V and mass-energy density of 140 Wh kg-1 at 0.1 C, and it can also retain 67.37 mAh g-1 with a capacity retention rate of 96.4% after 200 cycles at 2 C. On the other hand, a novel combination reaction mechanism is first revealed for forming NFS from the mixtures of Na2 Fe(SO4 )2 ·nH2 O (n = 2, 4) and FeSO4 ·H2 O during the sintering process. The inspiring results would provide a novel perspective to synthesize high-performance alluaudite sulfate and analogs by aqueous methods.

5.
Small ; : e2401465, 2024 May 15.
Article in English | MEDLINE | ID: mdl-38750613

ABSTRACT

Lithium (Li) metal batteries have attracted considerable research attention due to their exceptionally high theoretical capacity. However, the commercialization of Li metal batteries faces challenges, primarily attributed to uncontrolled growth of Li dendrites, which raises safety concerns and lowers coulombic efficiency. To mitigate Li dendrites growth and attain dense Li deposition, the hybrid SiO2-Cu2O lithiophilic film applied to a 3D copper foam current collector is developed to regulate the interfacial properties for achieving even and dense Li deposition. The SiO2-Cu2O possesses strong Li+ trapping capability through strong lithiophilicity from Cu2O. Additionally, the SiO2-Cu2O enables uniform ion diffusion through the domain-limiting effect of the holes in the SiO2 layer, inducing an even and dense Li plating/stripping behavior at a large capacity. Furthermore, the SiO2 layer promotes the formation of an initial high inorganic content Solid Electrolyte Interphase (SEI) through selective preferential binding with anion and solvent molecules. When the SiO2-Cu2O@Li anode is coupled with a LiFePO4 (LFP) cathode, the resulting full cell exhibits superior cycling stability and rate performance. These results provide a facile approach to construct a lithiophilic current collector for practical Li metal anodes.

6.
Small ; : e2401089, 2024 May 05.
Article in English | MEDLINE | ID: mdl-38705868

ABSTRACT

With ever-increasing requirements for cathodes in the lithium-ion batteries market, an efficiency and eco-friendly upcycling regeneration strategy is imperative to meet the demand for high-performance cathode materials. Herein, a facile, direct and upcycling regeneration strategy is proposed to restore the failed LiCoO2 and enhance the stability at 4.6 V. Double effects combination of relithiation and outside surface reconstruction are simultaneously achieved via a facile solid-phase sintering method. The evolution process of the Li-supplement and grain-recrystallization is systematically investigated, and the high performance of the upcycled materials at high voltage is comprehensively demonstrated. Thanks to the favorable spinel LiCoxMn2-xO4 surface coating, the upcycled sample displays outstanding electrochemical performance, superior to the pristine cathode materials. Notably, the 1% surface-coated LiCoO2 achieves a high discharge-specific capacity of 207.9 mA h g-1 at 0.1 C and delivers excellent cyclability with 77.0% capacity retention after 300 cycles. Significantly, this in situ created spinel coating layer can be potentially utilized for recycling spent LiCoO2, thus providing a viable, promising recycling strategy insights into the upcycling of degraded cathodes.

7.
Small ; 20(17): e2307615, 2024 Apr.
Article in English | MEDLINE | ID: mdl-38111975

ABSTRACT

Transition metal phosphides (TMPs) have been regarded as the prospective anodes for lithium-ion batteries (LIBs). However, their poor intrinsic conductivity and inevitable large volume variation result in sluggish redox kinetics and the collapse of electrode structure during cycling, which substantially hinders their practical use. Herein, an effective composite electrodes design strategy of "assembly and phosphorization" is proposed to construct synergistic N-doped carbon-encapsulated NiCoP@N-C-based composites, employing a metal-organic frameworks (MOFs) as sacrificial hosts. Serving as the anodes for LIBs, one representative P-NCP-NC-600 electrode exhibits high reversible capacity (858.5 mAh g-1, 120 cycles at 0.1 A g-1) and superior long-cycle stability (608.7 mAh g-1, 500 cycles at 1 A g-1). The impressive performances are credited to the synergistic effect between its unique composite structure, electronic properties and ideal composition, which achieve plentiful lithium storage sites and reinforce the structural architecture. By accompanying experimental investigations with theoretical calculations, a deep understanding in the lithium storage mechanism is achieved. Furthermore, it is revealed that a more ideal synergistic effect between NiCoP components and N-doped carbon frameworks is fundamentally responsible for the realization of superb lithium storage properties. This strategy proposes certain instructive significance toward designable high-performance TMP-based anodes for high-energy density LIBs.

