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  1. Nargatti KI, Ahankari SS, Dizon JRC, Subramaniam RT
    ACS Omega, 2024 Mar 12;9(10):11730-11737.
    PMID: 38496988 DOI: 10.1021/acsomega.3c09139
    The agglomeration of reduced graphene oxide (rGO) in water makes the development of rGO inks for supercapacitor printing challenging. Cellulose nanofiber (CNF), a biodegradable and renewable nanomaterial, can act as a nanospacer, preventing the agglomeration and restacking of rGO flakes. In this work, rGO/CNF films were fabricated using an environmentally friendly water-based rGO/CNF ink. In the absence of an additional binder/surfactant, the rGO/CNF films demonstrated remarkably enhanced hydrophilicity while retaining good electrical conductivity. The concentration of CNF was varied to observe the variation in the electrochemical performance. At a current density of 1 mA/cm2, the rGO/CNF-15 film exhibited a maximum areal capacitance of 98.61 mF/cm2, closely matching that of pure rGO films. Because of its excellent electrical performance, ease of manufacturing, and environmental friendliness, this water-based rGO/CNF ink may have promising applications in the printing of supercapacitor electrodes.
  2. Periasamy V, Elumalai PNN, Talebi S, Subramaniam RT, Kasi R, Iwamoto M, et al.
    RSC Adv, 2023 Feb 14;13(9):5744-5752.
    PMID: 36816072 DOI: 10.1039/d3ra00457k
    Conventional three-electrode systems used in electrochemical measurement demand time-consuming and maintenance intensive procedures to enable accurate and repeatable electrochemical measurements. Traditionally, different metal configurations are used to establish the electrochemical gradient required to acquire the redox activity, and vary between different electrochemical measurement platforms. However, in this work, we report using the same metal (gold) for the counter, working and reference electrodes fabricated on a miniaturized printed circuit board (PCB) for a much simpler design. Potassium ferricyanide, widely used as a redox probe for electrochemical characterization, was utilized to acquire cyclic voltametric profiles using both the printed circuit board-based gold-gold-gold three-electrode and conventional three-electrode systems (glassy carbon electrode or graphite foil as the working electrode, platinum wire as the counter electrode, and Ag/AgCl as the reference electrode). The results show that both types of electrode systems generated similar cyclic voltammograms within the same potential window (-0.5 to +0.7 V). However, the novel PCB-based same-metal three-electrode electrochemical cell only required a few activation cycles and exhibited impressive cyclic voltametric repeatability with higher redox sensitivity and detection window, while using only trace amounts of solutions/analytes.
  3. Liu L, Bashir S, Ling GZ, Hoe LK, Liew J, Kasi R, et al.
    ChemSusChem, 2024 Jan 22;17(2):e202300876.
    PMID: 37695539 DOI: 10.1002/cssc.202300876
    Carbon-based materials have emerged as promising anodes for sodium-ion batteries (SIBs) due to the merits of cost-effectiveness and renewability. However, the unsatisfactory performance has hindered the commercialization of SIBs. During the past decades, tremendous attention has been put into enhancing the electrochemical performance of carbon-based anodes from the perspective of improving the compatibility of electrolytes and electrodes. Hence, a systematic summary of strategies for optimizing electrolytes between hard carbon, graphite, and other structural carbon anodes of SIBs is provided. The formulations and properties of electrolytes with solvents, salts, and additives added are comprehensively presented, which are closely related to the formation of solid electrolyte interface (SEI) and crucial to the sodium ion storage performance. Cost analysis of commonly used electrolytes has been provided as well. This review is anticipated to provide guidance in future rational tailoring of electrolytes with carbon-based anodes for sodium-ion batteries.
  4. Talebi S, Daraghma SMA, Subramaniam RT, Bhassu S, Gnana Kumar G, Periasamy V
    ACS Omega, 2020 Apr 14;5(14):7802-7808.
