A Self-Conditioned Metalloporphyrin as a Highly Stable Cathode for Fast Rechargeable Magnesium Batteries.
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ABSTRACT:
SUBMITTER: Abouzari-Lotf E
PROVIDER: S-EPMC8251709 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Magnesium rechargeable batteries potentially offer high-energy density, safety, and low cost due to the ability to employ divalent, dendrite-free, and earth-abundant magnesium metal anode. Despite recent progress, further development remains stagnated mainly due to the sluggish scission of magnesium-chloride bond and slow diffusion of divalent magnesium cations in cathodes. Here we report a battery chemistry that utilizes magnesium monochloride cations in expanded titanium disulfide. Combined theoretical modeling, spectroscopic analysis, and electrochemical study reveal fast diffusion kinetics of magnesium monochloride cations without scission of magnesium-chloride bond. The battery demonstrates the reversible intercalation of 1 and 1.7 magnesium monochloride cations per titanium at 25 and 60?°C, respectively, corresponding to up to 400?mAh?g-1 capacity based on the mass of titanium disulfide. The large capacity accompanies with excellent rate and cycling performances even at room temperature, opening up possibilities for a variety of effective intercalation hosts for multivalent-ion batteries.Magnesium rechargeable batteries potentially offer high-energy density, safety, and low cost. Here the authors show a battery that reversibly intercalates magnesium monochloride cations with excellent rate and cycle performances in addition to the large capacity.
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Project description:Lithium- and sodium-rich layered transition-metal oxides have recently been attracting significant interest because of their large capacity achieved by additional oxygen-redox reactions. However, layered transition-metal oxides exhibit structural degradation such as cation migration, layer exfoliation or cracks upon deep charge, which is a major obstacle to achieve higher energy-density batteries. Here we demonstrate a self-repairing phenomenon of stacking faults upon desodiation from an oxygen-redox layered oxide Na2RuO3, realizing much better reversibility of the electrode reaction. The phase transformations upon charging A2MO3 (A: alkali metal) can be dominated by three-dimensional Coulombic attractive interactions driven by the existence of ordered alkali-metal vacancies, leading to counterintuitive self-repairing of stacking faults and progressive ordering upon charging. The cooperatively ordered vacancy in lithium-/sodium-rich layered transition-metal oxides is shown to play an essential role, not only in generating the electro-active nonbonding 2p orbital of neighbouring oxygen but also in stabilizing the phase transformation for highly reversible oxygen-redox reactions.
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Project description:Multivalent cation rechargeable batteries are expected to perform well as high-capacity storage devices. Rechargeable magnesium batteries have an advantage in terms of resource utilization and safety. Here, we report on sulfur-doped vanadium pentoxide (S-V₂O₅) as a potential material for the cathodes of such a battery; S-V₂O₅ showed a specific capacity of 300 mAh·g-1. S-V₂O₅ was prepared by a method using a low-temperature plasma generated by carbon felt and a 2.45 GHz microwave generator. This study investigates the ability of S-V₂O₅ to achieve high capacity when added to metal oxide. The highest recorded capacity (420 mAh·g-1) was reached with MnO₂ added to composite SMn-V₂O₅, which has a higher proportion of included sulfur than found in S-V₂O₅. Results from transmission electron microscopy, energy-dispersive X-ray spectroscopy, Micro-Raman spectroscopy, and X-ray photoelectron spectroscopy show that the bulk of the SMn-V₂O₅ was the orthorhombic V₂O₅ structure; the surface was a xerogel-like V₂O₅ and a solid solution of MnO₂ and sulfur.