8.
Small ; 20(8): e2305576, 2024 Feb.
Article in English | MEDLINE | ID: mdl-37821400

ABSTRACT

Garnet solid electrolyte Li6.4 La3 Zr1.4 Ta0.6 O12 (LLZTO) is an excellent inorganic ceramic-type solid electrolyte; however, the presence of Li2 CO3 impurities on its surface hinders Li-ion transport and increases the interface impedance. In contrast to traditional methods of mechanical polishing, acid corrosion, and high-temperature reduction for removing Li2 CO3 , herein, a straightforward "waste-to-treasure" strategy is proposed to transform Li2 CO3 into Li3 PO4 and LiF in LiPF6 solution under 60 °C. It is found that the formation of Li3 PO4 during LLZTO pretreatment facilitates rapid Li-ion transport and enhances ionic conductivity, and the LLZTO/PAN composite polymer electrolyte shows the highest Li-ion transference number of 0.63. Additionally, the dense LiF layer serves to safeguard the internal garnet solid electrolyte against solvent decomposition-induced chemical adsorption. Symmetric Li/Li cells assembled with treated LLZTO/PAN composite electrolyte exhibit a critical current density of 1.1 mA cm-2 and a long lifespan of up to 700 h at a current density of 0.2 mA cm-2 . The Li/LiFePO4 solid-state cells demonstrate stable cycling performances for 141 mAh g-1 at 0.5 C, with capacity retention of 93.6% after 190 cycles. This work presents a novel approach to converting waste into valuable resources, offering the advantages of simple processes, and minimal side reactions.

9.
Chemistry ; 30(5): e202303454, 2024 Jan 22.
Article in English | MEDLINE | ID: mdl-37962516

ABSTRACT

The increasing demand for high-energy-density and high-safety energy storage devices has sparked a growing interest in all-solid-state lithium metal batteries (ASSLMBs). A high-quality inorganic solid-state electrolyte (ISE) is a fundamental requirement for ASSLMBs, and an effective ISE/Li interface is a key factor in attaining high-performance ASSLMBs. In this Concept, we initially summarize the challenges encountered by ISE/Li interfaces and delineate four commonly employed strategies for modifying the ISE/Li interface. Then, we explore the merits and drawbacks of coatings utilized as ISE/Li interfacial phases. We also delve into the commonly employed thermal bonding and innovative cold bonding methods utilized for in situ interface preparation. Lastly, we spotlight future directions for enhancing the functionality of ISE/Li interfaces and achieving high-performance ASSLMBs.

10.
Environ Sci Technol ; 58(18): 7782-7790, 2024 May 07.
Article in English | MEDLINE | ID: mdl-38664224

ABSTRACT

No prior studies have linked long-term air pollution exposure to incident sudden cardiac arrest (SCA) or its possible development trajectories. We aimed to investigate the association between long-term exposure to air pollution and SCA, as well as possible intermediate diseases. Based on the UK Biobank cohort, Cox proportional hazard model was applied to explore associations between air pollutants and SCA. Chronic obstructive pulmonary disease (COPD) and major adverse cardiovascular events (MACE) were selected as intermediate conditions, and multistate model was fitted for trajectory analysis. During a median follow-up of 13.7 years, 2884 participants developed SCA among 458 237 individuals. The hazard ratios (HRs) for SCA were 1.04-1.12 per interquartile range increment in concentrations of fine particulate matter, inhalable particulate matter, nitrogen dioxide, and nitrogen oxides. Most prominently, air pollutants could induce SCA through promoting transitions from baseline health to COPD (HRs: 1.06-1.24) and then to SCA (HRs: 1.16-1.27). Less importantly, SCA could be developed through transitions from baseline health to MACE (HRs: 1.02-1.07) and further to SCA (HRs: 1.12-1.16). This study provides novel and compelling evidence that long-term exposure to air pollution could promote the development of SCA, with COPD serving as a more important intermediate condition than MACE.