    PMID: 32309689 DOI: 10.1021/acsomega.9b03831
    Proteins have been increasingly suggested as suitable candidates for the fabrication of biological computers and other biomolecular-based electronic devices mainly due to their interesting structure-related intrinsic electrical properties. These natural biopolymers are environmentally friendly substitutes for conventional inorganic materials and find numerous applications in bioelectronics. Effective manipulation of protein biomolecules allows for accurate fabrication of nanoscaled device dimensions for miniaturized electronics. The prerequisite, however, demands an interrogation of its various electronic properties prior to understanding the complex charge transfer mechanisms in protein molecules, the knowledge of which will be crucial toward development of such nanodevices. One significantly preferred method in recent times involves the utilization of solid-state sensors where interactions of proteins could be investigated upon contact with metals such as gold. Therefore, in this work, proteins (hemoglobin and collagen) were integrated within a two-electrode system, and the resulting electronic profiles were investigated. Interestingly, structure-related electronic profiles representing semiconductive-like behaviors were observed. These characteristic electronic profiles arise from the metal (Au)-semiconductor (protein) junction, clearly demonstrating the formation of a Schottky junction. Further interpretation of the electronic behavior of proteins was done by the calculation of selected solid-state parameters. For example, the turn-on voltage of hemoglobin was measured to occur at a lower turn-on voltage, indicating the possible influence of the hem group present as a cofactor in each subunit of this tetrameric protein.
  5. Saidi NM, Omar FS, Numan A, Apperley DC, Algaradah MM, Kasi R, et al.
    ACS Appl Mater Interfaces, 2019 Aug 21;11(33):30185-30196.
    PMID: 31347822 DOI: 10.1021/acsami.9b07062
    To overcome the critical limitations of liquid-electrolyte-based dye-sensitized solar cells, quasi-solid-state electrolytes have been explored as a means of addressing long-term device stability, albeit with comparatively low ionic conductivities and device performances. Although metal oxide additives have been shown to augment ionic conductivity, their propensity to aggregate into large crystalline particles upon high-heat annealing hinders their full potential in quasi-solid-state electrolytes. In this work, sonochemical processing has been successfully applied to generate fine Co3O4 nanoparticles that are highly dispersible in a PAN:P(VP-co-VAc) polymer-blended gel electrolyte, even after calcination. An optimized nanocomposite gel polymer electrolyte containing 3 wt % sonicated Co3O4 nanoparticles (PVVA-3) delivers the highest ionic conductivity (4.62 × 10-3 S cm-1) of the series. This property is accompanied by a 51% enhancement in the apparent diffusion coefficient of triiodide versus both unmodified and unsonicated electrolyte samples. The dye-sensitized solar cell based on PVVA-3 displays a power conversion efficiency of 6.46% under AM1.5 G, 100 mW cm-2. By identifying the optimal loading of sonochemically processed nanoparticles, we are able to generate a homogenous extended particle network that effectively mobilizes redox-active species through a highly amorphous host matrix. This effect is manifested in a selective 51% enhancement in photocurrent density (JSC = 16.2 mA cm-2) and a lowered barrier to N719 dye regeneration (RCT = 193 Ω) versus an unmodified solar cell. To the best of our knowledge, this work represents the highest known efficiency to date for dye-sensitized solar cells based on a sonicated Co3O4-modified gel polymer electrolyte. Sonochemical processing, when applied in this manner, has the potential to make meaningful contributions toward the ongoing mission to achieve the widespread exploitation of stable and low-cost dye-sensitized solar cells.
  6. Wang J, Shao Y, Ma Y, Zhang D, Aziz SB, Li Z, et al.
    ACS Nano, 2024 Apr 09;18(14):10230-10242.
    PMID: 38546180 DOI: 10.1021/acsnano.4c00599
    The realization of sodium-ion devices with high-power density and long-cycle capability is challenging due to the difficulties of carrier diffusion and electrode fragmentation in transition metal selenide anodes. Herein, a Mo/W-based metal-organic framework is constructed by a one-step method through rational selection, after which MoWSe/C heterostructures with large angles are synthesized by a facile selenization/carbonization strategy. Through physical characterization and theoretical calculations, the synthesized MoWSe/C electrode delivers obvious structural advantages and excellent electrochemical performance in an ethylene glycol dimethyl ether electrolyte. Furthermore, the electrochemical vehicle mechanism of ions in the electrolyte is systematically revealed through comparative analyses. Resultantly, ether-based electrolytes advantageously construct stable solid electrolyte interfaces and avoid electrolyte decomposition. Based on the above benefits, the Na half-cell assembled with MoWSe/C electrodes demonstrated excellent rate capability and a high specific capacity of 347.3 mA h g-1 even after cycling 2000 cycles at 10 A g-1. Meanwhile, the constructed sodium-ion capacitor maintains ∼80% capacity retention after 11,000 ultralong cycles at a high-power density of 3800 W kg-1. The findings can broaden the mechanistic understanding of conversion anodes in different electrolytes and provide a reference for the structural design of anodes with high capacity, fast kinetics, and long-cycle stability.
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