High-performance Electrode Research Articles

Pushing Theoretical Potassium Storage Limits of MXenes through Introducing New Carbon Active Sites.

Surface-driven capacitive storage enhances rate performance and cyclability, thereby improving the efficacy of high-power electrode materials and fast-charging batteries. Conventional defect engineering, widely-employed capacitive storage optimization strategy, primarily focuses on the influence of defects themselves on capacitive behaviors. However, the role of local environment surrounding defects, which significantly affects surface properties, remains largely unexplored for lack of suitable material platform and has long been neglected. As proof-of-concept, typical Ti3C2Tx MXenes are chosen as model materials owing to metallic conductivity and tunable surface properties, satisfying the requirements for capacitive-type electrodes. Using density functional theory (DFT) calculations, the potential of MXenes with modulated local atomic environment is anticipated and introducing new carbon sites found near pores can activate electrochemically inert surface, attaining record theoretical potassium storage capacities of MXenes (291 mAh g-1). This supposition is realized through atomic tailoring via chemical scissor within sublayers, exposing new sp3-hybridized carbon active sites. The resulting MXenes demonstrate unprecedented rate performance and cycling stability. Notably, MXenes with higher carbon exposure exhibit a record-breaking capacity over 200 mAh g-1 and sustain a capacity retention higher than 80% after 20 months. These findings underscore the effectiveness of regulating defects' neighboring environment and illuminate future high-performance electrode design.

Synthesis of NiFeCo ternary layered hydroxides and their performances of electrochemical energy storage for solar cells

Ternary layered hydroxide are high-performance electrode materials for supercapacitors. In this study, nickel–iron-cobalt ternary layered hydroxides (NiFeCo-LDHs) with different nickel–iron molar ratios were grown on nickel foam using a one-step hydrothermal method. The effect of nickel–iron molar ratio on the electrochemical performance and morphology of NiFeCo-LDHs was investigated, and the electrode material at a nickel–iron molar ratio of 3:7 had better electrochemical performance up to 7.01F/cm2 (at 1 mA/cm2). The specific capacitance of the assembled hybrid supercapacitor reached 1575.00 mF/cm2 at 3 mA/cm2. In addition, the fabricated all-solid-state hybrid capacitor（742.86 mF/cm2 at 4 mA/cm2) was capable of lighting an LED after charged by a solar cell. The results indicated that the electrochemical performance of NiFeCo-LDHs was affected by the nickel–iron mole ratio and demonstrated the potential application of NiFeCo-LDHs in electrochemical energy storage.

Impact of Nitrogen-Enriched 1T/2H-MoS2/CdS as an Electrode Material for Hybrid Supercapacitor.

Transition metal chalcogenides (TMX) have attracted energy researchers due to their role as high-performance electrode materials for energy storage devices. A facile one-pot hydrothermal technique was adopted to synthesize a molybdenum disulfide/cadmium sulfide (MoS2/CdS) (MCS) composite. The as-prepared samples were subjected to characterization techniques such as XRD, FT-IR, SEM, TEM, and XPS to assess their structure, morphology, and oxidation states. The MoS2/CdS (MCS) composites were prepared in three different ratios of molybdenum and cadmium metals. Among them, the MCS 1:2 (Mo:Cd) ratio showed better electrochemical performance with a high specific capacitance of 1336 F g-1 (high specific capacity of 185.83 mAh g-1) at a specific current of 1 A g-1 for half-cell studies. Later, a hybrid supercapacitor (HSC) device was fabricated with N-doped graphene (NG) as an anode and MCS (1:2) as a cathode, delivering a high specific energy of 34 Wh kg-1 and a specific power of 7500 W kg-1. The high nitrogen content in the MoS2 structure in MCS composites alters the device's performance, where CdS supports the composite structure through its conductivity and encourages the easy accessibility of ions. The device withstands up to 10 000 cycles with a higher Coulombic efficiency of 97% and a capacitance retention of 90.25%. The high-performance NG//MCS (1:2) HSC may be a potential candidate alternative to the existing conventional material.