Subject(s)
Air Pollutants , Air Pollution , Pulmonary Disease, Chronic Obstructive , Pulmonary Disease, Chronic Obstructive/epidemiology , Humans , Male , Female , Particulate Matter , Middle Aged , Heart Arrest/epidemiology , Heart Arrest/chemically induced , Aged , Proportional Hazards Models
11.
Environ Sci Technol ; 58(14): 6226-6235, 2024 Apr 09.
Article in English | MEDLINE | ID: mdl-38557021

ABSTRACT

The updated climate models provide projections at a fine scale, allowing us to estimate health risks due to future warming after accounting for spatial heterogeneity. Here, we utilized an ensemble of high-resolution (25 km) climate simulations and nationwide mortality data from 306 Chinese cities to estimate death anomalies attributable to future warming. Historical estimation (1986-2014) reveals that about 15.5% [95% empirical confidence interval (eCI):13.1%, 17.6%] of deaths are attributable to nonoptimal temperature, of which heat and cold corresponded to attributable fractions of 4.1% (eCI:2.4%, 5.5%) and 11.4% (eCI:10.7%, 12.1%), respectively. Under three climate scenarios (SSP126, SSP245, and SSP585), the national average temperature was projected to increase by 1.45, 2.57, and 4.98 °C by the 2090s, respectively. The corresponding mortality fractions attributable to heat would be 6.5% (eCI:5.2%, 7.7%), 7.9% (eCI:6.3%, 9.4%), and 11.4% (eCI:9.2%, 13.3%). More than half of the attributable deaths due to future warming would occur in north China and cardiovascular mortality would increase more drastically than respiratory mortality. Our study shows that the increased heat-attributable mortality burden would outweigh the decreased cold-attributable burden even under a moderate climate change scenario across China. The results are helpful for national or local policymakers to better address the challenges of future warming.


Subject(s)
Cold Temperature , Hot Temperature , Temperature , Cities , China/epidemiology , Climate Change , Mortality
12.
Environ Res ; 252(Pt 3): 119054, 2024 Jul 01.
Article in English | MEDLINE | ID: mdl-38704007

ABSTRACT

BACKGROUND: The connections between fine particulate matter (PM2.5) and coarse particulate matter (PM2.5-10) and daily mortality of viral pneumonia and bacterial pneumonia were unclear. OBJECTIVES: To distinguish the connections between PM2.5 and PM2.5-10 and daily mortality due to viral pneumonia and bacterial pneumonia. METHODS: Using a comprehensive national death registry encompassing all areas of mainland China, we conducted a case-crossover investigation from 2013 to 2019 at an individual level. Residential daily particle concentrations were evaluated using satellite-based models with a spatial resolution of 1 km. To analyze the data, we employed the conditional logistic regression model in conjunction with polynomial distributed lag models. RESULTS: We included 221,507 pneumonia deaths in China. Every interquartile range (IQR) elevation in concentrations of PM2.5 (lag 0-2 d, 37.6 µg/m3) was associated with higher magnitude of mortality for viral pneumonia (3.03%) than bacterial pneumonia (2.14%), whereas the difference was not significant (p-value for difference = 0.38). An IQR increase in concentrations of PM2.5-10 (lag 0-2 d, 28.4 µg/m3) was also linked to higher magnitude of mortality from viral pneumonia (3.06%) compared to bacterial pneumonia (2.31%), whereas the difference was not significant (p-value for difference = 0.52). After controlling for gaseous pollutants, their effects were all stable; however, with mutual adjustment, the associations of PM2.5 remained, and those of PM2.5-10 were no longer statistically significant. Greater magnitude of associations was noted in individuals aged 75 years and above, as well as during the cold season. CONCLUSION: This nationwide study presents compelling evidence that both PM2.5 and PM2.5-10 exposures could increase pneumonia mortality of viral and bacterial causes, highlighting the more robust effects of PM2.5 and somewhat higher sensitivity of viral pneumonia.


