Bioinspired Micro/Nanofluidic Ion Transport Channels for Organic Cathodes in High‐Rate and Ultrastable Lithium/Sodium‐Ion Batteries

Abstract

Conjugated carbonyl compounds are considered as ideal substitutes for traditional inorganic electrodes in lithium/sodium ion batteries (LIBs/SIBs) due to their excellent redox reversibility and structural tunability. Here, a flexible sandwich‐structured 3,4,9,10‐perylenetetracarboxylic dianhydride (PTCDA)/reduced graphene oxide (RGO)/carbon nanotube (CNT) (PTCDA/RGO/CNT) composite film with bioinspired micro/nanofluidic ion transport channels and interconnected porous conductive frameworks is designed and obtained by vacuum‐filtration and heating methods for LIB/SIB applications. The PTCDA/RGO/CNT electrode with robust mechanical deformability exhibits high diffusion coefficients of Li+/Na+ and low Warburg coefficients. Thus, desirable electrochemical performances with high capacities of 131 and 126 mA h g−1 at 10 mA g−1, and ultralong cycling stability with over 99% capacity retention after 500 cycles at 200 mA g−1 are achieved for LIBs and SIBs, respectively. In particular, Li/Na‐ion full cells consisting of lithiated or sodiated electrospun carbon nanofiber anode and PTCDA/RGO/CNT‐based cathode are developed to exhibit high energy densities of 132.6 and 104.4 W h kg−1 at the power densities of 340 and 288 W kg−1 for LIBs and SIBs, respectively. The advantageous features demonstrated by constructing bioinspired micro/nanofluidic channels may provide a new pathway toward the design of next‐generation wearable energy storage devices.

Tailored Redox Kinetics, Electronic Structures and Electrode/Electrolyte Interfaces for Fast and High Energy‐Density Potassium‐Organic Battery

“…The LUMO, HOMO and E g of the prepared PTCDA‐based cathode materials analyzed with density functional tight theory (DFTB) method can therefore be utilized for a quantitative comparison . Thus far, many studies have focused on the smart design of electroactive monomers with controlled electronic structures (namely preparation of different monomers), while we demonstrate here the improved electronic conductivity of prepared polymeric cathodes and electronic structure of PTCDA segments via simply engineering the length of interconnected alkyl chains.…”

“…3) Understanding of the influences of macromolecular structure modifications on the redox kinetics. Previous works are mainly focused on designing new monomer molecules for enhancing performance of the polymer cathode . Much less attention has been put on the studies of their redox kinetics which have major influences on the rate performance and stability …”

A multifunctional polyimide nanofiber separator with a self-closing polyamide–polyvinyl alcohol top layer with a Turing structure for high-performance lithium–sulfur batteries

“…The relationships between the linear fittings of Z' and the square root in low frequency (ω -0.5 ) are shown in Figure 4e, the slope of which represents the Warburg factor to determine the Li + diffusion transportation. 60 It can be observed that the slopes of Li-S batteries with PI, PI/PA and PI/PA-PVA separators are 12.2, 63.1 and 43.4, respectively, which are much less than that for assembling Celgard separator (80.1), further confirming that the PI nanofiber-based separators show the better Li + transportation in the Li-S battery. The galvanostatic discharge-charge profiles of Li-S batteries assembled with PI, PI/PA-PVA and Celgard separators at 0.1 C are displayed in Figure 4f.…”

Na‐Ion Batteries—Approaching Old and New Challenges

“…[ 16 ] For this purpose, a wide catalog of materials are under research, such as conducting polymers, organosulfur compounds, organic radical compounds, carbonyl compounds (PTCDA and disodium rhodizonate). [ 18,80–82 ] These latter, carbonyl compounds, are the most studied family of organic electrodes in the last years, but they are still concerns that must be resolved. The main drawbacks of these systems are the dissolution of the cathode in the electrolyte that leads to rapid capacity fade, their low electronic conductivity that causes poor rate performance, and the increase of working potentials and tap density of the electrodes that would lead to high energy density cathodes.…”