Efficient Redox Research Articles

The Critical Analysis of Membranes toward Sustainable and Efficient Vanadium Redox Flow Batteries.

Vanadium redox flow batteries (VRFB) are a promising technology for large-scale storage of electrical energy, combining safety, high capacity, ease of scalability, and prolonged durability; features which have triggered their early commercial implementation. Furthering the deployment of VRFB technologies requires addressing challenges associated to a pivotal component: the membrane. Examples include vanadium crossover, insufficient conductivity, escalated costs, and sustainability concerns related to the widespread adoption of perfluoroalkyl-based membranes, e.g., perfluorosulfonic acid (PFSA). Herein, recent advances in high-performance and sustainable membranes for VRFB, offering insights into prospective research directions to overcome these challenges, are reviewed. The analysis reveals the disparities and trade-offs between performance advances enabled by PFSA membranes and composites, and the lack of sustainability in their final applications. The potential of PFSA-free membranes and present strategies to enhance their performance are discussed. This study delves into vital membrane parameters to enhance battery performance, suggesting protocols and design strategies to achieve high-performance and sustainable VRFB membranes.

Modulating electronic structure of Fe site by adjacent Cu site through orbital coupling in Cu-Fe2O3 catalyst derived from Fenton sludge quenching

The incorporation of specific atoms into catalysts derived from Fenton sludge has the potential to regulate active site for promoting peroxymonosulfate (PMS) activation. Here, quenching technology was employed in this study to facilitate the production of a highly active Fe2O3-based catalyst from Fenton sludge. In this process, Cu atoms effectively substituted Fe atoms and regulated the local electronic structure of neighbouring Fe sites, thereby enhancing the catalytic performance in PMS activation for the degradation of Levofloxacin (LEVO) in wastewater. The strong orbital coupling between Fe and Cu, as confirmed by comprehensive characterization and density functional theory (DFT), facilitated the delocalization of d-orbital electrons, thereby enabling efficient electron transfer and redox cycling of Cu2+/Cu+ and Fe3+/Fe2+. This allowed degradation reaction to proceed continuously. The present study will offer a novel approach to the design of Fenton sludge derived catalysts, thereby expanding the utilization of quenching chemistry in solid waste recycling.

Phosphotungstic Acid Clusters Decorated Znln2S4 Nanoflowers as Molecular-Scale S-Scheme Heterojunctions for Simultaneous H2 Evolution and Benzyl Alcohol Upgrading.

Simultaneous utilization of photogenerated electrons and holes to achieve overall redox reactions is attractive but still far from practical application. The emerging step (S)-scheme mechanism has proven to be an ideal approach to inhibit charge recombination and supply photoinduced charges with highest redox potentials. Herein, a hierarchical phosphotungstic acid (H3PW12O40, HPW)@Znln2S4 (ZISW) heterojunction was prepared through one-pot hydrothermal method for simultaneous hydrogen (H2) evolution and benzyl alcohol upgrading. The fabricated HPW-based heterojunctions indicated much enhanced visible-light absorption, promoted photogenerated charge transfer and inhibited charge recombination, owing to hierarchical architecture based on visible-light responsive Znln2S4 microspheres, and S-scheme charge transfer pathway. The S-scheme mechanism was further verified by free-radical trapping electron spin resonance (ESR) spectra. Moreover, the wettability of composite heterojunction was improved by the modification of hydrophilic HPW, contributing to gaining active hydrogen (H+) from water sustainably. The optimal ZISW-30 heterojunction photocatalyst indicated an enhanced hydrogen evolution rate of 27.59 mmol g-1 h-1 in benzyl alcohol (10 vol. %) solution under full-spectrum irradiation, along with highest benzaldehyde production rate is 8.32 mmol g-1 h-1. This work provides a promising guideline for incorporating HPW into S-scheme heterojunctions to achieve efficient overall redox reactions.

Adaptability of Heteropolytungstate Anions as Efficient Anode Redox Mediators in Redox Flow Polymer Electrolyte Fuel Cells.

