The current lifestyles, increasing population, and limited resources result in energy research being at the forefront of worldwide grand challenges, increasing the demand for sustainable and more efficient energy devices. In this context, additive manufacturing brings the possibility of making electrodes and electrical energy storage devices in any desired three-dimensional (3D) shape and dimensions, while preserving the multifunctional properties of the active materials in terms of surface area and conductivity. This paves the way to optimized and more efficient designs for energy devices. Here, we describe how three-dimensional (3D) printing will allow the fabrication of bespoke devices, with complex geometries, tailored to fit specific requirements and applications, by designing water-based thermoresponsive inks to 3D-print different materials in one step, for example, printing the active material precursor (reduced chemically modified graphene (rCMG)) and the current collector (copper) for supercapacitors or anodes for lithium-ion batteries. The formulation of thermoresponsive inks using Pluronic F127 provides an aqueous-based, robust, flexible, and easily upscalable approach. The devices are designed to provide low resistance interface, enhanced electrical properties, mechanical performance, packing of rCMG, and low active material density while facilitating the postprocessing of the multicomponent 3D-printed structures. The electrode materials are selected to match postprocessing conditions. The reduction of the active material (rCMG) and sintering of the current collector (Cu) take place simultaneously. The electrochemical performance of the rCMG-based self-standing binder-free electrode and the two materials coupled rCMG/Cu printed electrode prove the potential of multimaterial printing in energy applications.
Batteries that extend performance beyond the intrinsic limits of Li-ion batteries are among the most important developments required to continue the revolution promised by electrochemical devices. Of these next-generation batteries, lithium sulfur (Li–S) chemistry is among the most commercially mature, with cells offering a substantial increase in gravimetric energy density, reduced costs and improved safety prospects. However, there remain outstanding issues to advance the commercial prospects of the technology and benefit from the economies of scale felt by Li-ion cells, including improving both the rate performance and longevity of cells. To address these challenges, the Faraday Institution, the UK’s independent institute for electrochemical energy storage science and technology, launched the Lithium Sulfur Technology Accelerator (LiSTAR) programme in October 2019. This Roadmap, authored by researchers and partners of the LiSTAR programme, is intended to highlight the outstanding issues that must be addressed and provide an insight into the pathways towards solving them adopted by the LiSTAR consortium. In compiling this Roadmap we hope to aid the development of the wider Li–S research community, providing a guide for academia, industry, government and funding agencies in this important and rapidly developing research space.
Electrochemical double layer capacitors (EDLCs) are investigated with activated carbon electrodes and a lithium-ion electrolyte, in anticipation of potential future applications in hybridised battery-supercapacitor devices and lithium ion capacitors. An experimental study of a symmetric electrochemical double layer capacitor (EDLC) with activated carbon (AC) electrodes on aluminium foil current collectors and electrolyte 1 M LiPF6 in EC:EMC 50:50 v/v concludes a stability window to a maximum potential of 3 V, an equivalent in series resistance of 48 ohm for 1 cm 2 cell area (including the contact resistance between electrode and current collector) and an average specific electrode capacitance of 50.5 F g -1 . Three AC electrode materials are assessed via computer simulations based on a continuum ion and charge transport model with volumeaveraged equations, considering the pore size distribution for each electrode material and, depending on pore size, transport of tetrahedral solvated or flat solvated Li + ions and solvated or desolvated PF6ions. The computer simulations demonstrate that the best electrode material is an AC coating electrode with a hierarchical pore size distribution measured in the range of 0.5-180 nm and bimodal shape, and specific surface area BET = 808 m 2 g -1 .
Activated carbon materials are prepared from phenolic resin precursors by physical activation to fabricate electrodes for electric double-layer capacitors (EDLCs). Pore size and surface area of the carbon materials are controlled during the synthesizing process and after the carbonization through activation in a CO 2 atmosphere to different levels of burn-off. The resultant carbon materials were evaluated as EDLC electrodes, using electrochemical impedance spectroscopy (EIS) and galvanostatic charge-discharge (GCD) measurements with the organic electrolyte of spiro-(1,1 0 )-bipyrrolidinium tetrafluoroborate in propylene carbonate, SBPBF 4 /PC. The results of the study showed that the capacitance of carbon materials, as well as energy density of the EDLC cells, increased by increasing the level of burn-off (activation). The 46% activated carbon gave a capacitance of $160 F g À1 and an energy density of $35 W h kg À1 , at a current density of 1 mA cm À2 . The long term cycling tests showed high cycling stability of these carbon materials.
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