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1.
Nano Lett ; 23(8): 3181-3188, 2023 Apr 26.
Artículo en Inglés | MEDLINE | ID: mdl-37036714

RESUMEN

Sluggish desolvation in extremely cold environments caused by strong Li+-dipole interactions is a key inducement for the capacity decline of a battery. Although the Li+-dipole interaction is reduced by increasing the electrolyte concentration, its high viscosity inevitably limits ion transfer at low temperatures. Herein, Li+-dipole interactions were eliminated to accelerate the migration rate of ions in electrolytes and at the electrode interface via designing Li+-anion nanometric aggregates (LA-nAGGs) in low-concentration electrolytes. Li+ coordinated by TFSI- and FSI- anions instead of a donor solvent promotes the formation of an inorganic-rich interfacial layer and facilitates Li+ transfer. Consequently, the LA-nAGG-type electrolyte demonstrated a high ionic conductivity (0.6 mS cm-1) at -70 °C and a low activation energy of charge transfer (38.24 kJ mol-1), enabling Li||NiFe-Prussian blue derivative cells to deliver ∼83.1% of their room-temperature capacity at -60 °C. This work provides an advanced strategy for the development of low-temperature electrolytes.

2.
Angew Chem Int Ed Engl ; 63(2): e202311413, 2024 Jan 08.
Artículo en Inglés | MEDLINE | ID: mdl-38009687

RESUMEN

With its efficient nitrogen fixation kinetics, electrochemical lithium-mediated nitrogen reduction reaction (LMNRR) holds promise for replacing Haber-Bosch process and realizing sustainable and green ammonia production. However, the general interface problem in lithium electrochemistry seriously impedes the further enhancement of LMNRR performance. Inspired by the development history of lithium battery electrolytes, here, we extend the ring-chain solvents coupling law to LMNRR system to rationally optimize the interface during the reaction process, achieving nearly a two-fold Faradaic efficiency up to 54.78±1.60 %. Systematic theoretical simulations and experimental analysis jointly decipher that the anion-rich Li+ solvation structure derived from ring tetrahydrofuran coupling with chain ether successfully suppresses the excessive passivation of electrolyte decomposition at the reaction interface, thus promoting the mass transfer of active species and enhancing the nitrogen fixation kinetics. This work offers a progressive insight into the electrolyte design of LMNRR system.

3.
Angew Chem Int Ed Engl ; 63(20): e202320258, 2024 May 13.
Artículo en Inglés | MEDLINE | ID: mdl-38456300

RESUMEN

Large-scale energy storage devices play pivotal roles in effectively harvesting and utilizing green renewable energies (such as solar and wind energy) with capricious nature. Biphasic self-stratifying batteries (BSBs) have emerged as a promising alternative for grid energy storage owing to their membraneless architecture and innovative battery design philosophy, which holds promise for enhancing the overall performance of the energy storage system and reducing operation and maintenance costs. This minireview aims to provide a timely review of such emerging energy storage technology, including its fundamental design principles, existing categories, and prototype architectures. The challenges and opportunities of this undergoing research topic will also be systematically highlighted and discussed to provide guidance for the subsequent R&D of superior BSBs while conducive to bridging the gap for their future practical application.

4.
Nano Lett ; 22(8): 3473-3479, 2022 04 27.
Artículo en Inglés | MEDLINE | ID: mdl-35426684

RESUMEN

The key to enabling high energy density of organic energy-storage systems is the development of high-voltage organic cathodes; however, the redox voltage (<4.0 V vs Li/Li+) of state-of-the-art organic electrode materials (OEMs) remains unsatisfactory. Herein, we propose a novel dibromotetraoxapentacene (DBTOP) redox center to surpass the redox potential limit of OEMs, achieving ultrahigh discharge plateaus of approximately 4.4 V (vs Li+/Li). As theoretically analyzed, electron delocalization between dioxin active centers and benzene rings as well as electron-withdrawing bromine atoms endows the molecule with a low occupied molecular orbital level by diluting the electron density of dioxin in the whole p-π conjugated skeleton, and the strong π-π interactions among the DBTOP molecules provide a faster electrochemical kinetic pathway. This tetraoxapentacene redox center makes the working voltage of OEMS closer to the high-voltage inorganic electrodes, and its chemical and structural tunability may stimulate the further development of high-voltage organic cathodes.


