Heterolayered, one-dimensional nanobuilding block mat batteries.

The rapidly approaching smart/wearable energy era necessitates advanced rechargeable power sources with reliable electrochemical properties and versatile form factors. Here, as a unique and promising energy storage system to address this issue, we demonstrate a new class of heterolayered, one-dimensional (1D) nanobuilding block mat (h-nanomat) battery based on unitized separator/electrode assembly (SEA) architecture. The unitized SEAs consist of wood cellulose nanofibril (CNF) separator membranes and metallic current collector-/polymeric binder-free electrodes comprising solely single-walled carbon nanotube (SWNT)-netted electrode active materials (LiFePO4 (cathode) and Li4Ti5O12 (anode) powders are chosen as model systems to explore the proof of concept for h-nanomat batteries). The nanoporous CNF separator plays a critical role in securing the tightly interlocked electrode-separator interface. The SWNTs in the SEAs exhibit multifunctional roles as electron conductive additives, binders, current collectors and also non-Faradaic active materials. This structural/physicochemical uniqueness of the SEAs allows significant improvements in the mass loading of electrode active materials, electron transport pathways, electrolyte accessibility and misalignment-proof of separator/electrode interface. As a result, the h-nanomat batteries, which are easily fabricated by stacking anode SEA and cathode SEA, provide unprecedented advances in the electrochemical performance, shape flexibility and safety tolerance far beyond those achievable with conventional battery technologies. We anticipate that the h-nanomat batteries will open 1D nanobuilding block-driven new architectural design/opportunity for development of next-generation energy storage systems.

Effect of catalyst and oxidant concentrations in a TEMPO oxidation system on the production of cellulose nanofibers.

In traditional TEMPO oxidation systems, the high cost of TEMPO catalysts has been a significant barrier to the industrialization of oxidized CNF. From an economic perspective, presenting the characteristics of various CNFs produced with the oxidation systems with reduced catalyst usage could facilitate the industrial application of CNF across a wide range of fields. In this study, it was demonstrated that reducing the amount of TEMPO catalyst used (from 0.1 to 0.05 mmol g-1) in a conventional oxidation system increased the carboxylate content by approximately 6.3%. Furthermore, the activation of hydroxyl amine TEMPO, which is generated after the oxidation reaction of cellulose, was enhanced by adjusting the dosage of the inexpensive oxidant NaClO, leading to a 20% improvement in carboxylate content. This suggests that controlling the amount of NaClO as an oxidant can be a key parameter in adjusting the dosage of TEMPO to achieve the targeted degree of surface substitution. Results from the dispersion stability, UV-transmittance, and morphological properties of TEMPO-oxidized CNF using microfluidizing treatment showed that high carboxylate content plays a crucial role in producing high-purity CNF suspensions, which are small, uniform, and free from microfibers. Additionally, by varying the number of mechanical treatments applied to the oxidized cellulose, various types of CNF suspensions with different mean widths were obtained. We expect that these findings offer meaningful insights to end-users seeking a breakthrough in the performance limitations of final applications using cellulose nanomaterials.

MnO2-deposited lignin-based carbon nanofiber mats for application as electrodes in symmetric pseudocapacitors.

Low-cost, high-performance electrodes are highly attractive for practical supercapacitor applications. MnO2-deposited carbon nanofiber mats (MnO2-CNFMs) are prepared for use as binder-free supercapacitor electrodes. MnO2 is deposited on the mats in situ by hydrothermally decomposing aqueous KMnO4, leading to the formation of nanocrystals of MnO2. The MnO2-CNFM electrode produced with 38.0µmol KMnO4 (this electrode) shows a high specific capacitance of ~171.6F·g-1 at a scan rate of 5mV·s-1. Moreover, a symmetric supercapacitor with the electrode exhibits a specific capacitance of 67.0F·g-1, an energy density of 6.0Wh·kg-1 and a power density of 160W·kg-1 at a special current of 0.1A·g-1. Further, the symmetric supercapacitor displays excellent cycling stability, retains approximately 99% of the capacitance after 1000cycles. The simplicity and ease of preparation of the MnO2-CNFMs as well as their suitability for use in coin-type supercapacitor cells make them ideal for application in cost-effective and high-performance electrodes for supercapacitors.

Coffee-Driven Green Activation of Cellulose and Its Use for All-Paper Flexible Supercapacitors.

Cellulose, which is one of the most-abundant and -renewable natural resources, has been extensively explored as an alternative substance for electrode materials such as activated carbons. Here, we demonstrate a new class of coffee-mediated green activation of cellulose as a new environmentally benign chemical-activation strategy and its potential use for all-paper flexible supercapacitors. A piece of paper towel is soaked in espresso coffee (acting as a natural activating agent) and then pyrolyzed to yield paper-derived activated carbons (denoted as "EK-ACs"). Potassium ions (K+), a core ingredient of espresso, play a viable role in facilitating pyrolysis kinetics and also in achieving a well-developed microporous structure in the EK-ACs. As a result, the EK-ACs show significant improvement in specific capacitance (131 F g-1 at a scan rate of 1.0 mV s-1) over control ACs (64 F g-1) obtained from the carbonization of a pristine paper towel. All-paper flexible supercapacitors are fabricated by assembling EK-ACs/carbon nanotube mixture-embedded paper towels (as electrodes), poly(vinyl alcohol)/KOH mixture-impregnated paper towels (as electrolytes), and polydimethylsiloxane-infiltrated paper towels (as packaging substances). The introduction of the EK-ACs (as an electrode material) and the paper towel (as a deformable and compliant substrate) enables the resulting all-paper supercapacitor to provide reliable and sustainable cell performance as well as exceptional mechanical flexibility. Notably, no appreciable loss in the cell capacitance is observed after repeated bending (over 5000 cycles) or multiple folding. The coffee-mediated green activation of cellulose and the resultant all-paper flexible supercapacitors open new material and system opportunities for eco-friendly high-performance flexible power sources.

All-solid-state flexible supercapacitors fabricated with bacterial nanocellulose papers, carbon nanotubes, and triblock-copolymer ion gels.

We demonstrate all-solid-state flexible supercapacitors with high physical flexibility, desirable electrochemical properties, and excellent mechanical integrity, which were realized by rationally exploiting unique properties of bacterial nanocellulose, carbon nanotubes, and ionic liquid based polymer gel electrolytes. This deliberate choice and design of main components led to excellent supercapacitor performance such as high tolerance against bending cycles and high capacitance retention over charge/discharge cycles. More specifically, the performance of our supercapacitors was highly retained through 200 bending cycles to a radius of 3 mm. In addition, the supercapacitors showed excellent cyclability with C(sp) (~20 mF/cm(2)) reduction of only <0.5% over 5000 charge/discharge cycles at the current density of 10 A/g. Our demonstration could be an important basis for material design and development of flexible supercapacitors.