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1.
Angew Chem Int Ed Engl ; : e202407303, 2024 Jun 05.
Artigo em Inglês | MEDLINE | ID: mdl-38837854

RESUMO

The Li-CO2 batteries utilizing greenhouse gas CO2 possess advantages of high energy density and environmental friendliness. However, these batteries following Li2CO3-product route typically exhibit low work voltage (<2.5 V) and energy efficiency. Herein, we have demonstrated for the first time that cobalt phthalocyanine (CoPc) as homogeneous catalyst can elevate the work plateau towards 2.98 V, which is higher than its theoretical discharge voltage without changing the Li2CO3-product route. This unprecedented discharge voltage is illustrated by mass spectrum and electrochemical analyses that CoPc has powerful adsorption capability with CO2 (-7.484 kJ mol-1) and forms discharge intermediate of C33H16CoN8O2. Besides high discharge capacity of 18724 mAh g-1 and robust cyclability over 1600 hours (1000 mAh g-1 cut-off) at a current density of 100 mA g-1, the batteries show high temperature adaptability (-30-80 °C). Our work is paving a promising avenue for the progress of high-efficiency Li-CO2 batteries.

2.
Small ; 19(18): e2207619, 2023 May.
Artigo em Inglês | MEDLINE | ID: mdl-36775918

RESUMO

Al ion batteries (AIBs) are attracting considerable attention owing to high volumetric capacity, low cost, and high safety. However, the strong electrostatic interaction between Al3+ and host lattice leads to discontented cycling life and inferior rate capability. Herein, a new strategy of employing water molecules contained VOPO4 ·H2 O to boost Al3+ migration via the charge shielding effect of water is reported. It is revealed that VOPO4 ·H2 O with water lubrication effect and smaller steric hindrance owns high capacity and fast Al3+ diffusion, while the loss of unstable water upon cycling leads to a rapid performance degradation. To address this problem, ultrathin VOPO4 ·H2 O@MXene nanosheets are fabricated via the formed TiOV bond between VOPO4 ·H2 O and MXene. The MXene aided exfoliation results in enhanced VOwater bond strength between H2 O and VOPO4 that endows the obtained composite with strong water holding ability, contributing to the extraordinary cycling stability. Consequently, the VOPO4 ·H2 O@MXene delivers a high discharge potential of 1.8 V and maintains discharge capacities of 410 and 374.8 mAh g-1 after 420 and 2000 cycles at the current densities of 0.5 and 1.0 A g-1 , respectively. This work provides a new understanding of water-contained AIBs cathodes and vital guidance for developing high-performance AIBs.

3.
Artigo em Inglês | MEDLINE | ID: mdl-35835451

RESUMO

Silicon (Si), a high-capacity lithium-ion battery anode material, has aroused wide attention. Its further practical application has been limited by its huge volume change during the cycle. To reduce this defect, the double cross-linked product of glycinamide hydrochloride modified poly(acrylic acid) (PAG) and epoxidized natural rubber (ENR) was developed as a water-based binder to obtain sufficient elasticity and a sufficiently strong adhesive force. Due to the double cross-linked structures in the system, the binder was enabled to effectively disperse and transfer the stress generated by the volume expansion of the Si particles and keep the integrity of the electrode during the cycle, thus obtaining excellent cycle performance. When the current density was 1 A g-1, PE55 (PAG: ENR = 1:1 cross-linked polymer) electrode still achieved a specific capacity of 2322.2 mAh g-1 after 100 cycles of constant current charge and discharge, and PE55 binder exhibited excellent bonding properties (4.45 N) and mechanical properties (stress: 5.51 MPa, strain: 87.4%). The comparison of poly(acrylic acid) (PAA) electrodes suggests that the introduction of elastic polymer and the construction of double cross-linked structures can increase the stability of Si anodes.

4.
Materials (Basel) ; 14(17)2021 Aug 27.
Artigo em Inglês | MEDLINE | ID: mdl-34500985

RESUMO

The Zn/MnO2 battery is a promising energy storage system, owing to its high energy density and low cost, but due to the dissolution of the cathode material, its cycle life is limited, which hinders its further development. Therefore, we introduced agar as a microskin for a MnO2 electrode to improve its cycle life and optimize other electrochemical properties. The results showed that the agar-coating layer improved the wettability of the electrode material, thereby promoting the diffusion rate of Zn2+ and reducing the interface impedance of the MnO2 electrode material. Therefore, the Zn/MnO2 battery exhibited outstanding rate performance. In addition, the agar-coating layer promoted the reversibility of the MnO2/Mn2+ reaction and acted as a colloidal physical barrier to prevent the dissolution of Mn2+, so that the Zn/MnO2 battery had a high specific capacity and exhibited excellent cycle stability.

5.
ACS Appl Mater Interfaces ; 13(48): 57470-57480, 2021 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-34816716

RESUMO

Elevating the discharge voltage plateau is regarded as the most effective strategy to improve the energy density of Li||CFx batteries in consideration of the finite capacity of CFx (x ∼ 1) cathodes. Here, an electrolyte, with LiBF4 in 1,3-dimethyl-2-imidazolidinone (DMI)/1,2-dimethoxyethane (DME), is developed for the first time to substantially promote the discharge voltage of CFx without compromising the available discharge capacity. DME possesses the property of low viscosity, while DMI functions to increase the voltage plateau during discharge owing to its moderate nucleophilicity and donor number, which decreases the energy barrier for breaking C-F bonds. The optimized electrolyte exhibits a significantly high average discharge voltage of 2.69 V at a current density of 10 mA g-1, which is 11.6% higher than the control electrolyte (2.41 V). In addition, a high energy density of 2099 Wh kg-1 is achieved in the optimized electrolyte (vs 1905 Wh kg-1 in the control electrolyte), showing great potential for practical applications.