Synthesis and Characterization of Coconut-Derived Graphene Nano Sheet (GNS) and Its Properties in Nickel/GNS and Zinc/GNS Hybrid Electrodes

This study introduces a sustainable method of producing a graphene nano sheet (GNS) from coconut shells and investigates its application in GNS, Ni/GNS, and Zn/GNS electrodes for advanced energy storage devices. The GNS was synthesized in a scalable manner using a pyrolysis and impregnation technique, with its successful synthesis verified by X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDX), Raman spectroscopy, and electrical conductivity measurement characterizations. The study highlights the enhanced performance of Zn/GNS electrodes, which outperform both pure GNS and Ni/GNS variants. This superior performance is attributed to the smaller particle size of Zn (mean = 2.356 µm) compared to Ni (mean = 3.09 µm) and Zn’s more favourable electron configuration for electron transfer. These findings demonstrate the potential of bio-derived GNS composites as efficient, high-performance electrodes, paving the way for more sustainable and cost-effective energy storage solutions.

Bamboo-templated MOF-67-derived carbon: A high-performance electrode for supercapacitors

Carbon-based supercapacitors are highly regarded for their high specific power and long cycle life. However, they often face the challenge of low specific energy and difficulty in simultaneously improving both specific energy and specific power. In this study, a high-performance composite electrode was prepared using the cross-section of bamboo as raw material, followed by KOH activation, in-situ growth of ZIF-67, and carbonization. The bamboo-derived porous carbon showed significant improvement in performance indicators such as specific capacitance and energy density. Electrochemical characterization in a three-electrode system showed that at a current density of 1 mA cm−2, our composite electrode material achieved a peak specific capacitance of 24.7 F cm−2. When assembled into a symmetric supercapacitor, it can provide an energy density of 1.00 mWh cm−2 at a power density of 2.49 mW cm−2. Notably, at a substantial current density of 30 mA cm−2, the electrode maintained a capacitance retention of 96.2 % after 10,000 cycles. These results not only highlight the potential of bamboo-derived porous carbon but also point to a broad avenue for the preparation of energy storage devices by combining MOFs with bamboo.

High oxidation state on porous Ga-Ag9In4 catalyst enhance CO2 electroreduction to CO

The oxidation state of Ga, In and Ag active sites for the selective electrochemical conversion of CO2 to CO has been successfully modulated through the construction of a porous Ga-Ag9In4 liquid alloy catalyst. X-ray photoelectron spectroscopy measurements confirmed the formation of a higher amount of oxidized states on the high-performing Ga-Ag9In4 electrode surface during the CO2 reduction reaction process. Based on density functional theory calculations, the Ga-Ag9In4 catalyst with a high oxidized species exhibits an electronic-rich surface that promotes CO2 adsorption and activation. In a H-type electrolysis cell, the porous Ga-Ag9In4 catalyst exhibits a maximum Faradaic efficiency of 88 % for CO production, with current densities of 30.2 mA·cm−2. This strategy of porous liquid alloy engineering and oxidation state modulation in multicomponent systems has good application prospect and research value for enhancing electrocatalytic performance.

SrCoO3-based perovskites with enhanced electrochemical performance through structural tailoring induced by B-site substitution

The progression of supercapacitor technology hinges on the discovery of high-performance electrode materials to enhance energy storage. SrCoO3-δ perovskite holds considerable promise potential as an anion intercalation electrode material. To elucidate the structural and electrochemical performance modulation rules of SrCoO3-based perovskites, this study synthesized SrCo0.875M0.125O3-δ (M = Ti, Ta, Nb, Fe) perovskites with different B-site ion substitutions. The structural tailoring induced by B-site substitution were thoroughly investigated alongside their corresponding electrochemical performance. Notably, SrCo0.875Ti0.125O3-δ exhibited a simple cubic structure, while the other samples displayed a tetragonal structure. Additionally, SrCo0.875Fe0.125O3-δ displayed numerous oxygen vacancies and significant distortion in the [CoO6] octahedron, which is attributed to the lower valence state of Fe. At a current density of 1 A g−1, the specific capacities of SrCo0.875M0.125O3-δ (M = Nb, Ti, Fe, Ta) perovskites were 984.43, 853.33, 503.53, and 452.00C/g, respectively. SrCo0.875Nb0.125O3-δ demonstrated the highest specific capacity and capacity retention rate across various current density, owing to its relatively stable structure with appropriate oxygen vacancies and multivalent state changes of Nb. In contrast, SrCo0.875Fe0.125O3-δ, with excessive oxygen vacancies and severe structural distortions, exhibited restricted electrochemical performance, particularly at higher current densities. Integrating structural and performance analysis, this work proposes an optimization strategy for the electrochemical performance of SrCoO3-δ-based perovskite electrode materials, emphasizing the importance of tailoring multivalent B-site elements to achieve a stable perovskite structure with appropriate oxygen vacancies.

