Multilayer Electrode Research Articles

Effect of thermal shock on ZnO/Ag/ZnO nano-multilayers: Photoelectric property degradation

We investigated the degeneration at photoelectric properties of typical multilayer transparent conductive electrodes (TCEs) of ZnO/Ag/ZnO under thermal shock by experiments and simulation. The experimental data indicated a reduction in the visible region transparency and an increase in sheet resistance for ZnO/Ag/ZnO after undergoing thermal cyclic shock. This resulted in a significant decrease in the Haacke figure of merit (FOM) from 30.7 × 10-3 Ω−1 to 7.8 × 10-3 Ω−1. We identified oxygen diffusion into Ag at the ZnO/Ag interface using molecular dynamics (MD) simulations. Concurrently, density functional theory (DFT) simulations showed that interstitial oxygen creates impurity charge centers within Ag, indirectly causing the deterioration of the photoelectric properties of ZnO/Ag/ZnO. This finding highlights the challenge of maintaining optoelectronic stability in TCO/metal/TCO (OMO) thin films for practical applications and provides both experimental and theoretical support for designing highly reliable optoelectronic devices.

Aminated silver nanowires as current collectors and binders for the preparation of multilayer graphite loading high-performance silk fiber electrodes

The rapid development of wearable electronic devices has put forward high requirements for their energy storage devices. Currently, fiber supercapacitors have attracted widespread attention owing to their miniature sizes and high flexibility, but an improvement in their electrochemical performance is often limited by the loading of conductive energy storage materials. Herein, a multilayer graphene loading strategy based on amino silver nanowires (NH2-AgNWs) was developed to prepare silk electrodes, wherein NH2-AgNWs were used as current collectors and binders to increase the conductivity of silk electrodes and achieve multilayer loading graphene on silk. The prepared silk electrode exhibited a high specific capacitance of 37.14 mF/cm because of the multilayer loading of the conductive energy storage material. The generality of this method is further demonstrated with a cotton thread substrate electrode, which exhibited a specific capacitance of 69.45 mF/cm. Additionally, a parallel fiber-shaped supercapacitor (PFSS) was assembled, at the maximum power density of 74.48 mW/m2, the energy density reaches 1468.87 mWh/m2. The PFSS exhibited a capacitance retention rate of 93.01 % when the bending degree was 90°. This study proposes a multilayer graphene loading strategy based on NH2-AgNWs for the preparation of fiber electrodes and a flexible fiber supercapacitor was assembled.

High-Performance Organic Field-Effect Transistors Based on Two-Dimensional Vat Orange 3 Crystals

The exploration and research of low-cost, environmentally friendly, and sustainable organic semiconductor materials are of immense significance in various fields, including electronics, optoelectronics, and energy conversion. Unfortunately, these semiconductors have almost poor charge transport properties, which range from ∼ 10−4 cm2⋅V−1⋅s−1 to ∼ 10−2 cm2⋅V−1⋅s−1. Vat orange 3, as one of these organic semiconductors, has great potential due to its highly conjugated structure. We obtain high-quality multilayered Vat orange 3 crystals with two-dimensional (2D) growth on h-BN surfaces with thickness of 10–100 nm using physical vapor transport. Raman’s results confirm the stability of the chemical structure of Vat orange 3 during growth. Furthermore, by leveraging the structural advantages of 2D materials, an organic field-effect transistor with a 2D vdW vertical heterostructure is further realized with h-BN encapsulation and multilayered graphene contact electrodes, resulting in an excellent transistor performance with On/Off ratio of 104 and high field-effect mobility of 0.14 cm2⋅V−1⋅s−1. Our results show the great potential of Vat orange 3 with 2D structures in future nano-electronic applications. Furthermore, we showcase an approach that integrates organic semiconductors with 2D materials, aiming to offer new insights into the study of organic semiconductors.

Surface modification of multilayer graphene electrodes by local printing of platinum nanoparticles using spark ablation for neural interfacing.