Subject(s)
Air Pollutants , Air Pollution , Cross-Over Studies , Particulate Matter , Particulate Matter/analysis , Particulate Matter/adverse effects , Humans , China/epidemiology , Male , Female , Aged , Middle Aged , Air Pollution/adverse effects , Air Pollution/analysis , Air Pollutants/analysis , Air Pollutants/adverse effects , Pneumonia, Bacterial/mortality , Pneumonia/mortality , Pneumonia/chemically induced , Environmental Exposure/adverse effects , Aged, 80 and over , Particle Size , Pneumonia, Viral/mortality , Adult
13.
Am J Respir Crit Care Med ; 207(5): 602-612, 2023 03 01.
Article in English | MEDLINE | ID: mdl-36170612

ABSTRACT

Rationale: Air pollution has been linked with sleep disturbance in adults, but the association in children remains unclear. Objectives: To examine the associations of prenatal and postnatal exposure to fine particulate matter (particulate matter ⩽2.5 µm in aerodynamic diameter; PM2.5) with sleep quality and sleep disturbances among children in 551 Chinese cities. Methods: A total of 1,15,023 children aged 3-7 years from the Chinese National Cohort of Motor Development were included. Sleep quality was measured using the Children's Sleep Habits Questionnaire (CSHQ). PM2.5 exposure was estimated using a satellite-based model. Generalized additive mixed models with Gaussian and binomial distributions were used to examine the associations of PM2.5 exposure with CSHQ scores and risk of sleep disturbance, respectively, adjusting for demographic characteristics and temporal trends. Measurements and Main Results: Early-life PM2.5 exposure was associated with higher total CSHQ score, and the association was stronger for exposure at age 0-3 years (change of CSHQ score per interquartile range increase of PM2.5 = 0.46; 95% confidence interval [CI], 0.29-0.63) than during pregnancy (0.22; 95% CI, 0.12-0.32). The associations were more evident in sleep-disordered breathing and daytime sleepiness. Postnatal PM2.5 exposure was associated with increased risk of sleep disturbance (adjusted odds ratio for per-interquartile range increase of PM2.5 exposure at age 0-3 years, 1.10; 95% CI, 1.04-1.15), but no associations were found for prenatal exposure. Children who were exclusively breastfed for <6 months and had neonatal ICU admission may be more vulnerable to sleep disturbance related to PM2.5 exposure. Conclusions: PM2.5 exposure can impair sleep quality in preschool children.


Subject(s)
Air Pollutants , Air Pollution , Sleep Wake Disorders , Adult , Female , Pregnancy , Infant, Newborn , Child, Preschool , Humans , Infant , Cities , Particulate Matter/adverse effects , Air Pollution/adverse effects , China , Sleep , Air Pollutants/adverse effects , Environmental Exposure/adverse effects
14.
Ecotoxicol Environ Saf ; 272: 116091, 2024 Mar 01.
Article in English | MEDLINE | ID: mdl-38340600

ABSTRACT

BACKGROUND: Whether and to what extent the impact of exposure to various polychlorinated biphenyls (PCBs) congeners on diabetes, as well as the important contributors, have remained unclear. OBJECTIVE: We aimed to investigate the association patterns between PCBs mixture and diabetes, identify the critical congeners, and explore the potential modifiers. METHODS: The present study included 5900 U.S. adults from the National Health and Nutrition Examination Survey (NHANES) conducted between 2007 and 2016. Weighted logistic regression, restricted cubic spline regression, weighted quantile sum (WQS) regression and Bayesian kernel machine regression (BKMR) were applied to estimate the linear and non-linear associations of single and mixed PCB exposure with diabetes. Subgroup analyses were also conducted to explore potential sex differences. RESULTS: In the weighted logistic regression model, total PCBs were positively associated with diabetes (OR = 1.33, P < 0.025), and significant non-linear associations were observed using RCS analyses. The non-linear positive association between PCBs mixed exposure and diabetes was likewise found in the WQS and BKMR results. PCB180, PCB194, PCB196, and PCB167 were with the highest weights in the WQS, and PCB209 and PCB66 were with the highest posterior inclusion probabilities in the BKMR. Additionally, exposure to total PCBs and most of individual PCB congeners were significantly associated with elevated risk of in females (OR = 1.74; P for trend < 0.001), while fewer significant associations were observed in males. CONCLUSION: The present study highlighted the importance of the long-term surveillance of PCBs and the need to enhance protective measures against them. Notably, these associations were non-linear, congener-specific, and significantly stronger in females than males, especially at relatively high levels of PCBs exposure. Further prospective and mechanistic studies were warranted to ascertain the causal effects between PCBs mixture and diabetes.