Heteropolyanions (HPAs) are known as the candidate for an anode redox mediator for redox flow polymer electrolyte fuel cells (PEFCs). The electrochemical properties of HPAs differ depending on the transition elements and heteroatoms in HPAs. For example, heteropolytungstate anions (W-HPAs), in which the transition element is tungsten, have a lower one-electron reduction potential than other HPAs. Therefore, it has been reported that redox flow PEFCs adapted with W-HPAs exhibit high power generation performance. On the other hand, studies on the heteroatoms of HPAs are limited only to electrochemical properties, and statistical and comprehensive studies on the power generation performance of redox flow PEFCs are lacking. Thus, it is beneficial to clarify the optimal heteroatom in order to design anolytes suitable for redox flow PEFCs. In this study, heteropolytungstate anions with different heteroatoms were adapted as anodic redox mediators in a redox flow PEFC. In power generation tests, the redox flow PEFC with an anolyte of zinctungstate anion showed the highest performance. Zinctungstate anion exhibited the fastest reduction and oxidation rates among the W-HPAs investigated in this study.

Chemomechanics Engineering Promotes the Catalytic Activity of Spinel Oxides for Sulfur Redox Reaction

AbstractCooperative catalysis is a promising approach to enhance the sluggish redox kinetics of lithium polysulfides (LiPSs) for practical lithium–sulfur (Li–S) batteries. However, the elusory synergistic effect among multiple active sites makes it challenging to accurately customize the electronic structure of catalysts. Herein, a strategy of precisely tailoring eg orbitals of spinel oxides through chemomechanics engineering is porposed to regulate LiPSs retention and catalysis. By manipulating the regulable cations in MnxCo3‐xO4, it is theoretically and experimentally revealed that the lattice strain induced by the Jahn–Teller active and high‐spin Mn3+ at octahedral (Oh) sites can increase the eg occupancy of low‐spin Co3+Oh, which effectively regulates the chemical affinity toward LiPSs and establishes an unblocked channel for intrinsic charge transfer. This leads to a volcano‐type correlation between the eg occupancy at Oh sites and sulfur redox activity. Benefitting from the cooperative catalysis of dual‐active sites, MnCo2O4 with an average eg occupancy of 0.45 affords the most appropriate adsorption strength and rapid redox kinetics toward LiPSs, leading to remarkable rate performance and capacity retention for the assembled Li–S batteries. This work demonstrates the promise of chemomechanics engineering for optimizing the eg occupancy to achieve efficient sulfur redox catalysts.

Integration of Co Single Atoms and Ni Clusters on Defect-Rich ZrO2 for Strong Photothermal Coupling Boosts Photocatalytic CO2 Reduction.

We report a solvothermal method for the synthesis of an oxygen vacancy-enriched ZrO2 photocatalyst with Co single atoms and Ni clusters immobilized on the surface. This catalyst presents superior performance for the reduction of CO2 in H2O vapor, with a CO yield reaching 663.84 μmol g-1 h-1 and a selectivity of 99.52%. The total solar-to-chemical energy conversion efficiency is up to 0.372‰, which is among the highest reported values. The success, on one hand, depends on the Co single atoms and Ni clusters for both extended spectrum absorption and serving as dual-active centers for CO2 reduction and H2O dissociation, respectively; on the other hand, this is attributed to the enhanced photoelectric and thermal effect induced by concentrated solar irradiation. We demonstrate that an intermediate impurity state is formed by the hybridization of the d-orbital of single-atom Co with the molecular orbital of H2O, enabling visible-light-driven excitation over the catalyst. In addition, Ni clusters play a crucial role in altering the adsorption configuration of CO2, with the localized surface plasmon resonance effect enhancing the activation and dissociation of CO2 induced by visible-near-infrared light. This study provides valuable insights into the synergistic effect of the dual cocatalyst toward both efficient photothermal coupling and surface redox reactions for solar CO2 reduction.

Enhanced Energy Storage Performance through Controlled Composition and Synthesis of 3D Mixed Metal-Oxide Microspheres.