In this paper, we present the surface modification of multilayer graphene electrodes with platinum (Pt) nanoparticles (NPs) using spark ablation. This method yields an individually selective local printing of NPs on an electrode surface at room temperature in a dry process. NP printing is performed as a post-process step to enhance the electrochemical characteristics of graphene electrodes. The NP-printed electrode shows significant improvements in impedance, charge storage capacity (CSC), and charge injection capacity (CIC), versus the equivalent electrodes without NPs. Specifically, electrodes with 40% NP surface density demonstrate 4.5 times lower impedance, 15 times higher CSC, and 4 times better CIC. Electrochemical stability, assessed via continuous cyclic voltammetry (CV) and voltage transient (VT) tests, indicated minimal deviations from the initial performance, while mechanical stability, assessed via ultrasonic vibration, is also improved after the NP printing. Importantly, NP surface densities up to 40% maintain the electrode optical transparency required for compatibility with optical imaging and optogenetics. These results demonstrate selective NP deposition and local modification of electrochemical properties in graphene electrodes for the first time, enabling the cohabitation of graphene electrodes with different electrochemical and optical characteristics on the same substrate for neural interfacing.

Scalable fabrication of multi-layered Cu-based electrodes via solvent-free method for the selective electrochemical conversion of CO2 to C2+ products

A novel solvent-free procedure for multi-layered Cu-based gas diffusion electrodes was developed for CO2 electroreduction. Physical properties were evaluated and optimized to enhance C2+ production.

Multilayer Ti3C2Tx MXene electrode decorated with polypyridine for efficient symmetric supercapacitors

A multilayer Ti3C2Tx MXene electrode decorated with polypyridine was employed to fabricate an efficient symmetric supercapacitor.

Efficient transparent blue-emitted perovskite light-emitting diodes based on multilayer transparent top electrodes

A blue emitted transparent perovskite light-emitting diode was prepared by using quasi two-dimensional perovskite materials and multilayer transparent top electrodes.

Correction: Multilayer Ti3C2Tx MXene electrode decorated with polypyridine for efficient symmetric supercapacitors

Correction for ‘Multilayer Ti3C2Tx MXene electrode decorated with polypyridine for efficient symmetric supercapacitors’ by Peng Lin et al., Sustainable Energy Fuels, 2024, https://doi.org/10.1039/D4SE00892H.

3D spatiotemporally scalable in vivo neural probes based on fluorinated elastomers.

Electronic devices for recording neural activity in the nervous system need to be scalable across large spatial and temporal scales while also providing millisecond and single-cell spatiotemporal resolution. However, existing high-resolution neural recording devices cannot achieve simultaneous scalability on both spatial and temporal levels due to a trade-off between sensor density and mechanical flexibility. Here we introduce a three-dimensional (3D) stacking implantable electronic platform, based on perfluorinated dielectric elastomers and tissue-level soft multilayer electrodes, that enables spatiotemporally scalable single-cell neural electrophysiology in the nervous system. Our elastomers exhibit stable dielectric performance for over a year in physiological solutions and are 10,000 times softer than conventional plastic dielectrics. By leveraging these unique characteristics we develop the packaging of lithographed nanometre-thick electrode arrays in a 3D configuration with a cross-sectional density of 7.6 electrodes per 100 µm2. The resulting 3D integrated multilayer soft electrode array retains tissue-level flexibility, reducing chronic immune responses in mouse neural tissues, and demonstrates the ability to reliably track electrical activity in the mouse brain or spinal cord over months without disrupting animal behaviour.