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Project description:In recent decades, rechargeable Mg batteries (RMBs) technologies have attracted much attention because the use of thin Mg foil anodes may enable development of high-energy-density batteries. One of the most critical challenges for RMBs is finding suitable electrolyte solutions that enable efficient and reversible Mg cells operation. Most RMB studies concentrate on the development of novel electrolyte systems, while only few studies have focused on the practical feasibility of using pure metallic Mg as the anode material. Pure Mg metal anodes have been demonstrated to be useful in studying the fundamentals of nonaqueous Mg electrochemistry. However, pure Mg metal may not be suitable for mass production of ultrathin foils (<100 microns) due to its limited ductility. The metals industry overcomes this problem by using ductile Mg alloys. Herein, the feasibility of processing ultrathin Mg anodes in electrochemical cells was demonstrated by using AZ31 Mg alloys (3 % Al; 1 % Zn). Thin-film Mg AZ31 anodes presented reversible Mg dissolution and deposition behavior in complex ethereal Mg electrolytes solutions that was comparable to that of pure Mg foils. Moreover, it was demonstrated that secondary Mg battery prototypes comprising ultrathin AZ31 Mg alloy anodes (≈25 μm thick) and Mgx Mo6 S8 Chevrel-phase cathodes exhibited cycling performance equal to that of similar cells containing thicker pure Mg foil anodes. The possibility of using ultrathin processable Mg metal anodes is an important step in the realization of rechargeable Mg batteries.
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Project description:The high anodic stability of electrolytes for rechargeable magnesium batteries enables the use of new positive electrodes, which can contribute to an increase in energy density. In this study, novel Ph3COMgCl-, Ph3SiOMgCl-, and B(OMgCl)3-based electrolytes were prepared with AlCl3 in triglyme. The Ph3COMgCl-based electrolyte showed anodic stability over 3.0?V vs. Mg but was chemically unstable, whereas the Ph3SiOMgCl-based electrolyte was chemically stable but featured lower anodic stability than the Ph3COMgCl-based electrolyte. Advantageously, the B(OMgCl)3-based electrolyte showed both anodic stability over 3.0?V vs. Mg (possibly due to the Lewis acidic nature of B in B(OMgCl)3) and chemical stability (possibly due to the hard acid character of B(OMgCl)3). B(OMgCl)3, which was prepared by reacting boric acid with a Grignard reagent, was characterized by nuclear magnetic resonance (NMR) spectroscopy, Fourier-transform infrared spectroscopy (FTIR), and X-ray absorption spectroscopy (XAS). The above analyses showed that B(OMgCl)3 has a complex structure featuring coordinated tetrahydrofuran molecules. 27Al NMR spectroscopy and Al K-edge XAS showed that when B(OMgCl)3 was present in the electrolyte, AlCl3 and AlCl2+ species were converted to AlCl4-. Mg K-edge XAS showed that the Mg species in B(OMgCl)3-based electrolytes are electrochemically positive. As a rechargeable magnesium battery, the full cell using the B(OMgCl)3-based electrolyte and a Mo6S8 Chevrel phase cathode showed stable charge-discharge cycles. Thus, B(OMgCl)3-based electrolytes, the anodic stability of which can be increased to ~3?V by the use of appropriate battery materials, are well suited for the development of practical Mg battery cathodes.
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Project description:To suppress the dendrite formation and alleviate volume expansion upon striping/platting is a key challenge for developing practical lithium metal anodes. Lithium metal in powder form possesses great potential to address this issue due to large specific surface area. However, the fabrication of powdery metallic lithium is largely restricted because of its unique softness, stickiness, and high reactivity. Here, a safe and readily accessible cryomilling process toward lithium powders is reported. Nanoscaled lithium powders (<500 nm) are successfully prepared from lithium foils with the assistance of a high-melting-point ionic liquid under cryogenic temperature. The prepared lithium powder anode exhibits superior electrochemical properties in symmetric cells, including extraordinarily low yet stable overpotential (≈50 mV), ultrahigh area capacity (30 mAh cm-2), and good long-term cyclability (1200 h) even cycling at high current density (10 mA cm-2). The powdery form of lithium also functions as a favorable prelithiation reagent for lithium-free anodes (e.g., Si, SiO, and SnO2). The findings open up a new avenue for the real-world application of lithium metal anodes for next-generation lithium batteries.
