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Graphene oxide (GO) membranes have great potential for separation applications due to their low-friction water permeation combined with unique molecular sieving ability. However, the practical use of deposited GO membranes is limited by the inferior mechanical robustness of the membrane composite structure derived from conventional deposition methods. Here, we report a nanostructured GO membrane that possesses great permeability and mechanical robustness. This composite membrane consists of an ultrathin selective GO nanofilm (as low as 32 nm thick) and a postsynthesized macroporous support layer that exhibits excellent stability in water and under practical permeability testing. By utilizing thin-film lift off (T-FLO) to fabricate membranes with precise optimizations in both selective and support layers, unprecedented water permeability (47 L·m-2·hr-1·bar-1) and high retention (>98% of solutes with hydrated radii larger than 4.9 A) were obtained.

In this paper, we challenge the common assumption that collapsing the spatial dimensions of a 3D (spatial-channel) tensor in a convolutional neural network (CNN) into a vector via global pooling removes all spatial information. Specifically, we demonstrate that positional information is encoded based on the ordering of the channel dimensions, while semantic information is largely not. Following this demonstration, we show the real world impact of these findings by applying them to two applications. First, we propose a simple yet effective data augmentation strategy and loss function which improves the translation invariance of a CNN's output. Second, we propose a method to efficiently determine which channels in the latent representation are responsible for (i) encoding overall position information or (ii) region-specific positions. We first show that semantic segmentation has a significant reliance on the overall position channels to make predictions. We then show for the first time that it is possible to perform a `region-specific' attack, and degrade a network's performance in a particular part of the input. We believe our findings and demonstrated applications will benefit research areas concerned with understanding the characteristics of CNNs., ICCV 2021

Carbon-based supercapacitors exhibit great rate capability, power density and cycle life, but suffer from relatively low energy density. Polyaniline provides high specific capacitance, but lacks cycling stability. By combining carbon-based materials with tetraaniline, an oligomer of polyaniline, a hybrid composite is formed that demonstrates improved supercapacitor performance relative to either material alone. In this study, the reduced graphene oxide-oligoaniline composites have been synthesized by a one-step hydrothermal process without the need for adding any oxidizing or reducing agents. FTIR, Raman spectroscopy, XPS, and MALDI-TOF mass spectroscopy indicate the successful reduction of GO to rGO and the formation of aniline oligomers. Unlike most polyaniline nanostructures for which charge storage kinetics are limited by slow diffusion-controlled reactions, the majority of oligoaniline in this composite is exposed to the electrolyte and stores charge through fast surface-controlled reactions. The unique microstructure of the rGO-oligoaniline composites facilitates transport of ions and electrons, leading to greater utilization of the active materials, high specific capacitance of 640 F/g at 0.2 mA/cm2 (corresponding to 707 C/g specific capacity), great rate capability and good cycle stability (91% retention after 2000 cycles).

Three-dimensional graphenes are versatile materials for a range of electronic applications and considered among the most promising candidates for electrodes in future electric double layer capacitors (EDLCs) as they are expected to outperform commercially used activated carbon. Parameters such as electrical conductivity and active surface area are critical to the final device performance. By adding carbon nanodots to graphene oxide in the starting material for our standard laser-assisted reduction process, the structural integrity (i.e. lower defect density) of the final 3D-graphene is improved. As a result, the active surface area in the hybrid starting materials was increased by 130% and the electrical conductivity enhanced by nearly an order of magnitude compared to pure laser-reduced graphene oxide. These improved material parameters lead to enhanced device performance of the EDLC electrodes. The frequency response, i.e. the minimum phase angle and the relaxation time, were significantly improved from −82.2° and 128 ms to −84.3° and 7.6 ms, respectively. For the same devices the specific gravimetric device capacitance was increased from 110 to a maximum value of 214 F g−1 at a scan rate of 10 mV s−1.

Interferrometric scattering microscopy is used to mass quantify individual Cathepsin K enzymes in solution. Treatments for osteoporosis are assessed by monitoring the oligomerization of Cathepsin K.

