In Situ Polymerization of Ultra-Thin and Defect-Free Polyamide Layer for Effectively Impeding the Polysulfides Shuttle.

Lithium-sulfur (Li-S) batteries present significant potential for next-generation high-energy-density devices. Nevertheless, obstacles such as the polysulfide shuttle and Li-dendrite growth severely impede their commercial production. It is still hard to eliminate gaps between individual particles on separators that serve as potential conduits for polysulfide shuttling. Herein, the synthesis of a nanoscale thickness and defect-free cross-linked polyamide (PA) layer on a polypropylene (PP) separator is presented through in situ polymerization. The PA modification layer can effectively impede the diffusion of polysulfides with a thickness of only 1.5 nm, as evidenced by the results of cyclic voltammetry (CV) and time-of-flight (TOF) testing. Therefore, the Li/Li symmetric battery assembled with the functional separator exhibits an overpotential of merely 12 mV after 1000 h of cycling under test conditions of 1 mA cm-2-1 mAh cm-2. Furthermore, the capacity degradation rate of the Li-S battery is only 0.06% per cycle over 450 cycles at 1 C, while the Li-S pouch cell retains 87.63% of its capacity after 50 cycles. This work will significantly advance the preparation and application of molecules in Li-S batteries, and it will also stimulate further research on defect-free modification of separators.

Enhancing the supercapacitive performance of a carbon-based electrode through a balanced strategy for porous structure, graphitization degree and N,B co-doping.

Regarding carbon-based electrodes, simultaneously establishing a well-defined meso-porous architecture, introducing abundant hetero-atoms and improving the graphitization degree can effectively enhance their capacitive performance. However, it remains a significant challenge to achieve a good balance between defects and graphitization degree. In this study, the porous structure and composition of carbon materials are co-optimised through a 'dual-function' strategy. Briefly, K3Fe(C2O4)3 and H3BO3 were hybridised with a gelatin aqueous solution to form a homogeneous composite hydrogel, followed by lyophilisation and carbonisation. Owing to the dual functionality of raw materials, the graphitization, activation and hetero-atom doping processes can occur simultaneously during a one-step high-temperature treatment. The resultant carbon material exhibits a high graphitization degree (ID/IG = 0.9 ± 0.1), high hetero-atom content (N: 9.0 ± 0.3 at.%, B: 6.9 ± 0.5 at.%) and a large specific area (1754 ± 58 m2/g). The as-prepared electrode demonstrates a superior capacitance of 383 ± 1F g-1 at 1 A/g. Interestingly, the cyclic voltammetry (CV) curves exhibit a distinctive pair of broad redox peaks, which is uncommon in KOH electrolyte. Experiment data and density functional theory (DFT) simulation verify that N-5, B co-doping enhances the activity of the faradic reaction of carbon electrodes in KOH electrolyte. Furthermore, the fabricated Zn-ion hybrid supercapacitor (ZHSC) based on this carbon electrode delivers a high-energy density of 140.7 W h kg-1 at a power density of 840 W kg-1.