The development of intrinsically safe and environmentally sustainable energy storage devices is a significant challenge. Recent advances in aqueous rechargeable lithium-ion batteries (ARLIBs) have made considerable steps in this direction. In parallel to the ongoing progress in the design of aqueous electrolytes that expand the electrochemically stable potential window, the design of negative electrode materials exhibiting large capacity and low intercalation potential attracts great research interest. Herein, we report the synthesis of high purity nanoscale Chevrel Phase (CP) MoS a simple, efficient and controllable molecular precursor approach with significantly decreased energy consumption compared to the conventional approaches. Physical characterization of the obtained product confirms the successful formation of CP-MoS and reveals that it is crystalline nanostructured in nature. Due to their unique structural characteristics, the MoS nanocubes exhibit fast kinetics in a 21 m lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) electrolyte as a result of the shorter Li ion diffusion distance. Full battery cells comprised of MoS and LiMnO as negative and positive electrode materials, respectively, operate at 2.23 V delivering a high energy density of 85 W h kg (calculated on the total mass of active materials) under 0.2 C-rate. At 4 C, the coulombic efficiency (CE) is determined to be 99% increasing to near 100% at certain cycles. Post-mortem physical characterization demonstrates that the MoS anode maintained its crystallinity, thereby exhibiting outstanding cycling stability. The cell outperforms the commonly used vanadium-based (VO (B), VO) or (NASICON)-type LiTi(PO) anodes, highlighting the promising character of the nanoscale CP-MoS as a highly efficient anode material. In summary, the proposed synthetic strategy is expected to stimulate novel research towards the widespread application of CP-based materials in various aqueous and non-aqueous energy storage systems.
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http://dx.doi.org/10.1039/d2nr02014a | DOI Listing |
Angew Chem Int Ed Engl
November 2024
State Key Laboratory of Coordination Chemistry, MOE Key Laboratory of Mesoscopic Chemistry, MOE Key Laboratory of High Performance Polymer Materials and Technology, Jiangsu Key Laboratory of Advanced Organic Materials, Tianchang New Materials and Energy Technology Research Center, Research Institute of Green Chemistry and Engineering, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, Jiangsu, 210023, China.
Rechargeable magnesium batteries are regarded as a promising multi-valent battery system for low-cost and sustainable energy storage applications. Boron-based organic magnesium salts with terminal substituent fluorinated anions (Mg[B(OR)], R=fluorinated alkyl) have exhibited impressive electrochemical stability and oxidative stability. Nevertheless, their deployment is hindered by the complicated synthesis routes and the surface passivation of Mg metal anode.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2024
School of Chemistry, University of Glasgow, G12 8QQ Glasgow, U.K.
Sustainable batteries are key for powering electronic devices of the future, with aqueous zinc-ion batteries (AZIBs) standing out for their use of abundant, readily available elements, and safer production processes. Among the various electrode materials studied for AZIBs, the Chevrel Phase, MoS has shown promise due to its open framework, but issues with zinc ion trapping have limited its practical application. In this work, we employed computational methods to investigate the insertion-deinsertion mechanism in a series of isostructural MoSSe ( = 0-8) solid solutions as materials that could balance the gravimetric capacity and reversible cycling for AZIBs.
View Article and Find Full Text PDFACS Omega
August 2024
Department of Materials Science and Engineering, The Ohio State University, Columbus, Ohio 43210, United States.
The Chevrel phase compounds CuMoS, NiMoS, and FeMoS, synthesized by self-propagating high temperature synthesis, were evaluated as photocatalysts for visible light photocatalytic desulfurization. Investigations began with reflectance measurements from which absorbance spectra were calculated using the Kubelka-Munk transformation. The absorbance data was then used to create Tauc plots to find the direct and indirect bandgaps of the Chevrel phase compounds.
View Article and Find Full Text PDFNanoscale
July 2024
Department of Chemistry, University of Manchester, Oxford Road, Manchester, M13 9PL, UK.
The nanoscale form of the Chevrel phase, MoS, is demonstrated to be a highly efficient zinc-free anode in aqueous zinc ion hybrid supercapacitors (ZIHSCs). The unique morphological characteristics of the material when its dimensions approach the nanoscale result in fast zinc intercalation kinetics that surpass the ion transport rate reported for some of the most promising materials, such as TiS and TiSe. Raman spectroscopy, post-mortem X-ray diffraction, Hard X-ray photoelectron spectroscopy, and density functional theory (DFT) calculations were combined to understand the overall mechanism of the zinc ion (de)intercalation process.
View Article and Find Full Text PDFPhys Chem Chem Phys
June 2024
Department of NanoEngineering, University of California San Diego, CA 92093, USA.
The concept of aromaticity is primarily invented to account for the high stability of conjugated organic compounds that possess a specific structural and chemical stability with (4 + 2) π electrons. In 1988, quasi-aromaticity was theoretically proposed for the MoS core in the Mo(μ-S)(μ-S)(χ-dtp)(μ-dtp) L compound (χ: chelating ligand; dtp: (EtO)PS) illustrated by canonical molecular orbitals. However, the origin of the quasi-aromaticity and chemical bonding remains ambiguous, lacking a thorough analysis in terms of stability and quantitative measurement of the aromatic character.
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