Binary transition metal oxide complexes (BTMOCs) in three-dimensional (3D) layered structures show great promise as electrodes for supercapacitors (SCs) due to their diverse oxidation states, which contribute to high specific capacitance. However, the synthesis of BTMOCs with 3D structures remains challenging yet crucial for their application. In this study, we present a novel approach utilizing a single-step hydrothermal technique to fabricate flower-shaped microspheres composed of a NiCo-based complex. Each microsphere consists of nanosheets with a mesoporous structure, enhancing the specific surface area to 23.66 m2 g-1 and facilitating efficient redox reactions. When employed as the working electrode for supercapacitors, the composite exhibits remarkable specific capacitance, achieving 888.8 F g-1 at 1 A g-1. Furthermore, it demonstrates notable electrochemical stability, retaining 52.08% capacitance after 10,000 cycles, and offers a high-power density of 225 W·kg-1, along with an energy density of 25 Wh·kg-1, showcasing its potential for energy storage applications. Additionally, an aqueous asymmetric supercapacitor (ASC) was assembled using NiCo microspheres-based complex and activated carbon (AC). Remarkably, the NiCo microspheres complex/AC configuration delivers a high specific capacitance of 250 F g-1 at 1 A g-1, with a high energy density of 88 Wh kg-1, for a power density of 800 W kg-1. The ASC also exhibits excellent long-term cyclability with 69% retention over 10,000 charge-discharge cycles. Furthermore, a series of two ASC devices demonstrated the capability to power commercial blue LEDs for a duration of at least 40 s. The simplicity of the synthesis process and the exceptional performance exhibited by the developed electrode materials hold considerable promise for applications in energy storage.

Rational sonochemical engineering of Ag2CrO4/g-C3N4 heterojunction for eradicating RhB dye under full broad spectrum

In this novel research, S-scheme Ag2CrO4/g-C3N4 heterojunctions were generated by sonochemical hybridization of different compositions of Ag2CrO4 nanoparticles [EVB = +2.21 eV] and g-C3N4 sheets [ECB = −1.3 eV] for destructing RhB dye under artificial solar radiation. The as-synthesized nanocomposites were subjected to X-ray diffraction [XRD], diffuse reflectance spectrum [DRS], X-ray photoelectron spectroscopy [XPS], N2-adsorption-desorption isotherm, photoluminescence [PL] and high resolution transmission electron microscope [HRTEM] analysis to explore the interfacial interactions between g-C3N4 sheets and Ag2CrO4 nanoparticles. Spherical Ag2CrO4 nanoparticles deposited homogeneously on the wrinkles points of g-C3N4 sheets at nearly equidistant from each other facilitating the uniform absorption of solar radiations. The absorbability of solar radiations was enhanced by introducing 20 wt % Ag2CrO4 on g-C3N4 sheets. The surface area of g-C3N4 sheets was reduced from 37.5 to 16.4 m2/g and PL signal intensity diminished by 80 % implying the successful interfacial interaction between Ag2CrO4 nanoparticles and g-C3N4 sheets. The photocatalytic performance of heterojunctions containing 20 % Ag2CrO4 and 80 % g-C3N4 destructed 96 % of RhB dye compared with 60 and 33 % removal on the surface of pristine g-C3N4 sheets and Ag2CrO4, respectively. Benzoquinone and ammonium oxalate are strongly scavenged the dye decomposition revealing the strong influence of valence band holes of Ag2CrO4 and superoxide radicals in destructing RhB dye under solar radiations. S-scheme charge transportation mechanism was suggested rather than type II heterojunction on the light of scavenger trapping experiments results and PL spectrum of terephthalic acid. Overall, this research work illustrated the manipulation of novel S-scheme heterojunction with efficient redox power for destructing various organic pollutants persisted in water resources.

A Water-in-Salt Electrolyte for Room-Temperature Fluoride-Ion Batteries Based on a Hydrophobic-Hydrophilic Salt.