Selective electrosorption of heavy metal ions from wastewater with S-doped hierarchical porous carbon derived from waste Camellia oleifera shell

Capacitive deionization (CDI) has garnered significant attention in desalination and the removal of heavy metal ions. The quest for cost-effective and high-performance electrode materials is crucial to advance CDI applications. Herein, we report a sulfur-doped hierarchical porous carbon (SPC) derived from waste camellia oleifera shells via a sustainable hydrothermal carbonization process followed by KOH/ammonium salt activation. The optimized SPC-0.2 exhibits exceptional characteristics, featuring a high specific surface area of 1875 m2 g−1 and substantial sulfur doping at 8.65 %, leading to enhanced specific capacitance (161.3 F g−1) in a 1 M NaCl solution. Under optimal operating conditions (1.2 V, 10 mL min−1, 500 mg L−1 NaCl), the SPC-0.2 electrode achieves a notable desalination capacity of 26.64 mg g−1. In particular, the electrode can selectively remove >99 % of Cr3+ and Cu2+ ions (each 10 mg L−1) in a 100 mg L−1 NaCl solution. This high selectivity is attributed to the formation of sulfides via low adsorption energies between the doped sulfur atoms and the targeted heavy metal ions. Furthermore, the SPC-0.2 electrode demonstrates robust reusability and high efficiency in the actual water body. Collectively, our findings underscore the significant potential of the synthesized SPC as an electrode material for CDI, particularly in the selective capacitive removal of heavy metal ions from wastewater. This work not only contributes to the circular economy by using waste biomass, but also offers a viable solution for environmental remediation.

Strong and high-conductivity hydrogels with all-polymer nanofibrous networks for applications as high-capacitance flexible electrodes

Flexible devices, such as soft bioelectronics and stretchable supercapacitors, have their practical performance limited by electrodes which are desired to have high conductivity and capacitance, outstanding mechanical flexibility and strength, great electrochemical stability, and good biocompatibility. Here, we report a simple and efficient method to synthesize a nanostructured conductive hydrogel to meet such criteria. Specifically, templated by a hyperconnective nanofibrous network from aramid hydrogels, the conducting polymer, polypyrrole, assembles conformally onto nanofibers through in-situ polymerization, generating continuous nanostructured conductive pathways. The resulting conductive hydrogel shows superior conductivity (72 S cm−1) and fracture strength (27.2 MPa). Supercapacitor electrodes utilizing this hydrogel exhibit high specific capacitance (240 F g−1) and cyclic stability. Furthermore, bioelectrodes of patterned hydrogels provide favorable bioelectronic interfaces, allowing high-quality electrophysiological recording and stimulation in physiological environments. These high-performance electrodes are readily scalable to applications of energy and power systems, healthcare and medical technologies, smart textiles, and so forth.

Hydrogen adsorption on fcc metal surfaces towards the rational design of electrode materials

The successful large-scale implementation of hydrogen as an energy vector requires high performance electrodes and catalysts made of abundant materials. Rational materials design strategies are the most efficient means of reaching this goal. Here we present a study on the adsorption of H-atoms onto fcc transition metal surfaces and propose descriptors for the rational design of electrodes and catalysts by means of correlations between fundamental properties of the materials and among other properties, their experimentally measured performance as hydrogen evolution electrodes (HEE). A large set of quantum mechanical modelling data at the DFT level was produced, covering the adsorption of H-atoms onto the most stable surfaces (100), (110) and (111) of: Ag, Au, Co, Cu, Ir, Ni, Pd, Pt and Rh. For each material and surface, a coverage dependent set of minimum energy structures was produced and chemical potentials for adsorption of H-atoms were obtained. Averaging procedures are here proposed to approach modelling to the experiments. Several correlations between the computed data and experimentally measured quantities are done to validate our methodology: surface plane dependent adsorption energies, chemical potentials and experimentally determined surface energies and work functions. We search for descriptors of catalytic activity by testing correlations between the DFT data obtained from our averaging procedures and experimental data on HEE performance. Our methodology allows us to obtain linear correlations between the adsorption energy of H-atoms and the exchange current density (i0) in a HEE, avoiding the volcano-like plots. We show that the chemical potential has limitations as a descriptor of i0 because it reaches an early plateau in terms of i0. Simple quantities obtained from database data such as the first stage electronegativity (χ) as devised by Mulliken has a strong linear correlation i0. With a quantity we denominate modified second-stage electronegativity (χ2m) we can reproduce the typical volcano plot in a correlation with i0. A theoretical and conceptual framework is presented. It shows that both χ and χ2m, that depend on the first ionization potential, second ionization potential and electron affinity of the elements can be used as descriptors in rational design of electrodes or of catalysts for hydrogen systems.

