CoSe materials with different nanostructures are used as pseudocapacitive Mg-storage cathodes, which exhibit fast solid-state Mg ions diffusion kinetics. In this work, CoSe with different nanostructures including hollow microspheres (H-CoSe), nano-polyhedra (P-CoSe) and nanorods (R-CoSe) are fabricated by using facile one-step hydrothermal methods, and used as pseudocapacitive electrodes for rechargeable Mg batteries. It is observed that R-CoSe exhibits the highest reversible capacity of 233 mA h g at 50 mA g and an excellent rate capability of 116 mA h g at 500 mA g, ascribing to the 1D nanorod structure which facilitates the solid-state Mg diffusion. Benefitting from the stable hierarchical structure, H-CoSe exhibits a superior long-term cycling stability of 350 cycles. A mechanism study indicates that the redox reaction reversibly occurs between CoSe and metallic Co. Further investigation demonstrates that the fast solid-state Mg diffusion kinetics and surface-controlled pseudocapacitive behavior enhance the electrochemical performance. This work highlights a novel and efficient Mg-storage strategy of using pseudocapacitive materials, and the performance and solid-state Mg diffusion kinetics of CoSe could be optimized by rational structural tailoring.
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Angew Chem Int Ed Engl
January 2025
UT Austin: The University of Texas at Austin, Materials Science and Engineering, 1 University Station C2200, 78712, Austin, UNITED STATES OF AMERICA.
The extensive commercialization of practical solid-state batteries (SSBs) necessitates the development of high-loading solid-state cathodes with fast charging capability. However, electrochemical kinetics are severely delayed in thick cathodes due to tortuous ion transport pathways and slow solid-solid ion diffusion, which limit the achievable capacity of SSBs at high current densities. In this work, we propose a conductivity gradient cathode with low-tortuosity to enable facile ion transport and counterbalance ion concentration gradient, thereby overcoming the kinetic limitations and achieving fast charging capabilities in thick cathodes.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
Guizhou Provincial Key Laboratory of Computing and Network Convergence, School of Information, Guizhou University of Finance and Economics, Guiyang, Guizhou 550025, P. R. China.
Developing superionic conductor (SIC) materials offers a promising pathway to achieving high ionic conductivity in solid-state electrolytes (SSEs). The LiGePS (LGPS) family has received significant attention due to its remarkable ionic conductivity among various SIC materials. molecular dynamics (AIMD) simulations have been extensively used to explore the diffusion behavior of Li ions in LiGePS.
View Article and Find Full Text PDFAdv Mater
January 2025
Max Planck Institute for Solid State Research, Heisenbergstr. 1, 70569, Stuttgart, Germany.
The rapid advancement of covalent organic frameworks (COFs) in recent years has firmly established them as a new class of molecularly precise and highly tuneable porous materials. However, compared to other porous materials, such as zeolites and metal-organic frameworks, the successful integration of hierarchical porosity into COFs remains largely unexplored. The challenge lies in identifying appropriate synthetic methods to introduce secondary pores without compromising the intrinsic structural porosity of COFs.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, GBRCE for Functional Molecular Engineering, School of Chemistry, IGCME, Sun Yat-Sen University, Guangzhou 510275, China.
Exploring the interactions between oxygen molecules and metal sites has been a significant topic. Most previous studies concentrated on enzyme-mimicking metal sites interacting with O to form M-OO species, leaving the development of new types of O-activating metal sites and novel adsorption mechanisms largely overlooked. In this study, we reported an Fe(II)-doped metal-organic framework (MOF) [FeZnH(bibtz)] (, Hbibtz = 1,1'-5,5'-bibenzo[][1,2,3]triazole), featuring an unprecedented tetrahedral Fe(II)HN site.
View Article and Find Full Text PDFNano Lett
January 2025
Tianjin Key Lab for Rare Earth Materials and Applications, Center for Rare Earth and Inorganic Functional Materials, School of Materials Science and Engineering, National Institute for Advanced Materials, Nankai University, Tianjin 300350, P.R. China.
Although aliovalent ion substitution is an important strategy for enhancing ionic conductivity in halide electrolytes, the choice of doping ions is often restricted to tetravalent ions, and investigations into the intrinsic origin of the doping mechanism are lacking. In this work, we investigated the effects of Zr, Ta and W doping on the crystal structure and ionic conductivity of yttrium-based rare-earth halides. Only Zr achieves fast ion diffusion in both the (001) and (002) crystal planes by affecting the volume of the octahedron and the tetrahedral interstitial space, whereas Ta significantly enhances the ion diffusion rate in the (001) crystal plane while suppressing it in the (002) plane, and W does the opposite.
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