Asunto(s)
Dioxinas , Electrodos , Electrones , Litio/química , Oxidación-Reducción
5.
Nano Lett ; 22(7): 2898-2906, 2022 Apr 13.
Artículo en Inglés | MEDLINE | ID: mdl-35353004

RESUMEN

The practical application of aqueous high-rate Zn metal battery (ZMB) is limited due to accelerated dendrite formation at high current densities. It is urgent to find an electrolyte, which could not only be mechanically stiff to clamp down dendrites but also not sacrifice ionic conductivity and interfacial compatibility. Herein, a new type of dynamically "solid-liquid" interconvertible electrolyte based on non-Newtonian fluid (NNFE) is proposed. Liquidity characteristic of NNFE is favorable for electrochemical kinetics and interfacial compatibility. Furthermore, in an area with high current rate NNFE would respond and mechanically stiffen to dissuade localized increase in Zn dendrite growth. Even at a current density of 50 mA cm-2, NNFE enables reversible and stable operation of a Zn symmetrical cell over 20 000 cycles. For Zn//Na5V12O32 (NVO) full cell, the NNFE also realizes lengthy cycling for 5000 periods at 5 A g-1. This research opens up new inspirations to high-rate Zn metal even other metal batteries.

6.
Nano Lett ; 21(12): 5021-5027, 2021 Jun 23.
Artículo en Inglés | MEDLINE | ID: mdl-34078078

RESUMEN

Effective recycling of spent Li metal anodes is an urgent need for energy/resource conservation and environmental protection, making Li metal batteries more affordable and sustainable. For the first time, we explore a unique sustainable healable lithium alloy anode inspired by the intrinsic healing ability of liquid metal. This lithium alloy anode can transform back to the liquid state through Li-completed extraction, and then the structure degradation generated during operation could be healed. Therefore, an ultralong cycle life of more than 1300 times can be successfully realized under harsh conditions of 5 mA h cm-2 capacitance by a process of two healing behaviors. This design improves the sustainable utilization of Li metal to a great extent, bringing about unexpected effects in the field of lithium-based anodes even at an unprecedentedly high discharge current density (up to 25 mA cm-2) and capacity (up to 50 mA h cm-2).

7.
Angew Chem Int Ed Engl ; 60(42): 22933-22939, 2021 Oct 11.
Artículo en Inglés | MEDLINE | ID: mdl-34431192

RESUMEN

A built-in electric field in electrocatalyst can significantly accumulate higher concentration of NO3 - ions near electrocatalyst surface region, thus facilitating mass transfer for efficient nitrate removal at ultra-low concentration and electroreduction reaction (NO3 RR). A model electrocatalyst is created by stacking CuCl (111) and rutile TiO2 (110) layers together, in which a built-in electric field induced from the electron transfer from TiO2 to CuCl (CuCl_BEF) is successfully formed . This built-in electric field effectively triggers interfacial accumulation of NO3 - ions around the electrocatalyst. The electric field also raises the energy of key reaction intermediate *NO to lower the energy barrier of the rate determining step. A NH3 product selectivity of 98.6 %, a low NO2 - production of <0.6 %, and mass-specific ammonia production rate of 64.4 h-1 is achieved, which are all the best among studies reported at 100 mg L-1 of nitrate concentration to date.