In-situ N, P co-doped porous carbon derived from biomass waste for supercapacitors

The development of heteroatom-doped porous carbon derived from biomass waste with high-performance electrodes for supercapacitors has been drawn extensive research. Herein, N, P co-doped porous carbon (NPC) was successfully synthesized using Chinese fir sawdust as a carbon source, NaOH as an activator, urea as a nitrogen source, and melamine phosphate as the phosphorus and nitrogen source by pretreatment with low-temperature NaOH/urea system. The low-temperature pretreatment and melamine phosphate greatly promoted the porous structure and uniform distributions of heteroatom about the NPC. The optimized NPC exhibits high specific surface area (1849 m2/g), hierarchical porous structure with high mesoporosity (87.3 %), appropriate heteroatom content (3.32 at% N, 0.36 at% P), and excellent wettability. This unique facilitates improved electrolyte diffusion efficiency and ion transfer rate. In the three-electrode system, the specific capacitance of the NPC electrode is as high as 260 F/g at 0.5 A/g and remains at 235 F/g at 10 A/g, and the charge transfer resistance is very low (0.08 Ω). In addition, the assembled symmetric supercapacitors deliver an energy density of 15.9 Wh/kg at a power density of 246 W/kg, a long cycling life with 90 % capacitance retention after 5000 cycles. The environment-friendly NPC has a broad development prospect for carbon-based high-performance electrodes for supercapacitors.

Graphene oxide from coconut shells for high-performance supercapacitor application

Globally, the demand for materials with high ultrafast charge rates yet slow discharge continues to rise which has resulted in extensive research into supercapacitors. Although the current supercapacitors can meet such demands, the high processing cost coupled with the use of toxic chemicals remains a major concern. In this study, porous graphene oxide (GO) with a unique morphology was synthesized by an improved Tour’s method for supercapacitor application using coconut shells as a precursor. The structure of the synthesized material consists of partially graphitized walls of porous GO. The surface morphology, the defects created in the GO, and the specific surface area of the as-synthesized materials were studied. When evaluated as an electrode material for supercapacitors, a specific capacitance of 173 F/g at 0.5 A/g in 0.5 M Na2SO4 and 139 F/g at 0.5 A/g in 2 M KOH was recorded. Moreover, a high capacitance retention of 99.3% was recorded after 1000 cycles, confirming the good cyclic stability of the synthesized electrode material. The good electrochemical performance can be attributed to the electrode material’s intrinsic structural and compositional superiorities. These findings indicate the potential of using coconut shells as a precursor for the synthesis of high-performance graphene-based supercapacitor electrodes with improved cost-effectiveness and reduced environmental impact.

PTFE as a Multifunctional Binder for High-Current-Density Oxygen Evolution.

Binder plays a crucial role in constructing high-performance electrodes for water electrolysis. While most research has been focused on advancing electrocatalysts, the application of binders in electrode design has yet to be fully explored. Herein, the in situ incorporation of polytetrafluoroethylene (PTFE) as a multifunctional binder, which increases electrochemical active sites, enhances mass transfer, and strengthens the mechanical and chemical robustness of oxygen evolution reaction (OER) electrodes, is reported. The NiFe-LDH@PTFE/NF electrode prepared by co-deposition of PTFE with NiFe-layered double hydroxide onto nickel foam demonstrates exceptional long-term stability with a minimal potential decay rate of 0.034mV h-1 at 500mA cm-2 for 1000 h. The alkaline water electrolyzer utilizing NiFe-LDH@PTFE/NF requires only 1.584V at 500mA cm-2 and sustains high energy efficiency over 1000 h under industrial operating conditions. This work opens a new path for stabilizing active sites to obtain durable electrodes for OER as well as other electrocatalytic systems.

