Composite Interface Research Articles

The effect of electrophoretic deposition of carbon nanotubes on carbon fiber on interfacial properties of the thermoplastic polyimide composite

In order to improve the interfacial properties of carbon fiber/polyimide (CF/PI) composite, silanization reaction carbon nanotubes (CNTs) were introduced to the surface of carbon fiber by electrophoretic deposition to prepare CF/CNT/PI composite. The effects of carbon fiber surface treatment on the mechanical properties of the composites were studied. The results showed that the interlaminar shear strength and bending strength of the composite materials were increased by 11% and 9%, respectively. The scanning electron microscope and Atomic Force Microscope (AFM) was used to analyze the fine structure of composite interface phase. The results show that the introduction of CNTs creates an interface transition layer of CNTs reinforced PI resin between the fiber and the matrix.

Study on manufacturing and mechanical properties of stainless-clad bimetallic steel

The stainless-clad bimetallic steel not only has strong corrosion resistance, but also has low production cost and high strength. Compared with a single stainless steel or ordinary carbon steel material, the strengths of stainless-clad bimetallic steel are obvious, such as a wider market prospect and better material properties. Presently, the stainless-clad bimetallic steel has been successfully applied in the maintenance system of railway steel bridge panels and high-rise building curtain wall. In order to promote the application of stainless-clad bimetallic steel in structural engineering, this paper systematically introduces the manufacturing process of the stainless-clad bimetallic steel, including production technology and welding technology. In addition, the mechanical properties such as corrosion resistance and composite interface properties are studied and analyzed. The research of the stainless-clad bimetallic steel has important economic significance, social significance and strategic value. It is hoped that results from this paper can provide reference for researches on the stainless-clad bimetallic steel in the further.

Fabrication of Ceramic-Polymer Piezo-Composites with Triply Periodic Minimal Interfaces via Digital Light Processing

The geometry of the phase interface in co-continuous piezoelectric composites is critical in improving their piezoelectric properties. However, conventional co-continuous piezoelectric composites are mostly simple structures such as wood stacks or honeycombs, which are prone to stress concentrations at the joints, thus reducing the fatigue service performance and force–electric conversion efficiency of piezoelectric composites. Such simple structures limit further improvements in the overall performance of co-continuous piezoelectric composites. In this study, based on the digital light processing 3D printing method, we investigated the influence of three different structures–the gyroid, diamond, and woodpile interfaces–on the piezoelectric and mechanical properties of co-continuous ceramic/polymer piezoelectric composites. These findings demonstrate that the gyroid and diamond interfaces outperformed the ceramic skeleton of the woodpile interface in terms of both mechanical and electrical properties. When the ceramic volume percentage was 50%, the piezo-composite of the gyroid surface exhibited the greatest hydrostatic figure of merit (HFOM), reaching 4.23×10−12 Pa−1, and its piezoelectric coefficient (d33) and relative dielectric constant (εr) reached 115 pC/N and 748, respectively. The research results lay the foundation for the application of co-continuous piezoelectric composites in underwater communication and detection.

The interface bonding properties of Mg/SiC composite doped with Zr, Al, and Zn elements: A first-principles study

In order to improve the mechanical properties of silicon carbide composite materials based on magnesium, Zr, Al, and Zn are frequently utilized as alloying elements. The mechanical properties of the composite material are closely related to the interface bonding strength. Theoretical calculations on the impact of adding components on the strength of the interface bonding are currently not thorough enough. In this work, the first-principles calculations are performed to investigate the impact of doping Zr, Al, and Zn elements in the Mg matrix on the interface bonding of 6 H-SiC/Mg and the effect of alloy elements on the interface stability and electronic structure in composite interfaces. The results showed that Al and Zn elements may segregate from the interface in the form of a second phase, whereas Zr elements are difficult to segregate from the Mg/SiC composite interface. Zr tends to increase the stability of the Mg/SiC composite interface over the full range of ∆μSi, whereas Al and Zn tend to weaken it. In addition, the stability order of the doped interface is Zr>Al>Zn. The electronic structure of the doping interface shows that the bonding at the interface is both ionic and covalent. The segregation behavior of doped elements at the interface and the variation in covalent bonding strengths between interfaces are the primary variables impacting interface bonding. The internal cleavage layer of the composite material's adhesion work can be examined to reveal that the composite interface is not the material's probable fracture failure point.