Subject(s)
Diabetes Mellitus , Environmental Pollutants , Polychlorinated Biphenyls , Adult , Female , Humans , Male , Polychlorinated Biphenyls/toxicity , Polychlorinated Biphenyls/analysis , Environmental Pollutants/toxicity , Environmental Pollutants/analysis , Environmental Exposure/analysis , Nutrition Surveys , Bayes Theorem , Diabetes Mellitus/epidemiology
15.
Nano Lett ; 23(1): 276-282, 2023 Jan 11.
Article in English | MEDLINE | ID: mdl-36576749

ABSTRACT

The uncontrollable growth of lithium (Li) dendrites and the instability of the Li/electrolyte interface hinder the development of next-generation rechargeable lithium metal batteries. The combination of inorganic nanoparticles and polymers as the artificial SEI layer shows great potential in regulating lithium-ion flux. Here, we design spatially confined LiF nanoparticles in an aligned polymer matrix as the artificial SEI layer. A high dielectric polymer matrix homogenizes the electric field near the surface of lithium metal. Aligned pores with LiF nanoparticles promote the lithium-ion transport across the artificial SEI layer. The synergistic effect of the highly polar ß-phase PVDF and LiF nanoparticles provides high stability over 900 h for the Li//Li symmetrical cell. Besides, a Li//LFP full battery equipped with this artificial layer shows good performance in the commercial carbonate electrolyte, demonstrating the great potential of this protective film in lithium metal batteries.

16.
Nano Lett ; 23(7): 2623-2629, 2023 Apr 12.
Article in English | MEDLINE | ID: mdl-36926919

ABSTRACT

Polymer electrolytes have been studied as an alternative to organic liquid electrolytes but suffer from low ionic conductivity. Propylene carbonate (PC) proves to be an interesting solvent but is incompatible with graphitic anodes due to its cointercalation effect. In this work, adding poly(ethylene oxide) (PEO) into a PC-based electrolyte can alter the solvation structure as well as transform the solution into a polymer electrolyte with high ionic conductivity. By spectroscopic techniques and calculations, we demonstrate that PEO can compete with PC in solvating the Li+ ions, reducing the Li+-PC bond strength, and making it easier for PC to be desolvated. Due to the unique solvation structure, PC-cointercalation-induced graphite exfoliation is inhibited, and the reduction stability of the electrolyte is improved. This work will extend the applications of the PC-based electrolytes, deepen the understandings of the solvation structure, and spur designs of advanced electrolytes.

17.
Angew Chem Int Ed Engl ; 63(25): e202404554, 2024 Jun 17.
Article in English | MEDLINE | ID: mdl-38563638

ABSTRACT

The loss of active materials is one of the main culprits of the battery failures. As a typical example, the presence of inactive lithium, also known as "dead lithium", contributes to the rapid capacity deterioration and reduces energy output in lithium batteries. This phenomenon has long been recognized as irreversible. In this Minireview, the first of this kind, we aim to summarize the formation of inactive lithium and reassess its impact on battery performance metrics. Additionally, we explore various strategies that have been devised to rejuvenate inactive lithium. This comprehensive overview of the latest advancements in reactivating inactive lithium not only offers insights into restoring capacity and enhancing battery performance metrics but also provides a foundation for future research in reviving other inactive materials found in next-generation batteries, such as lithium metal batteries, lithium-sulfur batteries, other alkali metal batteries, and liquid flow batteries.