| S-EPMC6918098 | biostudies-literature
Project description:Nowadays, research on electrochemical storage systems moves into the direction of post-lithium-ion batteries, such as aluminum-ion batteries, and the exploration of suitable materials for such batteries. Vanadium pentoxide (V2O5) is one of the most promising host materials for the intercalation of multivalent ions. Here, we report on the fabrication of a binder-free and self-supporting V2O5 micrometer-thick paper-like electrode material and its use as the cathode for rechargeable aluminum-ion batteries. The electrical conductivity of the cathode was significantly improved by a novel in-situ and self-limiting copper migration approach into the V2O5 structure. This process takes advantage of the dissolution of Cu by the ionic liquid-based electrolyte, as well as the presence of two different accommodation sites in the nanostructured V2O5 available for aluminum-ions and the migrated Cu. Furthermore, the advanced nanostructured cathode delivered a specific discharge capacity of up to ~170 mAh g-1 and the reversible intercalation of Al3+ for more than 500 cycles with a high Coulomb efficiency reaching nearly 100%. The binder-free concept results in an energy density of 74 Wh kg-1, which shows improved energy density in comparison to the so far published V2O5-based cathodes. Our results provide valuable insights for the future design and development of novel binder-free and self-supporting electrodes for rechargeable multivalent metal-ion batteries associating a high energy density, cycling stability, safety and low cost.
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Project description:Recent years have seen an intense and renewed interest in the Mg battery research, naming Mg-S the ?Holy Grail? battery, and expectations that Mg battery system will be able to compete and surpass Li-ion batteries in a matter of years. Considerable progress has been achieved in the field of Mg electrolytes, where several new electrolytes with improved electrochemical performance and favorable chemical properties (non-corrosive, non-nucleophilic) were synthesized. Development in the field of cathodes remains a bit more elusive, with inorganic, sulfur, and organic cathodes all showing their upsides and downsides. This review highlights the recent progress in the field of Mg battery cathodes, paying a special attention to the performance and comparison of the different types of the cathodes. It also aims to define advantages and key challenges in the development of each type of cathodes and finally specific questions that should be addressed in the future research.
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Project description:Manganese oxide (MnO2) is one of the most promising intercalation cathode materials for zinc ion batteries (ZIBs). Specifically, a layered type delta manganese dioxide (?-MnO2) allows reversible insertion/extraction of Zn2+ ions and exhibits high storage capacity of Zn2+ ions. However, a poor conductivity of ?-MnO2, as well as other crystallographic forms, limits its potential applications. This study focuses on ?-MnO2 with nanoflower structure supported on graphite flake, namely MNG, for use as an intercalation host material of rechargeable aqueous ZIBs. Pristine ?-MnO2 nanoflowers and MNG were synthesized and examined using X-ray diffraction, electron spectroscopy, and electrochemical techniques. Also, performances of the batteries with the pristine ?-MnO2 nanoflowers and MNG cathodes were studied in CR2032 coin cells. MNG exhibits a fast insertion/extraction of Zn2+ ions with diffusion scheme and pseudocapacitive behavior. The battery using MNG cathode exhibited a high initial discharge capacity of 235 mAh/g at 200?mA/g specific current density compared to 130 mAh/g which is displayed by the pristine ?-MnO2 cathode at the same specific current density. MNG demonstrated superior electrical conductivity compared to the pristine ?-MnO2. The results obtained pave the way for improving the electrical conductivity of MnO2 by using graphite flake support. The graphite flake support significantly improved performances of ZIBs and made them attractive for use in a wide variety of energy applications.
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Project description:Great focus has recently been placed on anionic redox, to which high capacities of Li-rich layered oxides are attributed. With almost doubled capacity compared with state-of-the-art cathode materials, Li-rich layered oxides still fall short in other performance metrics. Among these, voltage decay upon cycling remains the most hindering obstacle, in which defect electrochemistry plays a critical role. Here, we reveal that the metastable state of cycled Li-rich layered oxide, which stems from structural defects in different dimensions, is responsible for the voltage decay. More importantly, through mild thermal energy, the metastable state can be driven to a stable state, bringing about structural and voltage recovery. However, for the classic layered oxide without reversible anionic redox, thermal energy can only introduce cation disordering, leading to performance deterioration. These insights elucidate that understanding the structure metastability and reversibility is essential for implementing design strategies to improve cycling stability for high-capacity layered oxides.
| S-EPMC7919000 | biostudies-literature