Novel metal-organic anode material by in-situ chelating Ni2+ with tannic acid on carbon nanotube for high-performance Li storage

Lithium-ion batteries (LIBs) with natural organic anode are attracting intensive interest for application owing to their structural diversity, cost-effectiveness, eco-friendliness, and high specific capacity. However, directly usage of natural organic materials as anode materials usually encounters poor electrochemical properties such as low reversible capacity and short cycling life. Thus, developing high-performance organic electrode materials for LIBs remains a great challenge. Herein, we present a rational design and fabrication of TA-Ni@CNTs by in-situ coating TA-Ni polymers onto the surface of carbon nanotubes (CNTs) as a superior anode material for LIBs. Specifically, the highly conductive CNTs can effectively relieve the aggregation of TA-Ni and improve the electronic conductivity. Meanwhile, the strong chelation among nickel irons and catechol groups enhances the structure stability and inhibits the dissolving property. Consequently, as an anode material for LIBs, the resulting TA-Ni@CNTs achieves a high reversible capacity of 1418.8 mAh·g−1 at 0.1 A·g−1 after 216 cycles and an outstanding cycling stability with 951.1 mAh·g−1 at 0.5 A·g−1 after 323 cycles. The presented design strategy holds great promise for developing more-efficient electrode materials for LIBs.

20 Seconds to fabricate high-performance NiFe-based anode for seawater electrolysis via bidirectional pulse current method

Direct electrolysis of seawater to produce green hydrogen has attracted great attention. While the development of efficient and rapid manufacturing processes for high-performance electrodes, particularly for the oxygen evolution reaction (OER), remains trail. Here, we introduce an innovative approach to fabricate high-performance NiFe-based OER electrodes using an ultrafast and eco-friendly bidirectional pulse current (BPC) method, which remarkably shortens the production time to only 20 s. Our BPC method alternates oxidation and reduction currents within a single period, promoting the in-situ formation of porous NiFe(oxy)hydroxide nanosheets through dissolution/deposition processes. Moreover, this methodology creatively utilizes the “Cl− induced effect”, typically a hindrance in other electrochemical systems involving seawater or brine, to enhance the synthesis of electrodes from NaCl-based electrolyte devoid of additional Ni/Fe cations. The prepared NiFe-based electrode (NFF O-R 20 s) demonstrates remarkable OER catalytic activity, with optimal overpotentials (ηj) of 272, 308 and 367 mV at current densities (j) of 10, 100 and 1000 mA cm−2, respectively. Impressively, it maintains a low cell voltage of 1.59 V after enduring 1000 h of operation under the industrially current density of 300 mA cm−2, with a direct current energy consumption of 3.8 kWh Nm−3 H2 for overall alkaline seawater electrolysis. Our BPC preparation approach provides a promising path to construction high-catalytic activity, good-stability electrode, and low-energy consumption direct seawater electrolyzer.

Optimizing nickel-aluminium layered double hydroxides for supercapacitors: The role of 3D structural assembly

Nickel-aluminium layered double hydroxides (NiAl-LDHs) have emerged as promising electrode materials for supercapacitors (SCs) due to their inherently high specific surface area and theoretical specific capacitance, which are primarily attributed to the rapid pseudocapacitive response at the surface. However, NiAl-LDHs typically form agglomerated nanosheets, leading to a significant reduction in specific surface area, which is crucial for enhancing the number of active sites and improving the capacitive properties of the materials. To overcome this limitation, 2D nanostructures were assembled into 3D architectures by synthesizing NiAl-LDHs with distinct morphologies in a one-step hydrothermal process using an alkaline agent (NH4F). This approach resulted in the formation of 3D NiAl-LDH/HN4F structures, which exhibit a larger contact area and a greater number of redox-active sites. Consequently, the 3D NiAl-LDH/HN4F electrodes demonstrated a significantly higher specific surface area, leading to remarkable improvements in specific capacitance (1219 ± 30F g−1) and energy density (61 ± 1 Wh kg−1) compared to their 2D counterparts. This structural enhancement increases both the surface area and active site density while providing a new framework for designing high-performance LDH-based electrodes.