Impact of Coating Layer Parameters on Electrode Tortuosity

The performance of Li-ion batteries is highly influenced by the microstructure of the assembled electrodes. Typically, porosity is chosen as a standard characteristic parameter, describing the morphology of the material components in the coated layer. However, transport phenomena and concentration polarization resistance also depend on the tortuosity of the electrode coating [1]. Therefore, it is crucial to determine the relationship between coating parameters (such as coating speed and drying parameters) and their effect on the tortuosity. Especially for thick electrodes an elongation of ionic transport pathways can arise due to the inhomogeneous distribution of the materials. Dead ends, branches, and surface impurities can lead to an increase in effective tortuosity [2], which can be minimized by careful selection of the coating parameters. A high binder concentration at the layer surface, caused by binder particles migrating during the drying process, can lead to a blockage of Li-channels [3, 4]. This can not only diminish the mechanical stability of the electrode but also harm the cycling performance, due to limitations in mass and charge transport [5].Electrochemical impedance spectroscopy can be used as a characterization technique to investigate the tortuosity of the electrode. Symmetric cells in combination with a non-intercalating electrolyte create a blocking condition of the cells. Extrapolating the spectrum's high and low-frequency regions, offsets in the real part of the impedance can be determined in the Nyquist plot (Figure 1a). The ionic resistance can be determined, and consequently, tortuosity can be calculated. A modified transmission line model can be used for in-depth analysis.In the case of homogenously distributed material, tortuosity should be an intrinsic value. In this work, a threshold value of the electrode thickness was determined, above which the tortuosity increases drastically (Figure 1b). This leads to the conclusion that when increasing the thickness, changes in the layer composition can arise.Additionally, the correlation between tortuosity and porosity was investigated and associated Bruggeman coefficients were compared.In a previous study, the multilayer coating technique has proven itself to be beneficial for increasing the electrochemical performance of high-loading electrodes containing cells [6]. Subsequent coating of multiple layers on top of each other enables the possibility to fine-tune material distributions along the layer thickness. Particularly, electrodes with an imposed binder gradient, of low concentration at the electrode separator interface, show a noteworthy decrease in tortuosity [7].This study was done on cathode samples with NMC811 as active material. Processing was done with both water and NMP, to show the impact of the solvent on the electrode tortuosities. Acknowledgments This work was financially supported by the Austrian Federal Ministry for Climate Action, Environment, Energy, Mobility, Innovation and Technology (bmk).[1] B. Tjaden, D. J. L. Brett, and P. R. Shearing, “Tortuosity in electrochemical devices: a review of calculation approaches,” International Materials Reviews, vol. 63, no. 2, pp. 47–67, Feb. 2018, doi: 10.1080/09506608.2016.1249995.[2] J. Landesfeind, J. Hattendorff, A. Ehrl, W. A. Wall, and H. A. Gasteiger, “Tortuosity Determination of Battery Electrodes and Separators by Impedance Spectroscopy,” J Electrochem Soc, vol. 163, no. 7, pp. A1373–A1387, 2016, doi: 10.1149/2.1141607jes.[3] F. Font, B. Protas, G. Richardson, and J. M. Foster, “Binder migration during drying of lithium-ion battery electrodes: Modelling and comparison to experiment,” J Power Sources, vol. 393, no. December 2017, pp. 177–185, Jul. 2018, doi: 10.1016/j.jpowsour.2018.04.097.[4] S. Jaiser, M. Müller, M. Baunach, W. Bauer, P. Scharfer, and W. Schabel, “Investigation of film solidification and binder migration during drying of Li-Ion battery anodes,” J Power Sources, vol. 318, pp. 210–219, 2016, doi: 10.1016/j.jpowsour.2016.04.018.[5] M. Baunach, S. Jaiser, S. Schmelzle, H. Nirschl, P. Scharfer, and W. Schabel, “Delamination behavior of lithium-ion battery anodes: Influence of drying temperature during electrode processing,” Drying Technology, vol. 34, no. 4, pp. 462–473, 2016, doi: 10.1080/07373937.2015.1060497.[6] L. Neidhart, K. Fröhlich, N. Eshraghi, D. Cupid, F. Winter, and M. Jahn, “Aqueous Manufacturing of Defect-Free Thick Multi-Layer NMC811 Electrodes,” Nanomaterials, vol. 12, no. 3, pp. 1–15, 2022, doi: 10.3390/nano12030317.[7] L. Neidhart, K. Fröhlich, F. Winter, and M. Jahn, “Implementing Binder Gradients in Thick Water-Based NMC811 Cathodes via Multi-Layer Coating,” Batteries, vol. 9, no. 3, p. 171, Mar. 2023, doi: 10.3390/batteries9030171. Figure 1

Potential and Limitations of Research Battery Cell Types for Electrochemical Data Acquisition

Developing new electrode materials or electrolytes for lithium-ion batteries requires reliable electrochemical testing thereof. In academic research, coin-type cells and small pouch-type cells are commonly being assembled for this purpose. In our study [1], using commercial highly homogeneous and robust LiNi0.33Mn0.33Co0.33O2 (NMC111) cathodes, graphite anodes and 1M LiPF6 in EC/DMC with 3% VC as the electrolyte, four experienced researchers from the Institute for Applied Materials at Karlsruhe Institute of Technology assembled a variety of coin cells within a round robin test. For different cell building parameters, the battery lifetimes systematically varied from a few hundred to well over 2000 cycles before a capacity retention of 80 % was reached. As a benchmark, the same electrodes and electrolyte were incorporated as single- and multi-layer electrode stacks into pouch-type cells and reach almost 4000 cycles with a rate of 1 C.Missplacing of electrodes and varying amount of electrolyte within a coin-cell were already addressed as performance influencing factors in the literature. In this study, one clear outcome with high impact on previously collected electrochemical data on coin cells, is that the steel grade of cell parts, as well as the in-housed total height of the electrode stack have dramatic influence on cell lifetime and the quality of the acquired electrochemical data. We present our best practice for coin cell manufacturing resulting from the round robin test. Further, it is shown that inappropriate testing conditions like poor cell contacting and cycler settings have additional impact on data collection. In this regard, we emphasize essential parameters for obtaining high quality data.Additionally, using the same electrodes, we show direct rate performance differences of calendered vs. uncalendered electrodes, as well as half vs. full-cell test results by means of rate capability and long-term cycling stability. While compression of anodes is less crucial for rate capability, substantial differences are measured in case of the cathodes, highlighting the importance of sufficient cathode densification. Moreover, for long-term capacity retention studies, it is demonstrated that electrode densification of both, cathode and anode is crucial for high long-term capacity retention.Our results are bridging the gap between lab research and industry-type battery cells. It is shown how key performance parameters can be projected from corresponding lab scale battery cell data, if certain important criteria are met vs. where the projections have their limits.[1] A. Smith, P. Stüble, L. Leuthner, A. Hofmann, F. Jeschull and L. Mereacre, Batteries & Supercaps 2023, e202300080. Figure 1