8.
Bioorg Med Chem Lett ; 29(22): 126685, 2019 11 15.
Artículo en Inglés | MEDLINE | ID: mdl-31607606

RESUMEN

C14 alkyl benzoate ABG001, derived from naturally occurring gentisides, was reported to exhibit neurotrophic activity which is similar to NGF (Nerve Growth Factor). In this research, ABG001 was modified by the strategy of isosteric replacement and conformational restriction with the purpose of improving the bioactivity. The cellular neurotrophic activity of those ABG001 derivatives were evaluated, among which 3-hydroxyquinolin-2-(1H)-one A3 and 4-decylphenol ester B7 displayed much better neurotrophic activity compared with ABG001, which highlights the potential of those novel scaffolds for future neurotrophic agent development.


Asunto(s)
Ácido Benzoico/farmacología , Productos Biológicos/farmacología , Gentiana/química , Proyección Neuronal/efectos de los fármacos , Animales , Ácido Benzoico/química , Ácido Benzoico/aislamiento & purificación , Productos Biológicos/química , Productos Biológicos/aislamiento & purificación , Relación Dosis-Respuesta a Droga , Medicina Tradicional China , Estructura Molecular , Células PC12 , Ratas , Relación Estructura-Actividad
9.
Sci Total Environ ; 926: 171815, 2024 May 20.
Artículo en Inglés | MEDLINE | ID: mdl-38513859

RESUMEN

Typhoons can bring substantial casualties and economic ramifications, and effective prevention strategies necessitate a comprehensive risk assessment. Nevertheless, existing studies on its comprehensive risk assessment are characterized by coarse spatial scales, limited incorporation of geographic big data, and rarely considering disaster mitigation capacity. To address these problems, this study combined multi-source geographic big data to develop the Comprehensive Risk Assessment Model (CRAM). The model integrated 17 indicators from 4 categories of factors, including exposure, vulnerability, hazard, and mitigation capacity. A subjective-objective combination weighting method was introduced to generate the indicator weights, and comprehensive risk index of typhoon disasters was calculated for 987 counties along China's coastal regions. Results revealed a pronounced spatial heterogeneity of the comprehensive typhoon risk, which exhibited an overall decreasing trend from the southeast coastal areas toward the northwest inland territories. 61.7 % of the counties exhibited a medium-to-high level of comprehensive risk, and counties with very-high risks are predominantly concentrated in the Shandong Peninsula, Yangtze River Delta, Hokkien Golden Triangle, Greater Bay Area, Leizhou Peninsula, and Hainan Province, mainly due to high exposure and hazard factors. The correlation coefficient between the risk assessment results and typhoon-induced direct economic losses reached 0.702, indicating the effectiveness and reliability of the CRAM. Meanwhile, indicators from intrinsic attributes of typhoons and geographic big data had pronounced importance, and regional mitigation capacity should be improved. Our proposed method can help to scientifically understand spatial patterns of comprehensive risk and mitigate the effects of typhoon disasters in China's coastal regions.

10.
Scand J Clin Lab Invest ; 73(4): 339-43, 2013.
Artículo en Inglés | MEDLINE | ID: mdl-23611255

RESUMEN

We sought to measure serum salusin-α levels in patients with coronary artery disease (CAD) and to assess their correlation with the severity of the disease. We enrolled 172 patients with CAD and 91 controls. We assessed the angiographic severity of CAD by coronary atherosclerosis index (CAI) and detected serum salusin-α levels by enzyme-linked immunosorbent assay (ELISA). We demonstrated that CAD patients had significantly lower serum salusin-α levels compared to controls. Moreover, serum salusin-α levels were independently and negatively correlated with the presence and severity of CAD. These findings indicated that salusin-α might serve as a potential biomarker for predicting the development and progression of CAD.