Carbon materials are widely used for supercapacitor applications thanks to their high surface area, good rate capability, and excellent cycling stability. However, the development of high energy density carbon supercapacitors still remains a challenge. In this work, hollow Co3O4 nanoboxes have been embedded into three-dimensional macroporous laser-scribed graphene (LSG) to produce composite electrodes with improved electrochemical performance. Here, Co3O4 provides high capacity through fast and reversible redox reactions, while LSG serves as a conductive network to maintain high power. The open nanobox morphology is a unique solution for extracting the maximum capacity from Co3O4, resulting in electrodes whose surfaces, both internal and external, are accessible to the electrolyte. The electrochemical performance of the composite material is promising with a volumetric capacity of 60.0 C/cm3 and a specific capacity of 542.3 C/g, corresponding to 682.0 C/g of the constituent Co3O4. With a low equivalent series resistance of 0.9 Ω, the Co3O4/LSG electrode is able to maintain 113.1% of its original capacity after 10,000 cycles. This work provides new insights into the design of high-performance carbon/metal oxide nanocomposites for next-generation energy storage devices.

Supercapacitors are energy storage and conversion devices that display high power. In order to increase energy density, redox-active materials can be incorporated into the carbonaceous electrode(s). Although in recent years many studies have offered different redox-active candidates and composite methods, there is a constant search for an effective, easily producible and stable composite material. Here, we present a graphene/ferrocene composition as a redox active 3-D supercapacitor electrode material. The combination of highly reversible, conductive and strongly attached ferrocene with the high surface area and open porous structure of graphene results in high-power, high-energy density supercapacitors. The graphene scaffold is converted from graphene-oxide (GO) by laser irradiation, a facile, fast and eco-friendly method. The ferrocene is chemically bonded to the graphene by two different approaches that take advantage of the strong and stable pi–pi interactions between the carbon and the aromatic ligands. The excellent bonding between the components results in low internal resistance and high reversibility of the redox reaction. The composite demonstrated a 205% increase in specific capacitance from 87 F g−1 for pure laser reduced graphene oxide to 178 F g−1 for the composite with ferrocene. This is equivalent to an energy density of 6.19 W h kg−1 while maintaining a power density of 26.0 kW kg−1.

Producing highly oriented graphene is a major challenge that constrains graphene from fulfilling its full potential in technological applications. The exciting properties of graphene are impeded in practical bulk materials due to lattice imperfections that hinder charge mobility. A simple method to improve the structural integrity of graphene by utilizing laser irradiation on a composite of carbon nanodots (CNDs) and 3D graphene is presented. The CNDs attach themselves to defect sites in the graphene sheets and, upon laser-assisted reduction, patch defects in the carbon lattice. Spectroscopic experiments reveal graphitic structural recovery of up to 43% and electrical conductivity four times larger than the original graphene. The composites are tested as electrodes in electrochemical capacitors and demonstrate extremely fast RC time constant as low as 0.57 ms. Due to their low defect concentrations, the reduced graphene oxide-carbon nanodot (rGO-CND) composites frequency response is sufficiently fast to operate as AC line filters, potentially replacing today's electrolytic capacitors. Using this methodology, demonstrated is a novel line filter with one of the fastest capacitive responses ever reported, and an aerial capacitance of 68.8 mF cm-2 . This result emphasizes the decisive role of structural integrity for optimizing graphene in electronic applications.

2D nanomaterials are finding numerous applications in next-generation electronics, consumer goods, energy generation and storage, and healthcare. The rapid rise of utility and applications for 2D nanomaterials necessitates developing means for their mass production. This study details a new compressible flow exfoliation method for producing 2D nanomaterials using a multiphase flow of 2D layered materials suspended in a high-pressure gas undergoing expansion. The expanded gassolid mixture is sprayed in a suitable solvent, where a significant portion (up to 10% yield) of the initial hexagonal boron nitride material is found to be exfoliated with a mean thickness of 4.2 nm. The exfoliation is attributed to the high shear rates ((Formula presented.) > 105 s−1) generated by supersonic flow of compressible gases inside narrow orifices and converging-diverging channels. This method has significant advantages over current 2D material exfoliation methods, such as chemical intercalation and exfoliation, as well as liquid phase shear exfoliation, with the most obvious benefit being the fast, continuous nature of the process. Other advantages include environmentally friendly processing, reduced occurrence of defects, and the versatility to be applied to any 2D layered material using any gaseous medium. Scaling this process to industrial production has a strong possibility of reducing the cost of creating 2D nanomaterials. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

By combining electrochemical experiments with mass spectrometric analysis, it is found that using short chain oligomers to improve the cycling stability of conducting polymers in supercapacitors is still problematic. Cycling tests via cyclic voltammetry over a potential window of 0 to 1.0 V or 0 to 1.2 V in a two-electrode device configuration resulted in solid-state electropolymerization and chain scission. Electropolymerization of the aniline tetramer to generate long chain oligomers is shown to be possible despite the suggested decrease in reactivity and increase in intermediate stability with longer oligomers. Because aniline oligomers are more stable towards reductive cycling when compared to oxidative cycling, future conducting polymer/oligomer-based pseudocapacitors should consider using an asymmetric electrode configuration.