Corrosion Resistant Multilayered Electrode Comprising Ni3N Nanoarray Overcoated with NiFe‐Phytate Complex for Boosted Oxygen Evolution in Seawater Electrolysis

AbstractEngineering high‐performance oxygen evolution reaction (OER) anode material with high activity, selectivity, and strong robustness against chloride corrosion is critical to advance seawater electrolysis for large‐scale production of H2, yet a daunting challenge. Herein it is reported for the first time, the engineer of a multilayered electrode consisting of Ni foam‐supported Ni3N porous nanosheet array decorated with NiFe‐phytate coordination complex overlayer (NF/Ni3N@NiFe‐PA) via a facile interfacial coordination assembly, for remarkably boosted and sustained OER in alkaline seawater electrolysis. Benefitting from regulated electronic state by synergism between Ni and Fe species, boosted proton‐coupled electron transfer via accelerating proton movement with the aid of incorporated phytic acid as proton transfer relay, and promoted mass transfer rendered by unique superhydrophilic and superaerophobic property, the resulting NF/Ni3N@NiFe‐PA demonstrates prominent OER activity in seawater. Impressively, integrating anticorrosive Ni3N with NiFe‐PA complex and in situ generated NiFeOOH can collaboratively contribute to chloride repelling, leading to exceptional corrosion resistance of the electrode. This work affords a novel paradigm to engineer active and corrosion‐resistive anode for selective OER in saline water electrolysis via simultaneous geometric and electronic structural manipulation.

Stable and accurate representation of species diffusion in multilayer composite electrodes using physics-informed neural networks

Stable and accurate reconstruction of species diffusion in Li-ion cell electrodes is a crucial problem, especially in modeling emerging composite electrode materials. Lithium-ion batteries are typically modeled using electrode theory coupled with various transport mechanisms that the solid-phase diffusion equation represents the main computational burden. In this paper, a computationally efficient representation for species transport in multilayer electrode is proposed based on the physics-informed neural networks (PINNs). A multi-objective loss function is constructed to obtain an accurate representation of field variables. It consists of the residual of solid-phase diffusion equation, associated initial/boundary conditions together with interface conditions. To deal with the problem of distinct material properties, the whole computational domain is divided into several subdomains where different neural networks for PINN are adopted. By using continuity conditions at interfaces, a whole network is established by combining subnetworks. By this way, the field variables can be obtained accurately by training and learning the neural networks. Li-ion concentrations in electrodes with single-layer and multilayer plate under the galvanostatic, potentiostatic, time-dependent flux, as well as time-dependent concentration charging are analyzed, and the results are validated against solutions obtained from finite element and analytical analysis. In terms of practical application, the galvanostatic voltage profiles of bi-layer (graphite-Si/SiOx) and tri-layer (graphite-Si/SiOx-graphite) electrodes are obtained using the Butler–Volmer kinetic equation and the performance is validated through good agreement with past experimental data. This study demonstrates for the first time the usefulness of the PINN to an electrochemical energy problem for designing multilayer electrode materials.