Enhancing stability of Pickering emulsions: Insights into the interfacial dynamics of Zein-MCT composite nanoparticles

The interfacial adsorption properties of colloidal particles were critical to the formation and stability of Pickering emulsions. This study aimed to improve the surface hydrophobicity, adsorption properties of Zein nanoparticles (ZN) by using the hydrophobic substance Medium-chain triglyceride (MCT) to form hybrid nanoparticles (ZMN). We investigated the impact of varying Zein/MCT ratios on the interfacial stabilization mechanism of Pickering emulsions and deciphered the relationship between adsorption properties, the rheological behavior of interfacial layer, and emulsion stability. Results revealed that the surface hydrophobicity of nanoparticles affected their adsorption properties as well as the rheological behavior of the composite interface. Specifically, an increase in the Zein/MCT ratio promoted the exposure of hydrophobic groups, increased the surface hydrophobicity of ZMN. This further led to an enhanced diffusion ZMN from the aqueous phase to the interface (Kdiff increased from 0.033 mNm−1s−0.5 to 0.095 mNm−1s−0.5) and the rate of rearrangement at the interface (KR increased from −0.016 mNm−1s−0.5 to −0.009 mNm−1s−0.5) which resulted in rapid adsorption and densely accumulation of ZMN at the interface. Furthermore, the adsorption properties of the nanoparticles directly influenced the viscoelastic and strain properties of the interfacial layer. The interfacial layer composed of ZMN exhibited enhanced viscoelasticity, increasing from 4 mN/m to 7 mN/m at low frequencies and from 6.8 mN/m to 12.5 mN/m at high frequencies. It also exhibited lower viscous dissipation and a stronger deformation response under varying external pressures. As a consequence, the rate and extent of droplet aggregation in ZMN stabilized emulsions (ZMNPEs) were reduced, attributing to the high viscoelasticity as well as the strong strain response of the interfacial layer. This research not only introduces a novel strategy to enhance the stability of Pickering emulsions using Zein-MCT composite nanoparticles, but also deepens our understanding of the interplay between particle adsorption properties, interfacial rheology, and emulsion stability.

Investigation on Thermal Conductivity Silver-coated Copper/GaInSn Composite Thermal Interface Materials

To enhance the heat transfer performance of GaInSn liquid metal, a new type of composite thermal interface material with GaInSn as thermal conductive matrix and silver-coated copper particles as thermal conductive fillers was prepared in this article. The morphology of the composites were characterized by scanning electron microscopy. The thermal conductivity of silver-coated copper/GaInSn composites with different silver-coated copper particle contents were measured by laser flash method. The interfacial bonding of the composites were investigated by X-ray diffraction. The results show that when the volume ratio of silver-coated copper particles is 15%, thermal conductivity of the silver-coated copper/GaInSn composite reaches the largest value of 25.01 W·m−1·K−1. The silver-coated copper/GaInSn composite material and commercially available thermal grease were put into the chip and copper plate to simulate the actual application scenarios for comparison. The heat dissipation capacity of silver-coated copper/GaInSn composite material is obviously better than that of the two commercially available thermal grease, and the chip temperature can be reduced by about 5°C.

Superhydrophobicity PPS@MGFC composite membrane with nanofiber-like structure formed via TIPS and its oil-water separation performance

Oil/ water separation in extreme environments remains a challenging issue, with high requirements for material performance. Polyphenylene sulfide (PPS) has broad application prospects in extreme environments due to its unique performance. In this study, glass fiber cloth (GFC) modified with polydopamine/ phenyltriethoxysilane (PDA/PTES) (hereinafter referred to as MGFC) was used as the support, a superhydrophobic/ superlipophilic PPS nanofiber-like functional layer with low surface energy was prepared via thermally induced phase separation (TIPS) method, (hereinafter referred to as PPS@MGFC composite membrane). Relying on π-π conjugation between PTES and PPS, the composite interface was firmly bonded, effectively enhancing its structural stability. Meanwhile, when the PPS content was 4.2 wt%, the pure-water contact angle reached 156.8°, the oil contact angle reached 0 °. The prepared PPS@MGFC composite membrane showed strong oil-water separation performance in oil-water separation experiments. It could be used to separate various immiscible oil-water mixtures, the water content was less than 150 ppm and flux was higher than 6429 L·m−2·h−1 (gravity drive). For oil-in-water emulsions, the water content was less than 250 ppm, the flux was higher than 2500 L·m−2·h−1 (0.1 bar), and the separation efficiency was higher than 99.9%. In addition, the separation efficiency and flux remained stable in extreme environments and after recycling use. These results indicated that PPS@MGFC composite membrane created in this study has a significant deal of promise for use in the field of oil/water separation.