Zn-substituted Co3O4 crystal anchored on porous carbon nanofibers for high performance supercapacitors

Metal-organic frameworks (MOFs) are a promising class of electrode materials for supercapacitors. In this work, MOF-derived transition metal oxide/carbon nanofiber composites (ZnCoO/C) are synthesized through a freeze-drying method followed by a carbonization process. The crystal structure of the ZnCoO/C product is regulated by changing the ratio of Co to Zn, which in turn influences its electrode properties. The electrochemical tests reveal that the ZnCoO/C-2 electrode demonstrates an impressive specific capacitance of 356.3 F g-1 at 1 A g-1 and maintains a capacitance retention exceeding 77 % after 10,000 cycles, which exhibits a good cycling stability. It is found that appropriate Zn substitution can diminish the crystallinity of the material, augment the active sites, and enhance the specific capacitance of the electrode material. Considering the heteroatom substitution tends to introduce vacancy defects in the crystals, this work theoretically explores the effect of oxygen vacancies on the electrode materials. As the oxygen vacancy concentration increases, the band gap and the adsorption energy of the models decrease; conversely, the formation energy of the models shows an increasing tendency. This indicates that an increase in oxygen vacancies can enhance the electrical conductivity of electrode materials and facilitate their kinetic process but destroy the stability of crystal. This research explores the interplay between the microstructure and the electrochemical performance of electrode materials, providing a foundational reference for the design of structurally optimized high-performance electrodes and further elucidating the energy storage mechanisms in supercapacitors.

A Dual-Carbon Potassium-Ion Capacitor Enabled by Hollow Carbon Fibrous Electrodes with Reduced Graphitization.

The large size of K+ ions (1.38 Å) sets a challenge in achieving high kinetics and long lifespan of potassium storage devices. Here, a fibrous ZrO2 membrane is utilized as a reactive template to construct a dual-carbon K-ion capacitor. Unlike graphite, ZrO2-catalyzed graphitic carbon presents a relatively disordered layer arrangement with an expanded interlayer spacing of 0.378nm to accommodate K+ insertion/extraction. Pyridine-derived nitrogen sites can locally store K-ions without disrupting the formation of stage-1 graphite intercalation compounds (GICs). Consequently, N-doped hollow graphitic carbon fiber achieves a K+-storage capacity (primarily below 1V), which is 1.5 time that of commercial graphite. Potassium-ion hybrid capacitors are assembled using the hollow carbon fiber electrodes and the ZrO2 nanofiber membrane as the separator. The capacitor exhibits a high power of 40 000 W kg-1, full charge in 8.5 s, 93% capacity retention after 5000 cycles at 2 A g-1, and a low self-discharge rate of 8.6mV h-1. The scalability and high performance of the lattice-expanded tubular carbon electrodes underscores may advance the practical potassium-ion capacitors.

High-Performance Supercapacitor Electrodes for Enhanced Energy Storage in Microelectronic Devices Using Facile Green Synthesis of CdO Nanoparticles

High-Performance Supercapacitor Electrodes for Enhanced Energy Storage in Microelectronic Devices Using Facile Green Synthesis of CdO Nanoparticles

3D Co-doped carbon nanosheets as high-performance electrodes for Li-S batteries

3D petal-shaped Cobalt-doped carbon nanosheets (PCoCNS) were synthesized as excellent sulfur hosts for lithium-sulfur (Li-S) batteries. Co doping enhanced the affinity of the carbon surface for lithium polysulfides (LiPSs), inhibiting the shuttle effect. The electrocatalytic effect of the PCoCNS electrode exhibited enhanced polysulfide conversion kinetics, thereby promoting Li2S formation. Owing to the above advantages, the PCoCNS cathode exhibited satisfactory reversibility of 841 mAh/g with a high capacity retention of 91 %. Additionally, it displayed high coulombic efficiency (CE) values exceeding 97 % over 100 cycles at a current rate of 0.5C. Furthermore, the electrode demonstrated low polarization and exhibited an excellent rate performance, delivering a capacity of 575 mAh/g at the high rate of 3C. This study synthesized a promising sulfur cathode for enhancing the electrochemical performance of Li-S batteries.