Although various carbon nanomaterials including activated carbon, carbon nanotubes, and graphene have been successfully demonstrated for high-performance ultracapacitors, their capacitances need to be improved further for wider and more challenging applications. Herein, using nitrogen-doped graphene produced by a simple plasma process, we developed ultracapacitors whose capacitances (∼280 F/g(electrode)) are about 4 times larger than those of pristine graphene based counterparts without sacrificing other essential and useful properties for ultracapacitor operations including excellent cycle life (>200,000), high power capability, and compatibility with flexible substrates. While we were trying to understand the improved capacitance using scanning photoemission microscopy with a capability of probing local nitrogen-carbon bonding configurations within a single sheet of graphene, we observed interesting microscopic features of N-configurations: N-doped sites even at basal planes, distinctive distributions of N-configurations between edges and basal planes, and their distinctive evolutions with plasma duration. The local N-configuration mappings during plasma treatment, alongside binding energy calculated by density functional theory, revealed that the origin of the improved capacitance is a certain N-configuration at basal planes.
The high porosity of metal-organic frameworks (MOFs) has been used to achieve exceptional gas adsorptive properties but as yet remains largely unexplored for electrochemical energy storage devices. This study shows that MOFs made as nanocrystals (nMOFs) can be doped with graphene and successfully incorporated into devices to function as supercapacitors. A series of 23 different nMOFs with multiple organic functionalities and metal ions, differing pore sizes and shapes, discrete and infinite metal oxide backbones, large and small nanocrystals, and a variety of structure types have been prepared and examined. Several members of this series give high capacitance; in particular, a zirconium MOF exhibits exceptionally high capacitance. It has the stack and areal capacitance of 0.64 and 5.09 mF cm(-2), about 6 times that of the supercapacitors made from the benchmark commercial activated carbon materials and a performance that is preserved over at least 10000 charge/discharge cycles.
The increasing demands on high performance energy storage systems have raised a new class of devices, so-called lithium ion capacitors (LICs). As its name says, LIC is an intermediate system between lithium ion batteries and supercapacitors, designed for taking advantages of both types of energy storage systems. Herein, as a quest to improve the Li storage capability compared to that of other existing carbon nanomaterials, we have developed extrinsically defective multiwall carbon nanotubes by nitrogen-doping. Nitrogen-doped carbon nanotubes contain wall defects through which lithium ions can diffuse so as to occupy a large portion of the interwall space as storage regions. Furthermore, when integrated with 3 nm nickel oxide nanoparticles for a further capacity boost, nitrogen doping enables unprecedented cell performance by engaging anomalous electrochemical phenomena such as nanoparticles division into even smaller ones, their agglomeration-free diffusion between nitrogen-doped sites as well as capacity rise with cycles. The final cells exhibit a capacity as high as 3500 mAh/g, a cycle life of greater than 10,000 times, and a discharge rate capability of 1.5 min while retaining a capacity of 350 mAh/g.
A series of three-dimensional (3D) extended metal catecholates (M-CATs) was synthesized by combining the appropriate metal salt and the hexatopic catecholate linker, H6THO (THO(6-) = triphenylene-2,3,6,7,10,11-hexakis(olate)) to give Fe(THO)·Fe(SO4) (DMA)3, Fe-CAT-5, Ti(THO)·(DMA)2, Ti-CAT-5, and V(THO)·(DMA)2, V-CAT-5 (where DMA = dimethylammonium). Their structures are based on the srs topology and are either a 2-fold interpenetrated (Fe-CAT-5 and Ti-CAT-5) or noninterpenetrated (V-CAT-5) porous anionic framework. These examples are among the first catecholate-based 3D frameworks. The single crystal X-ray diffraction structure of the Fe-CAT-5 shows bound sulfate ligands with DMA guests residing in the pores as counterions, and thus ideally suited for proton conductivity. Accordingly, Fe-CAT-5 exhibits ultrahigh proton conductivity (5.0 × 10(-2) S cm(-1)) at 98% relative humidity (RH) and 25 °C. The coexistence of sulfate and DMA ions within the pores play an important role in proton conductivity as also evidenced by the lower conductivity values found for Ti-CAT-5 (8.2 × 10(-4) S cm(-1) at 98% RH and 25 °C), whose structure only contained DMA guests.
We report electrochemical performance of a TiO2 combined with a nitrogen-doped open channeled graphene anode composite for sodium ion batteries.
The electrochemical N 2 reduction reaction has attracted interest as a potential alternative to the Haber−Bosch process, but a significantly low conversion efficiency and a significantly low ammonia production rate stimulate the need for alternatives. Here, we represent the electrochemical reduction of nitric oxide (NO) on a nanostructured Ag electrode in combination with a rationally designed electrolyte containing the EDTA−Fe 2+ metal complex (EFeMC), which results in an ∼100% efficiency for NH 3 with a current density of 50 mA/cm 2 at −0.165 V RHE , without any degradation in catalytic activity or product selectivity up to 120 h. Economic analysis using itemized cost estimation predicted that the synthesis of ammonia from NO reduction in an EFeMC-designed electrolyte can be market competitive at an electricity price of $0.03 kWh −1 with a current density of >125 mA/cm 2 . Therefore, this approach opens an entirely new avenue of renewable electricitydriven ammonia synthesis.
Vanadium pentoxide (V 2 O 5 ) has received considerable attention as a lithium battery cathode because its specific capacity (>250 mA h g À1 ) is higher than those (<170 mA h g À1 ) of most commercial cathode materials. Despite this conspicuous advantage, V 2 O 5 has suffered from limited cycle life, typically below a couple of hundred cycles due to the agglomeration of its particles. Once V 2 O 5 particles are agglomerated, the insulating phases continuously expand to an extent that ionic and electronic conduction is severely deteriorated, leading to the significant capacity decay. In this study, in order to overcome the agglomeration issue, the electrodes were uniquely designed such that ultrathin V 2 O 5 nanowires were uniformly incorporated into graphene paper. In this composite structure, the dispersion of V 2 O 5 nanowires was preserved in a robust manner, and, as a result, enabled substantially improved cycle life: decent specific capacities were preserved over 100 000 cycles, which are 2-3 orders of magnitude larger than those of typical battery materials.
Water is a significant natural resource for humans. As such, wastewater containing heavy metals is seen as a grave problem for the environment. Currently, adsorption is one of the common methods used for both water purification and wastewater treatment. Adsorption relies on the physical and chemical interactions between heavy metal ions and adsorbents. Adsorptive membranes (AMs) have demonstrated high effectiveness in heavy metal removal from wastewater owing to their exclusive structural properties. This article examines the applications of adsorptive membranes such as polymeric membranes (PMs), polymer-ceramic membranes (PCMs), electrospinning nanofiber membranes (ENMs), and nano-enhanced membranes (NEMs), which demonstrate high selectivity and adsorption capacity for heavy metal ions, as well as both advantages and disadvantages of each one all, are summarized and compared shortly. Moreover, the general theories for both adsorption isotherms and adsorption kinetics are described briefly to comprehend the adsorption process. This work will be valuable to readers in understanding the current applications of various AMs and their mechanisms in heavy metal ion adsorption, as well as the recycling methods in heavy ions desorption process are summarized and described clearly. Besides, the influences of morphological and chemical structures of AMs are presented and described in detail as well.
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