The complex surface chemistry that dictates the interaction between MXene and polysulfides - the formation of thiosulfate via consumption of -OH surface groups, followed by Lewis acid-base interaction between the exposed Ti atoms and polysulfides - is unravelled. Interweaving carbon nanotubes between the MXene layers creates a porous, conductive network with high polysulfide adsorptivity, enabling sulfur hosts with excellent performance even at high loading (5.5 mg cm ).

We report the fabrication of high-performance, self-standing composite sp(2)-carbon supercapacitor electrodes using single-walled carbon nanotubes (CNTs) as conductive binder. The 3-D mesoporous mesh architecture of CNT-based composite electrodes grants unimpaired ionic transport throughout relatively thick films and allows superior performance compared to graphene-based devices at an ac line frequency of 120 Hz. Metrics of 601 μF/cm(2) with a -81° phase angle and a rate capability (RC) time constant of 199 μs are obtained for thin carbon films. The free-standing carbon films were obtained from a chlorosulfonic acid dispersion and interfaced to stainless steel current collectors with various surface treatments. CNT electrodes were able to cycle at 200 V/s and beyond, still showing a characteristic parallelepipedic cyclic votammetry shape at 1 kV/s. Current densities are measured in excess of 6400 A/g, and the electrodes retain more than 98% capacity after 1 million cycles. These promising results are attributed to a reduction of series resistance in the film through the CNT conductive network and especially to the surface treatment of the stainless steel current collector.

Three-dimensional (3D) vertically aligned carbon nanotube (CNT) patterns were utilized as templates for fabricating mesoporous hybrid architectures composed of CNTs and various crystalline metal oxide (MO; M = Co, Zn, Mn) nanoparticles by a microwave-assisted chemical approach. Post-synthesis thermal treatment of the CNT/MO patterns culminated in structural reorganization, depending on the treatment conditions. In air, CNTs were removed by oxidation. The remaining MO architectures preserved the shape and alignment of the original 3D CNT patterns, but with different porosity characteristics and improved MO crystallinity. Elastocapillary condensation and bending were demonstrated to be useful tools for further architecture alternation. The mesoporous nature of the CNT/MO hybrids and the MO materials were confirmed by N2-BET measurements. CNT/Co3O4 aligned strips were used as an example to demonstrate the potential application of the CNT/MO architectures as electrode materials for supercapacitive storage. Galvanostatic measurements showed that the CNT/Co3O4 strips were stable up to 1000 charge-discharge cycles at a current density of 377 μA/cm(2) with a specific capacitance as high as 123.94 F/g.

There is a growing demand for high-rate rechargeable batteries for powering electric vehicles and portable electronics. Here, we demonstrate a strategy for improving electrode performance by controlling the formation of solid electrolyte interphase (SEI). A composite electrode consisting of hard carbon (HC) and carbon nanotubes (CNTs) was used to study the formation of the SEI at different charging rates in an electrolyte consisting of 1 M NaClO 4 in a mixed solvent with ethylene carbonate (EC) and propylene carbonate (PC), as well as fluoroethylene carbonate (FEC) additive. The half-cell method was used to form the SEI at different charging rates (e.g., 1, 10, and 100 A/g). Symmetric capacitor cells were employed to study ion transport properties through the SEI. It was found that the SEI is a primary factor responsible for limiting the capacity of the composite anode material in conventional ester-based electrolytes. The electrode with the SEI formed at 100 A/g exhibited the lowest impedance and delivered nearly twice the capacity of the electrode with the SEI formed at 1 A/g. This significant difference is due to a thin SEI formed at the fast charging rate, as has been observed with ether-based electrolytes. An identical decay rate (0.11 mA h/g per cycle) was observed on the electrodes with SEIs formed at different charging rates in an ester electrolyte. No chemical difference among the three SEI layers was found. However, morphological differences of the SEI layers were observed. This difference is believed to account for the different electrochemical behaviors of the electrodes. This work shows that high charging rates can result in the formation of an optimal SEI layer, contradicting the widely accepted practice of using low charging rates during the SEI formation in alkali-ion batteries.

There has been rapidly growing interest in developing fast-charging batteries for electric vehicles. The solid electrolyte interphase (SEI) layer formed at the graphite/electrolyte interface plays an important role in determining the lithiation rate of lithium-ion batteries (LIBs). In this work, we investigated lithium-ion transport behavior in thin-film graphite electrodes with different graphite particle sizes and morphologies for understanding the role of the SEI layer in fast charging LIBs. We varied the properties of the SEI by changing the current rate during the SEI formation. We observed that forming the SEI layer at a much higher current density than is traditionally used leads to a substantial reduction in electrode impedance and a corresponding increase in ion diffusivity. This enables thin-film graphite electrodes to be charged at current rates as high as 12 C (i.e., about 5 min charging time), demonstrating that graphite is not necessarily prevented from fast charging. By comparing the SEI layers formed at different current densities, we observed that lithium-ion diffusivity across the SEI layer formed on a 23 μm commercial graphite at a current density currently used in the industry (e.g., 0.1 C) is approximately 8.9 × 10–10 cm2/s.

Rechargeable batteries with high-rate capability are needed for vehicle electrification. It is important to understand charge storage behavior in battery electrode materials. We have investigated the charge storage capacity and mechanism of alkali metal ions Li+, Na+, and K+ in graphite and hard carbon (HC) nanoparticles of 50 nm in particle size. The charge storage capacity of the carbon nanoparticles follows the order: Li+ > K+ > Na+ in the potential window between 3.00 and 0.01 V vs the individual metal/metal ion couple. Above the plateau regions (above 0 V vs Na/Na+, 0.25 V vs K/K+, and 0.35 V vs Li/Li+), the storage of the alkali metal ions proceeds via a capacitive mechanism due to charge adsorption on the surface and defective sites, leading to a similar specific storage capacity. In the potential range between 3.0 and 0.01 V vs Li/Li+ and at 1 A/g, graphite and HC nanoparticles deliver Li+ storage capacities of 690 and 564 mAh/g, respectively. The significantly higher Li+ storage capacity of the graphite nanoparticles than the theoretical capacity of commercial graphite (372 mAh/g) is due to the extra Li+ storage via the capacitive mechanism. However, at an extremely high current density (e.g., 100 A/g), the HC nanoparticles store more Li+ (324 mAh/g) than the graphite nanoparticles (262 mAh/g). This study sheds light on alkali metal ion storage behavior in carbon nanoparticles and suggests that electrodes fabricated with carbon nanoparticles hold great promise for developing fast-charging rechargeable batteries.

Advancements in electrochemical energy storage devices such as batteries and supercapacitors are vital for a sustainable energy future. Significant progress has been made in developing novel materials for these devices, but less attention has focused on developments in electrode and device manufacturing. While electrodes are traditionally made through slurry casting of electrochemically active material, advanced manufacturing techniques enable patterning of novel electrode architectures and control of device geometries in real-time, which can potentially result in electrodes with increased loading, improved electrochemical performance, and added functionality, such as flexibility and wearability. These inexpensive methods are particularly suited for lab-scale research and start-up companies, as they enable rapid prototyping without a full device production line. The present review describes three main methods of advanced manufacturing (inkjet printing, direct ink writing, and laser-induced graphene techniques) and evaluates the performance of batteries and supercapacitors fabricated via these methods in comparison to traditionally manufactured devices.

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