Realizing room-temperature, efficient, and reversible fluoride-ion redox is critical to commercializing the fluoride-ion battery, a promising post-lithium-ion battery technology. However, this is challenging due to the absence of usable electrolytes, which usually suffer from insufficient ionic conductivity and poor (electro)chemical stability. Herein we report a water-in-salt (WIS) electrolyte based on the tetramethylammonium fluoride salt, an organic salt consisting of hydrophobic cations and hydrophilic anions. The new WIS electrolyte exhibits an electrochemical stability window of 2.47 V (2.08-4.55 V vs Li+/Li) with a room-temperature ionic conductivity of 30.6 mS/cm and a fluoride-ion transference number of 0.479, enabling reversible (de)fluoridation redox of lead and copper fluoride electrodes. The relationship between the salt property, the solvation structure, and the ionic transport behavior is jointly revealed by computational simulations and spectroscopic analysis.

High Entropy Alloys Enable Durable and Efficient Lithium-Mediated CO2 Redox Reactions.

Designing electrocatalysts with high activity and durability for multistep reduction and oxidation reactions is challenging. High-entropy alloys (HEAs) are intriguing due to their tunable geometric and electronic structure through entropy effects. However, understanding the origin of their exceptional performance and identifying active centers is hindered by the diverse microenvironment in HEAs. Herein, NiFeCoCuRu HEAs designed with an average diameter of 2.17 nm, featuring different adsorption capacities for various reactants and intermediates in Li-mediated CO2 redox reactions, are introduced. The electronegativity-dependent nature of NiFeCoCuRu HEAs induces significant charge redistribution, shifting the d-band center closer to Fermi level and forming highly active clusters of Ru, Co, and Ni for Li-based compounds adsorptions. This lowers energy barriers and simultaneously stabilizes *LiCO2 and LiCO3+CO intermediates, enhancing the efficiency of both CO2 reduction and Li2CO3 decomposition over extended periods. This work provides insights into specific active site interactions with intermediates, highlighting the potential of HEAs as promising catalysts for intricate CO2 redox reactions.

Crafting defective ZnO nanoparticles: A green synthesis for enhanced photocatalytic degradation of organic pollutants

Surface defect engineering is a promising strategy for enhancing the number of surface-active sites to facilitate efficient redox reactions that occur on the surface of a photocatalyst. A green approach was employed to prepare urea- and choline-chloride-based deep eutectic solvent (DES) for the synthesis of ZnO/Zn(OH)2 supported by a DES complex (Zn precursor). Surface defects on ZnO nanoparticles (NPs) were tailored by decomposing the Zn precursor in air. In addition, calcination improved the crystallinity and surface-active sites of the defective ZnO by creating surface oxygen vacancies (Vo). The appearance of an Electron paramagnetic resonance peak at a g value of 1.96 confirms the formation of single-charged Vo defects on the surface of ZnO. The photocatalyst prepared at a reaction bath temperature of 75 °C (Vo-ZnO-75) showed the highest photocatalytic activity. The observed green emission in the photoluminescence spectrum and X-ray photoelectron spectroscopy analysis suggests the formation of defects on the ZnO surface. Consequently, Vo-ZnO-75 enhanced surface donor density (14.4×1020 cm−3) and lower charge transfer resistance (88.89 × 103 Ω). The optimized photocatalyst of Vo-ZnO-75 has 94% removal efficiency for rhodamine B degradation within 60 min. This study sheds new light on the development of an efficient and eco-friendly approach for preparing defective ZnO NPs for photocatalytic applications.