Asunto(s)
Enfermedad de la Arteria Coronaria/sangre , Péptidos y Proteínas de Señalización Intercelular/sangre , Anciano , Biomarcadores/sangre , Proteína C-Reactiva/metabolismo , Estudios de Casos y Controles , Angiografía Coronaria , Enfermedad de la Arteria Coronaria/diagnóstico por imagen , Femenino , Humanos , Masculino , Persona de Mediana Edad , Péptido Natriurético Encefálico/sangre , Fragmentos de Péptidos/sangre , Índice de Severidad de la Enfermedad
11.
Adv Mater ; 35(9): e2208590, 2023 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-36583421

RESUMEN

Li-S batteries hold promise for pushing cell-level energy densities beyond 300 Wh kg-1 while operating at low temperatures (LTs, below 0 °C). However, the capacity release of existing Li-S batteries at LTs is still barely satisfactory, and there is almost no verification of the practicability of Li-S batteries at LTs in the Ah-level pouch cell. Here, antecedent molecular dynamics (MDs) combined with density functional theory analysis are used to systematically investigate Li+ solvation structure in conventional Li-S batteries at LTs, which unprecedentedly reveals the positive correlation between lithium salt concentration and Li+ de-solvation barrier, indicating dilute electrolytes can enhance the Li+ de-solvation kinetics and thus improve the capacity performance of cryogenic Li-S batteries. These insights derived from theoretical simulations invested Li-S batteries with a 67.34% capacity retention at -40 °C compared to their room temperature performance. In particular, an Ah-level Li-S pouch cell using dilute electrolytes with a high sulfur loading (5.6 mg cm-2 ) and lean electrolyte condition is fabricated, which delivers a discharge capacity of about 1000 mAh g-1 and ultra-high energy density of 350 Wh kg-1 at 0 °C, offering a promising route toward a practical high-energy cryogenic Li-S battery.

12.
Nat Commun ; 14(1): 2267, 2023 Apr 20.
Artículo en Inglés | MEDLINE | ID: mdl-37081028

RESUMEN

Biphasic self-stratified batteries (BSBs) provide a new direction in battery philosophy for large-scale energy storage, which successfully reduces the cost and simplifies the architecture of redox flow batteries. However, current aqueous BSBs have intrinsic limits on the selection range of electrode materials and energy density due to the narrow electrochemical window of water. Thus, herein, we develop nonaqueous BSBs based on Li-S chemistry, which deliver an almost quadruple increase in energy density of 88.5 Wh L-1 as compared with the existing aqueous BSBs systems. In situ spectral characterization and molecular dynamics simulations jointly elucidate that while ensuring the mass transfer of Li+, the positive redox species are strictly confined to the bottom-phase electrolyte. This proof-of-concept of Li-S BSBs pushes the energy densities of BSBs and provides an idea to realize massive-scale energy storage with large capacitance.

13.
J Phys Chem Lett ; 14(44): 9986-9995, 2023 Nov 09.
Artículo en Inglés | MEDLINE | ID: mdl-37906171

RESUMEN

Side reactions caused by highly active water molecules, including severe corrosion, hydrogen evolution, and dendrite growth, are impediments to the advancement of aqueous zinc ion batteries (ZIBs). Here, inspired by the pivotal role of plant fibers to prevent dehydration in nature, we designed a unique water-retaining plant fiber (WRPF) separator with strong hygroscopic ability to adsorb and trap water molecules. Elaborated theoretical and experimental characterizations prove that high-activity water could be sequestered by a WRPF separator, alleviating water-induced side reactions and accelerating the desolvation of hydrate Zn2+. Prominently, reversible Zn plating and stripping could be realized in Zn//Cu batteries. Even with elevated cathodic mass loading (21.94 mg cm-2), the Zn//VS2 full cell delivers high areal capacity 3.3 mAh cm-2 and well-maintained stability. The present study offers a versatile design strategy for separators using nature-inspired materials, aiming to address the challenging issue of "water" and achieve ultrastable interfacial chemistry of Zn anode.