A facile method to convert biomolecule-based carbon nanodots (CNDs) into high-surface-area 3D-graphene networks with excellent electrochemical properties is presented. Initially, CNDs are synthesized by microwave-assisted thermolysis of citric acid and urea according to previously published protocols. Next, the CNDs are annealed up to 400 °C in a tube furnace in an oxygen-free environment. Finally, films of the thermolyzed CNDs are converted into open porous 3D turbostratic graphene (3D-ts-graphene) networks by irradiation with an infrared laser. Based upon characterizations using scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, Fourier-transform infrared spectroscopy, and Raman spectroscopy, a feasible reaction mechanism for both the thermolysis of the CNDs and the subsequent laser conversion into 3D-ts-graphene is presented. The 3D-ts-graphene networks show excellent morphological properties, such as a hierarchical porous structure and a high surface area, as well as promising electrochemical properties. For example, nearly ideal capacitive behavior with a volumetric capacitance of 27.5 mF L-1 is achieved at a current density of 560 A L-1 , which corresponds to an energy density of 24.1 mWh L-1 at a power density of 711 W L-1 . Remarkable is the extremely fast charge-discharge cycling rate with a time constant of 3.44 ms.

Electrochemical capacitors, also known as supercapacitors, are energy storage devices like batteries, yet they can be recharged a hundred to a thousand times faster. Because of their enabling features, supercapacitors are replacing batteries and capacitors in an increasing number of applications. Their high power density and excellent low temperature performance have made them the technology of choice for back-up power, cold starting, flash cameras and regenerative braking. They also play an important role in the progress of hybrid and electric vehicles. However, the low energy density of current supercapacitors is the main impediment to realizing the full commercial potential of this technology. This has triggered tremendous research efforts in order to develop new electrode materials that are capable of providing a huge amount of energy in a short period of time. In this talk, we will discuss the current status of graphene-based supercapacitors, highlight ongoing research activities and present challenges that must be addressed in the future. Several examples will be given on the rational design and fabrication of electrodes with the goal of making compact, reliable and energy dense supercapacitors that are mechanically flexible and possess both long cycle life and calendar life.

CAl(4)(2-/-) (D(4h), (1)A(1g)) is a cluster ion that has been established to be planar, aromatic, and contain a tetracoordinate planar C atom. Valence isoelectronic substitution of C with Si and Ge in this cluster leads to a radical change of structure toward distorted pentagonal species. We find that this structural change goes together with the cluster acquiring partial covalency of bonding between Si/Ge and Al(4), facilitated by hybridization of the atomic orbitals (AOs). Counter intuitively, for the AAl(4)(2-/-) (A = C, Si, Ge) clusters, hybridization in the dopant atom is strengthened from C, to Si, and to Ge, even though typically AOs are more likely to hybridize if they are closer in energy (i.e. in earlier elements in the Periodic Table). The trend is explained by the better overlap of the hybrids of the heavier dopants with the orbitals of Al(4). From the thus understood trend, it is inferred that covalency in such clusters can be switched off, by varying the relative sizes of the AOs of the main element and the dopant. Using this mechanism, we then successfully killed covalency in Si, and predicted a new aromatic cluster ion containing a tetracoordinate square planar Si, SiIn(4)(2-/-).

Supercapacitors are known for their rapid energy charge–discharge properties, often ten to a hundred times faster than batteries. However, there is still a demand for supercapacitors with even faster charge–discharge characteristics to fulfill the requirements of emerging technologies. The power and rate capabilities of supercapacitors are highly dependent on the morphology of their electrode materials. An electrically conductive 3D porous structure possessing a high surface area for ions to access is ideal. Using a flash of light, a method to produce highly interconnected 3D graphene architectures with high surface area and good conductivity is developed. The flash converted graphene is synthesized by reducing freeze-dried graphene oxide using an ordinary camera flash as a photothermal source. The flash converted graphene is used in coin cell supercapacitors to investigate its electrode materials properties. The electrodes are fabricated using either a precoating flash conversion or a postcoating flash conversion of graphene oxide. Both techniques produce supercapacitors possessing ultra-high power (5–7 × 105 W kg−1). Furthermore, optimized supercapacitors retain >50% of their capacitance when operated at an ultrahigh current density up to 220 A g−1.