Uncovering the discharge structure evolution and electrochemical performance of sulfur cathode host 2D-Fe0.89M0.11S2 (M = Ti, V)

The sulfur cathode host materials with excellent electronic conductivity and catalytic performance are the key to highly efficient Li-S redox chemistry for the lithium‑sulfur batteries (LSBs). Although 2D-FeS2 as sulfur cathode host shows high theoretical capacity and flat voltage plateaus, the Li-S redox chemical reaction mechanism is still unclear. By using the first-principles calculations, the formation energy, working voltage, theoretical capacity, electronic conductivity, adsorption performance, electrocatalytic mechanism, Li+ diffusion and Li2S decomposition barrier of 2D-FeS2 and M (M = Ti, V) doped 2D-FeS2 are investigated to evaluate its physicochemical properties. 2D-Fe0.89M0.11S2 is thermodynamically stable due to its low lattice distortion, formation energy and mixing enthalpy. The charging voltage of 2D-Fe0.89Ti0.11S2 is better than that of 2D-Fe0.89V0.11S2, but the charging voltage step is reversed. The electrical conductivity of 2D-Fe0.89M0.11S2 is superior to 2D-FeS2. The closer the highest molecule occupied orbitals is to the Fermi level, the lower the discharge voltage will be. 2D-Fe0.89V0.11S2 and its discharge structure 2D-Li2Fe0.89V0.11S2 improve the efficiency of catalytic reduction of Li2S4. 2D-Fe0.89V0.11S2 has low Li+ diffusion and decomposition barrier of Li2S, which has potential application value in promoting the Li-S redox chemistry. This work deepens the understanding of the doping strategy and provides theoretical guidance for the design and development of sulfur cathode host to improve the Li-S redox chemistry.

S-scheme NiO/C3N5 heterojunctions with enhanced interfacial electric field for boosting photothermal-assisted photocatalytic H2 and H2O2 production

Heterostructured visible-light-responsive photocatalysts represent a prospective approach to achieve efficient solar-to-chemical energy conversion. Herein, we propose a facile self-assembly technique to synthesize NiO nanoparticles/C3N5 nanosheets (NOCN) heterojunctions for hydrogen (H2) evolution catalysis and hydrogen peroxide (H2O2) production under visible light. In this regard, the black NiO nanoparticles (NPs) were tightly anchored on the surface of C3N5 nanosheets (CNNS) to construct S-scheme NOCN heterojunction, enabling efficient charge separation and high redox capability. Obtained results elucidated that the incorporated NiO NPs significantly promote light-harvesting efficiency and photo-to-thermal capacity over the NOCN composites. The enhanced photothermal effect facilitates the charge carrier transfer rate across the heterojunction and boosts the surface reaction kinetics. Accordingly, the photocatalytic performances of CNNS for H2 release and H2O2 production can be manipulated by introducing NiO NPs. The modified photocatalytic properties of NOCN composites are ascribed to the synergistic effects of all integrated components and the S-scheme heterojunction formation. Impressively, the high H2 evolution photocatalysis efficiency of NOCN nano-catalysts in seawater certifies their potential environmental applicability. Among all, the 12-NOCN nano-catalyst exhibits a higher photocatalytic efficiency for H2 release (112.2 μmol∙g−1∙h−1) and H2O2 production (91.2 μmol∙L−1∙h−1). Besides, the 12-NOCN nano-catalyst reveals excellent recyclability and structural stability. Additionally, the possible mechanism for photothermal-assisted photocatalysis is proposed. This work affords a feasible pathway to design photothermal-assisted S-scheme heterojunctions for diverse photocatalytic applications.

Bismuth nanoparticles anchored on n-doped graphite felts to give stable and efficient iron-chromium redox flow batteries

Bismuth nanoparticles anchored on n-doped graphite felts to give stable and efficient iron-chromium redox flow batteries

Oxygen-vacancies rich CuFe2O4 catalyst as efficient peroxymonosulfate activator for enhanced oxytetracycline degradation: Performance and mechanism