14.
ACS Nano ; 17(21): 21614-21625, 2023 Nov 14.
Artículo en Inglés | MEDLINE | ID: mdl-37916674

RESUMEN

Despite the numerous advantages of aqueous Zn batteries, their practical application under cryogenic conditions is hindered by the freezing of the electrolyte because the abundance of hydrogen bonds (H-bonds) between H2O molecules drives the aqueous system to transform to an orderly frozen structure. Here, a design of H-bond interactions based on the guiding ideology of "strong replaces weak" is proposed. The strong H-bonds formed between introduced eutectic components and water molecules break down the weak H-bonds in the original water molecule network, which contributes to an ultralow freezing point and a high ionic conductivity of 1.7 mS cm-1 at -40 °C. Based on multiperspective theoretical simulations and tailor-made in situ cooling Raman characterizations, it has been demonstrated that substituting weak H-bonds with strong H-bonds facilitates the structural reshaping of Zn2+ solvation and remodeling of the H-bond network in the electrolyte. Endowed with this advantage, reversible and stable Zn plating/stripping behaviors could be realized at -40 °C, and the full cells display a high discharge capacity (200 mA h g-1) at -40 °C with ∼75% capacity retention after 1000 cycles. This study will expand the design philosophy of antifreezing aqueous electrolytes and provide a perspective to promote the adoption of Zn metal batteries for cryogenic environment large-scale energy storage.

15.
Adv Mater ; 34(47): e2203699, 2022 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-35816349

RESUMEN

Rechargeable batteries based on Li-S chemistry show promise as being possible for next-generation energy storage devices because of their ultrahigh capacities and energy densities. Research over the past decade has demonstrated that the morphology of lithium polysulfides (LPSs) in electrolytes (soluble or insoluble) plays a decisive role in battery performance. Early studies have focused mainly on inhibiting the dissolution of LPSs and invested considerable effort to realize this objective. However, in recent years, a completely different view that the dissolution of LPSs during battery discharge/charge should be promoted has emerged. At this critical juncture in the large-scale application of Li-S batteries, it is time to summarize and discuss both sides of the contradiction. Herein, an overview of these two opposite views pertaining to soluble and insoluble LPSs, including their historical environment, classical strategies, advantages, and disadvantages. Finally, the future morphology of LPSs in Li-S batteries is predicted based on a multiangle review of research studies conducted thus far, and the reasoning behind this conjecture is thoroughly discussed.

16.
ACS Nano ; 15(8): 13847-13856, 2021 Aug 24.
Artículo en Inglés | MEDLINE | ID: mdl-34382785

RESUMEN

The sluggish solid-solid conversion kinetics from Li2S4 to Li2S during discharge is considered the main problem for cryogenic Li-S batteries. Herein, an all-liquid-phase reaction mechanism, where all the discharging intermediates are dissolved in the functional thioether-based electrolyte, is proposed to significantly enhance the kinetics of Li-S battery chemistry at low temperatures. A fast liquid-phase reaction pathway thus replaces the conventional slow solid-solid conversion route. Spectral investigations and molecular dynamics simulations jointly elucidate the greatly enhanced kinetics due to the highly decentralized state of solvated intermediates in the electrolyte. Overall, the battery brings an ultrahigh specific capacity of 1563 mAh g-1sulfur in the cathode at -60 °C. This work provides a strategy for developing cryogenic Li-S batteries.

17.
Nanoscale Adv ; 2(5): 1828-1836, 2020 May 19.
Artículo en Inglés | MEDLINE | ID: mdl-36132504

RESUMEN

The solid-state lithium metal battery (SSLMB) is one of the most optimal solutions to pursue next-generation energy storage devices with superior energy density, in which solid-state electrolytes (SSEs) are expected to completely solve the safety problems caused by direct use of a lithium metal anode. Most previous work has mainly focused on improving the electrochemical performance of SSLMBs, but the safety issues have been largely ignored due to the influence of the stereotype that batteries with SSEs are always safe. In the actual research process, however, some potential dangers of SSLMBs have been gradually revealed, so extra attention should be paid to this issue. This minireview summarizes several aspects that could raise safety concerns and provides a brief overview of the corresponding solutions to each aspect. Finally, general conclusions and perspectives on the research of SSLMBs with ultra-high safety are presented.

