Large-Area Fabrication of Porous Graphene Networks on Carbon Fabric via Millisecond Photothermal Processing of Polyaniline for Supercapacitors.

Supercapacitors demonstrate promising potential for flexible, multi-functional energy storage devices; however, their widespread adoption is confronted by fabrication challenges. To access a combination of desirable device qualities such as flexibility, lightweight, structural stability, and enhanced electrochemical performance, carbon fiber (CF) can be utilized as a current collector, alongside graphene as an electrochemically active material. Yet achieving a cost-effective, large-scale graphene production, particularly on CF, remains challenging. Here, a rapid (<1 min) photothermal approach is developed for the large-scale production of graphene directly onto CF, utilizing polyaniline (PANI) as a polymer precursor. The in situ electropolymerization of PANI on CF facilitates its rapid synthesis on large areas, followed by conversion into graphene networks, enabling the binder-free fabrication of supercapacitor devices. These devices exhibit an areal capacitance of 180 mF cm-2 (at 2 mA cm-2 in 1 m H2SO4), an order of magnitude higher than other fabric-based devices. Moreover, the devised photothermal strategy allows for one-step preparation of supercapacitor devices on areas exceeding 100 cm-2, yielding an absolute areal capacitance of 4.5 F. The proportional increase in capacitance with device area facilitates scaling and indicates the commercial viability of this approach for low-cost, energy-efficient, and high-throughput production of lightweight, high-performance graphene-based multi-functional supercapacitor devices.

Large Area Millisecond Preparation of High-Quality, Few-Layer Graphene Films on Arbitrary Substrates via Xenon Flash Lamp Photothermal Pyrolysis and Their Application for High-Performance Micro-supercapacitors.

We report a method for fast, efficient, and scalable preparation of high-quality, large area, few-layer graphene films on arbitrary substrates via high-intensity pulsed xenon flash lamp photothermal pyrolysis of thin precursor films at ambient conditions in millisecond time frames. The precursors comprised poly(2,2-bis(3,4-dihydro-3-phenyl-1,3-benzoxazine)), and cyclized polyacrylonitrile and possess significant absorption cross section within the bandwidth of the emission spectrum of a xenon flash lamp. By localizing light absorption to the precursor films, the process enabled the preparation of few-layer graphene films on any substrate, including thermally sensitive substrates without the need for any catalytic substrate as in chemical vapor deposition-based approaches or conductive electrodes as in electrochemical method-based approaches. The extent of conversion of the precursor films to graphene was strongly dependent on pulse energy and the local temperature achieved due to photothermal effect, which were controlled via pulse power modulation; it also depended on structural properties of the precursor and to a lesser extent on the substrate. The cPAN showed a higher efficiency for conversion to graphene, as confirmed by Raman spectra (ID/IG ∼ 0.3), and sheet resistance of 0.1 Ω cm. To demonstrate the utility of the process, graphene film electrodes prepared photothermally on carbon fiber current collector were used for the fabrication of micro-supercapacitors with a very high areal supercapacitance of 3.5 mF/cm2. Subsequent deposition of manganese oxide onto the fabricated electrodes significantly increased the energy storage capability of the supercapacitor, yielding a device with exceptionally high capacitance of 80 F/g at 1 mA current, good rate capability, and long cycle life.

Printed microfluidic sweat sensing platform for cortisol and glucose detection.

Wearable sweat biosensors offer compelling opportunities for improved personal health monitoring and non-invasive measurements of key biomarkers. Inexpensive device fabrication methods are necessary for scalable manufacturing of portable, disposable, and flexible sweat sensors. Furthermore, real-time sweat assessment must be analyzed to validate measurement reliability at various sweating rates. Here, we demonstrate a "smart bandage" microfluidic platform for cortisol detection and continuous glucose monitoring integrated with a synthetic skin. The low-cost, laser-cut microfluidic device is composed of an adhesive-based microchannel and solution-processed electrochemical sensors fabricated from inkjet-printed graphene and silver solutions. An antibody-derived cortisol sensor achieved a limit of detection of 10 pM and included a low-voltage electrowetting valve, validating the microfluidic sensor design under typical physiological conditions. To understand effects of perspiration rate on sensor performance, a synthetic skin was developed using soft lithography to mimic human sweat pores and sweating rates. The enzymatic glucose sensor exhibited a range of 0.2 to 1.0 mM, a limit of detection of 10 µM, and reproducible response curves at flow rates of 2.0 µL min-1 and higher when integrated with the synthetic skin, validating its relevance for human health monitoring. These results demonstrate the potential of using printed microfluidic sweat sensors as a low-cost, real-time, multi-diagnostic device for human health monitoring.

Roll-to-roll nanoimprint lithography using a seamless cylindrical mold nanopatterned with a high-speed mastering process.

The advanced optical and wetting properties of metamaterials, plasmonic structures, and nanostructured surfaces have been repeatedly demonstrated in lab-scale experiments. Extending these exciting discoveries to large-area surfaces can transform technologies ranging from solar energy and virtual reality to biosensors and anti-microbial surfaces. Although photolithography is ideal for nanopatterning of small, expensive items such as computer chips, nanopatterning of large-area surfaces is virtually impossible with traditional lithographic techniques due to their exceptionally slow patterning rates and high costs. This article presents a high-throughput process that achieves large-area nanopatterning by combining roll-to-roll (R2R) nanoimprint lithography (NIL) and nanocoining, a process that can seamlessly nanopattern around a cylinder hundreds of times faster than electron-beam lithography. Here, nanocoining is used to fabricate a cylindrical mold with nanofeatures spaced by 600 nm and microfeatures spaced by 2 µm. This cylindrical drum mold is then used on a R2R NIL setup to pattern over 60 feet of polymer film. Microscopy is used to compare the feature shapes throughout the process. This scalable process offers the potential to transfer exciting lab-scale demonstrations to industrial-scale manufacturing without the prohibitively high cost usually associated with the fabrication of a master mold.