Peroxymonosulfate (PMS) based advanced oxidation methods have gained attention for eliminating antibiotics like oxytetracycline (OTC) from wastewater. This study presents an innovative approach by incorporating oxygen vacancies (OVs) into CuFe2O4 to create OVs-CuFe2O4 materials. Compared to traditional CuFe2O4, OVs-CuFe2O4 offered superior catalytic performance due to its surface-rich OVs promoting rapid conversion of oxygen and efficient metal redox of Fe(Ⅱ)/Fe(Ⅲ) and Cu(Ⅰ)/Cu(Ⅱ). OVs-CuFe2O4/PMS achieved impressive 95.7 % OTC removal in 45 min with a rate constant of 0.107 min−1, which was 3.87 times of CuFe2O4/PMS. The OVs-CuFe2O4/PMS system exhibited a broad pH tolerance range of 3 to 11 with OTC removal efficiency above 89.3 %. The OVs-CuFe2O4/PMS system produced various free radicals and non-radical for OTC degradation. The OVs-CuFe2O4 also has good stability with removal efficiency of 81.9 % at fourth cycle. This research gives a strategy to construct oxygen vacancies enrich catalysts for efficient activation of PMS and treatment of antibiotics wastewater.

Extrinsic Pseudocapacitive NiSe/rGO/g-C3N4 Nanocomposite for High-Performance Hybrid Supercapacitors.

Battery-type materials with ultrahigh energy density show great potential for hybrid supercapacitors (HSCs). In this work, we have developed a nickel selenide (NiSe)/reduced graphene oxide (rGO)/graphitic carbon nitride (g-C3N4) ternary composite as a promising positive electrode for hybrid supercapacitors (HSCs). The extended π-conjugated planar layers of g-C3N4 promote strong interconnectivity with rGO, which further enhances surface area, surface free energy, and efficient electron/ionic path. Additionally, it establishes clear ion diffusion pathways, serving as ion reservoirs during charge and discharge and facilitating efficient redox reactions. As a result, the NiSe/g-C3N4/rGO nanocomposite electrode displayed a specific capacity of 412.6 mA h g-1 at 1 A g-1. Later, the HSC device was assembled using the nanocomposite as the positive electrode and activated carbon as the negative electrode, which delivered an energy density of 65.2 Wh kg-1 at a power density of 750 W kg-1. Notably, the HSC device maintained excellent cyclic stability, preserving 93.3% of its initial performance and Coulombic efficiency of 86.6% for 10,000 charge-discharge cycles at 5 A g-1. These findings underscore the potential utility of NiSe/g-C3N4/rGO as a versatile and effective electrode material for the strategic development of HSC devices.

Multifunctional enhanced energy density of flexible wide-temperature supercapacitors based on MXene/PANI conductive hydrogel

Conducting polymer-based conductive hydrogels can offer adjustable electronic characteristics and superior mechanical performance, thus holding significant promise for flexible supercapacitors. However, some of such hydrogel electrodes still suffer from inferior stability, unsatisfactory energy density, and narrow temperature tolerance, which limit their widespread use in flexible supercapacitors. Herein, polyaniline was coated on the surface of Ti3C2Tx MXene flakes by in-situ chemical oxidative polymerization of aniline monomer pre-assembled on the MXene surface. The resulting MXene/PANI conductive nanofillers, Fe3+ ions, and phytic acid were introduced into the gelatin/polyacrylamide hydrogel scaffold to form highly stretchable MPGP-Fey hydrogel electrodes. Benefiting from the highly electrochemical activity of MXene/PANI conductive nanocomposite, efficient redox transition of Fe3+/Fe2+, and high open structure, the assembled all-gel symmetrical MPGP-Fey supercapacitors can achieve a maximum specific capacitance of 847 mF/cm2, an impressive energy density of 71.8 μWh/cm2, and an exceptional cyclic stability, retaining 95 % capacitance retention after 5000 cycles. The phytic acid is advantageous in lowering the freezing points of both the hydrogel electrode and electrolyte layer. The developed supercapacitors demonstrate promising temperature-adaptive properties over a wide range of −30 ∼ 90 °C. When operated at −30 °C, an impressive stable output with long-term stability of 93 % retention are achieved. With the merits of good processability, high flexibility and stretchability, the present device can serve as an optimal energy source for powering diverse electronic components in practical applications.