Electrochemical sensor based on PVP coated cobalt ferrite/graphite/PANI nanocomposite for the detection of hydrazine

In this study, we developed a multi-layered electrode as an efficient nanocomposite electrochemical sensor for detecting carcinogenic hydrazine in water. Nano-cobalt ferrite (CoFe2O4) was prepared using poly (vinylpyrrolidone) (PVP), mixed with an optimum quantity of graphite and pasted on a stainless-steel current collector. The nanocomposite was further hybridised by electrodepositing with polyaniline (PANI). The obtained composite was characterized using XRD, FTIR, SEM, and electrochemical techniques. XRD analysis shows the successful formation of composite from individual precursors. According to SEM, wrinkled and layered morphology for graphite and aggregate clusters for cobalt with spike or tubular structure for polyaniline were observed. When subjected to amperometry current, the prepared electrode showed different peaks for different concentrations of hydrazine, such as 1 μM to 100 μM. Cyclic voltammetry studies showed an increase in oxidation and reduction peaks. These studies will lead to a new platform for their potential applications in detecting toxic materials in real samples such as water, plastic bottle, water etc.,

Multi-layering of carbon conductivity enhancers for boosting rapid recharging performance of high mass loading lithium ion battery electrodes

The ability of lithium ion batteries (LIBs) to provide rapid charging characteristics while retaining a substantial energy storage capacity is of paramount significance for their applicability in portable smart electronic devices. In this research, an effective approach to enhance re-charging rates of LIB cells was developed through incorporating carbon nanotube (CNT) conductivity boosters strategically into Li4Ti5O12 (LTO) electrodes. A layer-by-layer spray coating was exploited to manufacture multi-layer architectures that comprise sequential, discrete electrode layers of CNT-rich LTO and CNT-free LTO, aiming at promoting charge transfer kinetics of high mass loading electrodes. Initially, the optimal proportion of a CNT-rich layer and its best location within multi-layer electrode structures were investigated in half-cell configurations. The best performing multi-layer was then paired with a spray-coated LiFePO4 (LFP) positive electrode in full-cell LIBs, offering attractive power performance of ∼ 1500 W/kg that outperformed conventional LTO || LFP combinations.

Construction of ultrahigh capacity density carbon nanotube based MIM capacitor

Energy storage technology is a key for a clean and sustainable energy supply. but their energy density is restricted by surface charge storage. One effective way to enhance the energy density is electrodes nanosizing in constructing MIM capacitor. However, the overall performance of the capacitors is still limited by electrode specific surface area and bonding strength of their electrode nano-templates to the substrate. In this work, the spatial multilayer VCNTs electrode nano-templates were obtained by laser etching assistance, and MIM capacitors were constructed layer-by-layer with SnO2/Al2O3/SnO2 structures as the dielectric capacitor frameworks via ALD. Laser etching is demonstrated on Al substrate, allowing the spatial multilayer growth of VCNTs with ultrahigh electrode area. Laser etching also introduces an Al2O3 buffer layer, which induces VCNTs in-situ growth during CVD and ensures bonding strength to Al substrate. Moreover, the VCNTs facilitates more coverage by dielectric during ALD, thus reducing the micro-short circuits risk for capacitors. Impressively, the fabricated MIM capacitors have high planar capacity density (0.47∼1.92 mF/cm2) with a low leakage characteristic (5.7 × 10−7 A/cm2) at 1V, which could reach a high energy density (26 µWh/cm2) and power density (104 W/cm2), as well as excellent performance stability under atmospheric and water environments. This work shows a promising strategy for developing new energy storage devices with both high energy and power density, and it has important guiding significance for the electrode nano-templates materials design and preparation of energy storage devices.

Improving the Uniformity of Top Emitting Organic Light Emitting Diodes Using a Hybrid Electrode Structure

AbstractSome applications of organic light‐emitting diodes (OLEDs) require large area, high light output, and high uniformity. It is difficult to achieve these attributes simultaneously because of voltage drops in the contacts, which cannot easily satisfy high optical transparency and electrical conductivity simultaneously. In large area OLEDs, thin electrodes with high sheet resistance induce voltage drops across the devices, leading to non‐uniform distribution of light. However, thick electrodes with low sheet resistance decrease the light output due to low transmittance. To overcome this trade‐off, a multilayer hybrid electrode based on Ag (20 nm)/WO3/Ag (20 nm)/WO3 is designed to obtain high electrical conductance with low optical loss. Compared to conventional devices using a single Ag (40 nm) top electrode, there is a considerable increase in the external quantum efficiency (EQE) of the device using this electrode (from 11.5% to 25.5% at 1000 cd m−2), while maintaining similar sheet resistance. In addition, a large area (≈57 cm2) OLED with the hybrid electrode demonstrates a luminance uniformity of 77% as compared to a device using single silver electrode with uniformity of 66%. Therefore, the proposed Ag/WO3/Ag/WO3 hybrid electrode is a promising choice for the fabrication of efficient and uniform large‐area OLEDs.

