Although the reversible and inexpensive energy storage characteristics of the lithium–sulfur (Li‐S) battery have made it a promising candidate for electrical energy storage, the dendrite growth (anode) and shuttle effect (cathode) hinder its practical application. Here, it is shown that new electrolytes for Li‐S batteries promote the simultaneous formation of bilateral solid electrolyte interfaces on the sulfur‐host cathode and lithium anode, thus effectively suppressing the shuttle effect and dendrite growth. These high‐capacity Li‐S batteries with new electrolytes exhibit a long‐term cycling stability, ultrafast‐charge/slow‐discharge rates, super‐low self‐discharge performance, and a capacity retention of 94.9% even after a 130 d long storage. Importantly, the long cycle stability of these industrial grade high‐capacity Li‐S pouch cells with new electrolytes will provide the basis for creating robust energy dense Li‐S batteries with an extensive life cycle.

We developed a surfactant-free spray coating process to coat commercial cellulose-based paper with carbon nanotubes (CNTs) and prepared paper-CNTs current collectors for Li-ion batteries (LIBs). The paper-CNTs were used as current collectors for replacing conventional aluminum foil. Li-ion batteries assembled using paper-CNTs were coated with LiFePO4 as the active material and used as cathodes with Li as the anode, and the assembled LIBs showed a high energy density of 460 Wh kg−1 at a power density of 250 W kg−1. These electrodes were stable even at a current density as high as 600 mA g−1, and showed cycling stability for ~450 cycles at 150 mAh g−1. Furthermore, paper-CNTs based electrodes showed ~17% improvement in areal capacity compared to commercial aluminum-based electrodes suggesting that paper-CNTs can readily displace Al foils as current collectors. Summary: Paper based current collectors have been proposed as a cost-effective and simple replacement for aluminum current collectors. This has been achieved by a scalable spray coating of CNTs on printing papers without any surfactants or binders and subsequently testing them as current collectors for Li-ion batteries.

Resistive interfaces within the electrodes limit the energy and power densities of a battery, for example, a Li-ion battery (LIB). Typically, active materials are mixed with conductive additives in organic solvents to form a slurry, which is then coated on current collectors (e.g., bare or carbon-coated Al foils) to reduce the inherent resistance of the active material. Although many approaches using nanomaterials to either replace Al foils or improve conductivity within the active materials have been previously demonstrated, the resistance at the current collector active material interface (CCAMI), a key factor for enhancing the energy and power densities, remains unaddressed. We show that carbon nanotubes (CNTs), either directly grown or spray-coated on Al foils, are highly effective in reducing the CCAMI resistance of traditional LIB cathode materials (LiFePO 4 or LFP and LiNi 0.33 Co 0.33 Mn 0.33 O 2 or NMC). Moreover, the CNT coatings displace the need for currently used toxic organic solvents (e.g., N -methyl-2-pyrrolidone) by providing capillary channels, which improve the wetting of aqueous dispersions containing active materials. The vertically aligned CNT-coated electrodes exhibited energy densities as high as (1) ∼500 W h kg –1 at ∼170 W kg –1 for LFP and (2) ∼760 W h kg –1 at ∼570 W kg –1 for NMC. The LIBs with CCAMI-engineered electrodes withstood discharge rates as high as 600 mA g –1 for 500 cycles in the case of LFP, where commercial electrodes failed. The CNT-based CCAMI engineering approach is versatile with wide applicability to improve the performance of even textured active materials for both cathodes and anodes.

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