18.
Angew Chem Int Ed Engl ; 63(25): e202402624, 2024 Jun 17.
Article in English | MEDLINE | ID: mdl-38622075

ABSTRACT

Challenges such as shuttle effect have hindered the commercialization of lithium-sulfur batteries (LSBs), despite their potential as high-energy-density storage devices. To address these issues, we explore the integration of solar energy into LSBs, creating a photo-assisted lithium-sulfur battery (PA-LSB). The PA-LSB provides a novel and sustainable solution by coupling the photocatalytic effect to accelerate sulfur redox reactions. Herein, a perovskite quantum dot-loaded MOF material serves as a cathode for the PA-LSB, creating built-in electric fields at the micro-interface to extend the lifetime of photo-generated charge carriers. The band structure of the composite material aligns well with the electrochemical reaction potential of lithium-sulfur, enabling precise regulation of polysulfides in the cathode of the PA-LSB system. This is attributed to the selective catalysis of the liquid-solid reaction stage in the lithium-sulfur electrochemical process by photocatalysis. These contribute to the outstanding performance of PA-LSBs, particularly demonstrating a remarkably high reversible capacity of 679 mAh g-1 at 5 C, maintaining stable cycling for 1500 cycles with the capacity decay rate of 0.022 % per cycle. Additionally, the photo-charging capability of the PA-LSB holds the potential to compensate for non-electric energy losses during the energy storage process, contributing to the development of lossless energy storage devices.

19.
Angew Chem Int Ed Engl ; 63(28): e202404332, 2024 Jul 08.
Article in English | MEDLINE | ID: mdl-38700477

ABSTRACT

Solid electrolyte interphase (SEI) crucially affects the rate performance and cycling lifespan, yet to date more extensive research is still needed in potassium-ion batteries. We report an ultra-thin and KF-enriched SEI triggered by tuned fluorinated surface design in electrode. Our results reveal that fluorination engineering alters the interfacial chemical environment to facilitate inherited electronic conductivity, enhance adsorption ability of potassium, induce localized surface polarization to guide electrolyte decomposition behavior for SEI formation, and especially, enrich the KF crystals in SEI by self-sacrifice from C-F bond cleavage. Hence, the regulated fluorinated electrode with generated ultra-thin, uniform, and KF-enriched SEI shows improved capacity of 439.3 mAh g-1 (3.82 mAh cm-2), boosted rate performance (202.3 mAh g-1 at 8.70 mA cm-2) and durable cycling performance (even under high loading of ~8.7 mg cm-2). We expect this practical engineering principle to open up new opportunities for upgrading the development of potassium-ion batteries.

20.
Angew Chem Int Ed Engl ; : e202406597, 2024 May 17.
Article in English | MEDLINE | ID: mdl-38757727

ABSTRACT

Artificial interfaces provide a comprehensive approach to controlling zinc dendrite and surface corrosion in zinc-based aqueous batteries (ZABs). However, due to consistent volume changes during zinc plating/stripping, traditional interfacial layers cannot consistently adapt to the dendrite surface, resulting in uncontrolled dendrite growth and hydrogen evolution. Herein, dynamic covalent bonds exhibit the Janus effect towards zinc deposition at different current densities, presenting a holistic strategy for stabilizing zinc anode. The PBSC intelligent artificial interface consisting of dynamic B-O covalent bonds is developed on zinc anode to mitigate hydrogen evolution and restrict dendrite expansion. Owing to the reversible dynamic bonds, PBSC exhibits shape self-adaptive characteristics at low current rates, which rearranges the network to accommodate volume changes during zinc plating/stripping, resisting hydrogen evolution. Moreover, the rapid association of B-O dynamic bonds enhances mechanical strength at dendrite tips, presenting a shear-thickening effect and suppressing further dendrite growth at high current rates. Therefore, the assembled symmetrical battery with PBSC maintains a stable cycle of 4500 hours without significant performance degradation and the PBSC@Zn||V2O5 pouch cell demonstrates a specific capacity exceeding 170 mAh g-1. Overall, the intelligent interface with dynamic covalent bonds provides innovative approaches for zinc anode interfacial engineering and enhances cycling performance.

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