Advanced Multilayered Electrode with Planar Building Blocks Structure for High-Performance Lithium-Ion Storage.

To achieve the high-performance of lithium-ion battery, the optimization of electrode materials has generally been considered as the one of the important methods. But most of those works pay attention to the new materials preparation or interface modification rather than the structural innovation. Here, an advanced electrode (GDY/BP/GDY-E) with multilevel layered architecture constructed by planar building blocks stacking structure has been designed and fabricated to explore the structure design of the electrode. This new structure is assembled by graphdiyne (GDY) and black phosphorus (BP) in parallel to form a building block (GDY/BP/GDY). The electric fields between the two GDY sides of the planar building block structure contribute to the superior migration dynamics of lithium ions and desirable pseudocapacitance behavior. Meanwhile, the planar stacking structure of GDY/BP/GDY can efficiently inhibit volume expansion of BP and a series of parasitic reactions of electrolytes during the long-term cycling. The advanced GDY/BP/GDY-E exhibits excellent high-rate performance (1418.8 mAh g-1 at 0.1 A g-1 ) and cycling stability (391.7 mAh g-1 after 5000 cycles at 10 A g-1 ). Such structural design of electrode materials shows a new way to develop high-performance electrodes.

Boosting electrochemical oxidation of As(III) on Fe-doped RuO2/PEDOT/SnO2 nanocomposite anode: Fabrication, performance and mechanism

Design of electrode materials for stable and efficient electrocatalytic oxidation of As(Ⅲ) in arsenic-contaminated groundwater poses a great challenge due to the rapid deactivation of catalysts resulting from the high oxygen evolution potential (OEP) and considerable barrier to generating reactive oxygen species (ROS). Herein, an innovative TNAs/SnO2/PEDOT/Fe(III)-RuO2 multilayer electrode was synthesized by utilizing a PEDOT-coated SnO2 interlayer as a supportive framework to combine Fe-doped amorphous RuO2 catalytic layer with TiO2 nanotube array substrate. Such electrode exhibited high activity and stability for the oxidation of As(III) to As(V) due to the large surface area provided by the TiO2 nanotube arrays and the SnO2/PEDOT interlayer for facilitating the growth of the catalytic layer. The electrochemically active surface area of the electrode reached as high as 31.7 mF/cm2. Impressively, the doping of Fe into RuO2 layer led to a remarkable increase in the OEP value to 3.12 V, which boosted the indirect oxidation process mediated by ROS at a lower potential to achieve the As(III) oxidation ratio of 98.5%. DFT calculations revealed that the Fe-doped amorphous RuO2 weakened the adsorption strength of ·OH and ·SO4− intermediates and lowered the energy barrier for generating ROS. Combined with ESR results, the formation of ·OH and ·SO4− with strong oxidizing properties was fully verified, providing further evidence for the involvement of ROS as the main mediator of the oxidation mechanism of As(III). This work may provide valuable perspectives into the design of catalytic layer structures and heteroatom doping modifications for composite-coated electrodes.

Fabrication of Multi-Layered Paper-Based Supercapacitor Anode by Growing Cu(OH)2 Nanorods on Oxygen Functional Groups-Rich Sponge-Like Carbon Fibers.

This work addresses the challenges in developing carbon fiber paper-based supercapacitors (SCs) with high energy density by focusing on the limited capacity of carbon fiber. To overcome this limitation, a sponge-like porous carbon fiber paper enriched with oxygen functional groups (OFGs) is prepared, and Cu(OH)2 nanorods are grown on its surface to construct the SC anode. This design results in a multi-layered carbon fiber paper-based electrode with a specific structure and enhanced capacitance. The Cu(OH)2 @PCFP anode exhibits an areal capacitance of 547.83 mF cm-2 at a current density of 1mA cm-2 and demonstrates excellent capacitance retention of 99.8% after 10 000 cycles. Theoretical calculations further confirm that the Cu(OH)2 /OFGs-graphite heterostructure exhibits higher conductivity, facilitating faster charge transfer. A solid-state SC is successfully assembled using Ketjen Black@PCFP as the cathode and KOH/PVA as the gel electrolyte. The resulting device exhibits an energy density of 0.21Wh cm-2 at 1.50mW cm-2 , surpassing the performance of reported Cu(OH)2 SCs. This approach, combining materials design with an understanding of underlying mechanisms, not only expands the range of electrode materials but also provides valuable insights for the development of high-capacity energy storage devices.