Li1.3Al0.3Ti1.7(PO4)3 (LATP) is a promising solid-state electrolyte for next-generation solid-state lithium metal batteries, offering high ionic conductivity, superior air stability, and low cost. However, its practical application is hindered by high interface impedance due to rigid solid–solid contact with electrodes and instability when in contact with lithium metal. Here, a hybrid solid–liquid electrolyte is designed, consisting of a porous 3D LATP skeleton infiltrated with carbonate-based organic electrolyte, to ensure sufficient electrolyte wettability. Further, the thermodynamic instability between LATP and Li is solved by magnetron sputtering a layer of ferroelectric Ba0.5Sr0.5TiO3 (BST) onto the LATP surface. This BST interlayer prevents direct contact between LATP and Li metal, enhancing performance by dynamically regulating Li+ deposition, inhibiting dendrite growth, reducing overpotential and interface resistance, and improving Li+ transport. Compared to the LATP-based electrolyte (LATP-LE), the BST-modified hybrid electrolyte (B@LATP-LE) demonstrates largely improved ionic conductivity (0.42 to 1.38 mS cm−1) and outstanding electrochemical performance, achieving stable cycling for over 7000 h in LiLi cells and superior stability in LiFePO4Li and LiNi0.8Co0.1Mn0.1O2Li full cells. This approach offers a cost-effective solution to the interface issues of LATP and provides insights for high-performance lithium metal batteries.
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Electrochemical batteries and supercapacitors are considered ideal rechargeable technologies for next-generation energy storage systems. The key to further commercial applications of electrochemical energy storage devices is the design and investigation of electrode materials with high energy density and significant cycling stability. Recently, amorphous materials have attracted a lot of attention due to their more defects and structure flexibility, opening up a new way for electrochemical energy storage. In this perspective, we summarize the recent research regarding amorphous materials for electrochemical energy storage. This review covers the advantages and features of amorphous materials, the synthesis strategies to prepare amorphous materials, as well as the application and modification of amorphous electrodes in energy storage fields. Finally, the challenges and prospective remarks for future development in amorphous materials for electrochemical energy storage are concluded.
The advancement of lithium-sulfur (Li-S) batteries is severely retarded by lithium polysulfides (LiPSs) shuttling behavior and sluggish redox kinetics. Herein, the heterogeneous composite with defective Bi2Se3−x nanosheets and porous nitrogen-doped carbon (Bi2Se3−x/NC) is prepared by selenizing bismuth metal-organic frameworks as a multifunctional sulfur host. The highly efficient immobilization-conversion on LiPSs is realized by the synergistic effect of structure construction strategy and defect engineering. It is found that Bi2Se3−x with the suitable amount of selenium vacancies achieves the best electrochemical performance due to the advantages of its structure and composition. These results confirm the intrinsic correlation between defects and catalysis, which are revealed by computational and experimental studies. Due to these superiorities, the developed sulfur electrodes exhibited admirable stability and a fairly lower capacity decay rate of approximately 0.0278% per cycle over 1,000 cycles at a 3 C rate. Even at the high sulfur loading of 6.2 mg·cm−2, the cathode still demonstrates a high discharge capacity of 455 mAh·g−1 at 1 C. This work may enlighten the development of mechanism investigation and design principles regarding sulfur catalysis toward high-performance Li-S batteries.
The basal planes of transition metal dichalcogenides are basically inert for catalysis due to the absence of adsorption and activation sites, which substantially limit their catalytic application. Herein, a facile strategy to activate the basal plane of WS2 for hydrogen evolution reaction (HER) catalysis by phosphorous-induced electron density modulation is demonstrated. The optimized P doped WS2 (P-WS2) nanowires arrays deliver a low overpotential of 88 mV at 10 mA·cm−2 with a Tafel slope of 62 mV·dec−1 for HER, which is substantially better than the pristine counterpart. X-ray photoelectron spectroscopy confirms the surface electron densities of WS2 have been availably manipulated by P doping. Moreover, density functional theory (DFT) studies further prove P doping can redistribute the density of states (DOS) around EF, which endow the inert basal plane of P-WS2 with edge-like catalytic activity toward hydrogen evolution catalysis. Our work offers a facile and effective approach to modulate the catalytic surface of WS2 toward highly efficient HER catalysis.
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