18.
Dalton Trans ; 48(25): 9205-9213, 2019 Jun 25.
Artículo en Inglés | MEDLINE | ID: mdl-31157342

RESUMEN

Hierarchical porous MnCo2O4 yolk-shell microspheres have been synthesized via a facile chemical precipitation method with subsequent calcination treatment. The hierarchical porous MnCo2O4 yolk-shell microspheres as secondary nanomaterials can improve the effective contact area between the MnCo2O4 electrode and electrolyte, accommodate the volume variations during cycling, and shorten the Li+ diffusion path in the nanoparticles. Benefiting from their particular structure and interconnected pores, as anodes for lithium ion batteries, the hierarchical porous MnCo2O4 yolk-shell microspheres show high reversible lithium storage capacity, excellent cycling performance and enhanced rate capability. More importantly, they also exhibit long-life and high-rate lithium storage as high as 691.3 mA h g-1 after 500 cycles even at 1 C.

19.
ACS Omega ; 4(14): 16016-16025, 2019 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-31592125

RESUMEN

Porous multicomponent Mn-Sn-Co oxide microspheres (MnSnO3-MC400 and MnSnO3-MC500) have been fabricated using CoSn(OH)6 nanocubes as templates via controlling pyrolysis of a CoSn(OH)6/Mn0.5Co0.5CO3 precursor at different temperatures in N2. During the pyrolysis process of CoSn(OH)6/Mn0.5Co0.5CO3 from 400 to 500 °C, the part of (Co,Mn)(Co,Mn)2O4 converts into MnCo2O4 accompanied with structural transformation. The MnSnO3-MC400 and MnSnO3-MC500 microspheres as secondary nanomaterials consist of MnSnO3, MnCo2O4, and (Co,Mn)(Co,Mn)2O4. Benefiting from the advantages of multicomponent synergy and porous secondary nanomaterials, the MnSnO3-MC400 and MnSnO3-MC500 microspheres as anodes exhibit the specific capacities of 1030 and 750 mA h g-1 until 1000 cycles at 1 A g-1 without an obvious capacity decay, respectively.

20.
Mol Med Rep ; 18(4): 3547-3554, 2018 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-30106145

RESUMEN

Hypoxia­ischemia (H­I) is frequently observed in perinatal asphyxia and other diseases. It can lead to serious cardiac injury, cerebral damage, neurological disability and mortality. Previous studies have demonstrated that the phosphatidylinositol­3 kinase (PI3K)/protein kinase B (Akt) signaling pathway, which regulates a wide range of cellular functions, is involved in the resistance response to H­I through the activation of proteins associated with survival and inactivation of apoptosis­associated proteins. It can also regulate the expression of hypoxia­induced factor­1α (HIF­1α). HIF­1α can further regulate the expression of downstream proteins involved in glucose metabolism and angiogenesis, such as vascular endothelial growth factor and erythropoietin, to facilitate ischemic adaptation. Notably, HIF­1α may also induce detrimental effects. The effects of HIF­1 on ischemic outcomes may be dependent on the H­I duration, animal age and species. Thus, further investigation of the PI3K/Akt signaling pathway may provide further insights of the potential targets for treating diseases accompanied by H­I.


Asunto(s)
Subunidad alfa del Factor 1 Inducible por Hipoxia/metabolismo , Hipoxia/metabolismo , Isquemia/metabolismo , Fosfatidilinositol 3-Quinasas/metabolismo , Proteínas Proto-Oncogénicas c-akt/metabolismo , Transducción de Señal , Animales , Humanos , Hipoxia/patología , Isquemia/patología
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