6.
Front Microbiol ; 10: 28, 2019.
Artigo em Inglês | MEDLINE | ID: mdl-30828319

RESUMO

Alpine karst aquifers are important groundwater resources for the provision of drinking water all around the world. Yet, due to difficult accessibility and long-standing methodological limitations, the microbiology of these systems has long been understudied. The aim of the present study was to investigate the structure and dynamics of bacterial communities in spring water of an alpine limestone karst aquifer (LKAS2) under different hydrological conditions (base vs. event flow). The study was based on high-throughput 16S rRNA gene amplicon sequencing, study design and sample selection were guided by hydrology and pollution microbiology data. Spanning more than 27 months, our analyses revealed a taxonomically highly stable bacterial community, comprising high proportions of yet uncultivated bacteria in the suspended bacterial community fraction. Only the three candidate phyla Parcubacteria (OD1), Gracilibacteria (GN02), Doudnabacteria (SM2F11) together with Proteobacteria and Bacteroidetes contributed between 70.0 and 88.4% of total reads throughout the investigation period. A core-community of 300 OTUs consistently contributed between 37.6 and 56.3% of total reads, further supporting the hypothesis of a high temporal stability in the bacterial community in the spring water. Nonetheless, a detectable response in the bacterial community structure of the spring water was discernible during a high-discharge event. Sequence reads affiliated to the class Flavobacteriia clearly increased from a mean proportion of 2.3% during baseflow to a maximum of 12.7% during the early phase of the studied high-discharge event, suggesting direct impacts from changing hydrological conditions on the bacterial community structure in the spring water. This was further supported by an increase in species richness (Chao1) at higher discharge. The combination of these observations allowed the identification and characterization of three different discharge classes (Q1-Q3). In conclusion, we found a taxonomically stable bacterial community prevailing in spring waters from an alpine karst aquifer over the entire study period of more than 2 years. Clear response to changing discharge conditions could be detected for particular bacterial groups, whereas the most responsive group - bacteria affiliated to the class of Flavobacteriia - might harbor potential as a valuable natural indicator of "system disturbances" in karst aquifers.

7.
Biogeochemistry ; 141(3): 439-461, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30930510

RESUMO

Flooding is a major disturbance that impacts aquatic ecosystems and the ecosystem services that they provide. Predicted increases in global flood risk due to land use change and water cycle intensification will likely only increase the frequency and severity of these impacts. Extreme flooding events can cause loss of life and significant destruction to property and infrastructure, effects that are easily recognized and frequently reported in the media. However, flooding also has many other effects on people through freshwater aquatic ecosystem services, which often go unrecognized because they are less evident and can be difficult to evaluate. Here, we identify the effects that small magnitude frequently occurring floods (< 10-year recurrence interval) and extreme floods (> 100-year recurrence interval) have on ten aquatic ecosystem services through a systematic literature review. We focused on ecosystem services considered by the Millennium Ecosystem Assessment including: (1) supporting services (primary production, soil formation), (2) regulating services (water regulation, water quality, disease regulation, climate regulation), (3) provisioning services (drinking water, food supply), and (4) cultural services (aesthetic value, recreation and tourism). The literature search resulted in 117 studies and each of the ten ecosystem services was represented by an average of 12 ± 4 studies. Extreme floods resulted in losses in almost every ecosystem service considered in this study. However, small floods had neutral or positive effects on half of the ecosystem services we considered. For example, small floods led to increases in primary production, water regulation, and recreation and tourism. Decision-making that preserves small floods while reducing the impacts of extreme floods can increase ecosystem service provision and minimize losses.

8.
ACS Appl Mater Interfaces ; 8(49): 33619-33625, 2016 Dec 14.
Artigo em Inglês | MEDLINE | ID: mdl-27960427

RESUMO

We reported a rhombohedral Na-rich nickel hexacyanoferrate (r-NiHCF) with high discharge voltage, which also possesses long cycle stability and excellent rate capability when serving as the cathode material of Na-ion batteries. First-principles calculations suggest that the high working voltage of r-NiHCF is correlated to the asymmetric residence of Na+ ions in the rhombohedral framework in parallel with the low charge density at the Fe2+ ions. In both aqueous and ether-based electrolytes, r-NiHCF exhibits higher voltage than that of cubic NiHCF. Rate and cycle experiments indicate that r-NiHCF delivers a specific capacity of 66.8 mAh g-1 at the current density of 80 mA g-1, which is approximate to the theoretical capacity of r-NiHCF. A capacity retention of 96% can be achieved after 200 cycles. The excellent stability of r-NiHCF can be assigned to the absence of rhombohedral-cubic phase transition and negligible volume variation during electrochemical redox, as proven by the ex situ XRD patterns at different depths of charge/discharge and the DFT calculations, respectively.

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