Synergistic integration of Ni-metal organic framework/SnS2 nanocomposite and nickel foam electrode for ultrasensitive and selective electrochemical detection of albumin in simulated human blood serum

Albumin is a vital blood protein responsible for transporting metabolites and drugs throughout the body and serves as a potential biomarker for various medical conditions, including inflammatory, cardiovascular, and renal issues. This report details the fabrication of Ni-metal organic framework/SnS2 nanocomposite modified nickel foam electrochemical sensor for highly sensitive and selective non enzymatic detection of albumin in simulated human blood serum samples. Ni-metal organic framework/SnS2 nanocomposite was synthesized using solvothermal technique by combining Ni-metal–organic framework (MOF) with conductive SnS2 leading to the formation of a highly porous material with reduced toxicity and excellent electrical conductivity. Detailed surface morphology and chemical bonding of the Ni-MOF/SnS2 nanocomposite was studied using scanning electron microscopy, transmission electron microscopy, Fourier transform infra-red, and Raman analysis. The Ni-MOF/SnS2 nanocomposite coated on Ni foam electrode demonstrated outstanding electrochemical performance, with a low limit of detection (0.44 μM) and high sensitivity (1.3 μA/pM/cm2) throughout a broad linear range (100 pM–10 mM). The remarkable sensor performance is achieved through the synthesis of a Ni-MOF/SnS2 nanocomposite, enhancing electrocatalytic activity for efficient albumin redox reactions. The enhanced performance can be attributed due to the structural porosity of nickel foam and Ni-metal organic framework, which favours increased surface area for albumin interaction. The presence of SnS2 shows stability in acidic and neutral solutions due to high surface to volume ratio which in turn improves sensitivity of the sensing material. The sensor exhibited commendable selectivity, maintaining its performance even when exposed to potential interfering substances like glucose, ascorbic acid, K+, Na+, uric acid, and urea. The sensor effectively demonstrates its accuracy in detecting albumin in real samples, showcasing substantial recovery percentages of 105.1%, 110.28%, and 91.16%.

Defect-rich high-entropy spinel oxide catalyst for efficient vanadium redox flow battery

High entropy oxides (HEO) represent an innovative group of materials stabilized by incorporating configurational entropy. These materials are expected to display fascinating electrochemical properties. Herein, we successfully synthesized a defect-rich (CoCrFeMnNi)3O4 HEO catalyst with a single-phase spinel structure through a hydrothermal route pursued by calcination and, for the first time use it for vanadium redox flow battery (VRFB). Compared with monometallic oxide, Co3O4, and bimetallic oxide, (Fe,Co)3O4, the HEO catalyst reveals the utmost catalytic performance and reversibility towards the VO2+/VO2+ redox couple. Owing to the unique single-phase spinel structure and abundant oxygen vacancies, the VRFB flow cell using the HEO-modified heat-treated graphite felt (HEO-HGF) electrode achieves an outstanding energy efficiency of 79.23 % and 70.58 % at 160 and 240 mA/cm2, respectively, and shows good stability even for 500 cycles. This study provides new insight into other redox flow battery applications.

Diamino-Substituted Quinones as Cathodes for Lithium-Ion Batteries.

This study introduces a sustainable approach to designing organic cathode materials (OCMs) for lithium-ion batteries as a potential replacement for traditional metal-based electrodes. Utilizing green synthetic methodologies, we synthesized and characterized five distinct quinone derivatives and investigated their electrochemical attributes within Li-ion battery architectures. Notably, the observed specific capacities were lower than the theoretical predictions, suggesting limitations in achieving efficient redox reactions in a coin-cell configuration. Among the quinone derivatives studied, one variant derived from natural vanillin showed superior cycle stability, maintaining 58% capacity retention over 95 charge-discharge cycles, and achieving a Coulombic efficiency of 90%. Importantly, we discovered that the commonly used Super-P conductive carbon did not yield any measurable battery performance; instead, these quinones necessitated the incorporation of graphene nanoplatelets as the conductive matrix. Through a facile one-step synthesis in ethanol or water, we have demonstrated a viable synthetic route for producing OCMs, albeit with moderate performances, which have attempted to address common concerns of high solubility and poor redox reactivity of previous OCMs, thereby offering a sustainable pathway for the development of organic-based energy storage devices.