Interfacial debonding mechanism of magnesium phosphate cement onto old concrete substrates under freeze-thaw conditions

The interface created by the repair of damaged ordinary Portland concrete (OPC) structures using magnesium phosphate cement (MPC) is prone to cracking and debonding under freeze-thaw (F-T) conditions and may even cause engineering disasters. In this study, the entire debonding process, moisture migration and debonding mechanism of the MPC-OPC composite interface under F-T actions were investigated and a novel mixed mode fracture criterion was established. The primary findings are drawn as follows: (i) The interfacial crack initiates and propagates along the interface or kinks into the MPC side during F-T actions, depending on the position and thickness of the localized interface F-T damage zone (IFDZ) close to the interface on the MPC side; (ii) The net suction force causes capillary and film water in the mesopores and micropores to migrate to the freezing macropores inside the interface layer, whereas the increase in the liquid pressure caused by the water-ice phase transition causes crack initiation in the macropores and even the interface layer damage; (iii) The stiffness difference between MPC and OPC increases as the molar ratio of magnesia and phosphate (M/P) or the mass ratio of water to cement (W/B) of MPC increases, and the interface debonding mode shifts from propagating along the interface to kinking into the MPC side.

In Situ Electrochemically‐Bonded Self‐Adapting Polymeric Interface for Durable Aqueous Zinc Ion Batteries

AbstractThe implementation of aqueous zinc ion batteries (AZBs) is hindered by the notorious Zn dendrite growth and side reactions on Zn anodes. Herein, a novel strategy is introduced to overcome these hurdles by designing a self‐adapting soft polymeric composite interface (SAP). Unlike conventional methods relying on passive coating process, the approach leverages dynamic in situ electrochemical bonding via Zn─O interactions formed during cycling, ensuring intimate contact between the SAP interface and Zn electrode. The SAP interface boasts a robust network of hydrogen bonding and electrostatic interactions, which not only promotes the desolvation of Zn2+ and the repulsion of SO42−, facilitating uniform and rapid Zn2+ migration while effectively suppressing parasitic reactions; but also exhibits remarkable self‐adapting and self‐healing capabilities, enabling the interface to accommodate volume changes and repair mechanical failures over prolonged cycling. Consequently, highly reversible Zn electrodes are achieved with SAP, showcasing 3300 h at 1 mA cm−2/0.5 mAh cm−2 and 350 h at 20 mA cm−2/10 mAh cm−2 in the symmetric cells. The advantages of the SAP interface are further verified when paired with high mass loading LiMn2O4 cathodes in AZBs. The versatile SAP interface offers insights into advanced interface design for efficient and durable AZBs.

Synthesis of fractal crystallized organic microspheres together with constructing full covalent bonding at the interface to strengthen and toughen aramid fiber composites

Regulating the interface to simultaneously enhance the strength and toughness of aramid fiber composites remains a great challenge. Herein, a resilient, full covalent interface was constructed by introducing fractal crystallized organic microspheres into the interface of aramid fiber composites using the twice fluorination approach. Firstly, the aromatic polyamide with ether bonds was synthesized, and the fractal crystallized microspheres with a porous surface containing amino groups were prepared by thermally induced solution self-assembly. Subsequently, the twice fluorination method introduces C–F bonds to the surfaces of both fibers and microspheres, respectively. Then, the covalent bonds among fibers, microsphere, and resin were formed by the derivative reaction of C–F bonds. This interface boosts the interlaminar shear strength (ILSS) of composites by 100.5% to 36.7 MPa and the unnotched impact toughness of composites by 13.5%–1363 kJ/m2. Comparative analyses reveal the full covalent interface and the fractal structure of microspheres contribute 47.8% and 52.2% to the ILSS enhancement, respectively. In addition, the fractal structure of microspheres is the only factor for increased toughness. Finite element analysis reveals that the fractal crystallized microspheres combined with full covalent interface facilitate elastic stress transfer within the composites to enhance the performance of composites.

Molecular engineering of N-rich ZIF-integrated graphene composite interface for efficient physiochemical confinement and catalytic conversion of polysulfides in lithium–sulfur batteries

Lithium–sulfur (Li–S) batteries are regarded as one of the most promising energy storage systems because of their high theoretical specific capacity, energy density, low cost, and environmental benignancy. However, the practical application of Li–S batteries has been hindered by inevitable polysulfides shuttling behavior, the sluggish redox kinetics, and poor electrical conductivity of sulfur, which lead to rapid capacity decay and low active material utilization. In this study, we report a multifunctional layer consisting of N-rich zeolitic imidazolate frameworks (ZIF)/reduced graphene oxide (rGO) composite (NZG) as an electrocatalyst to overcome the drawbacks of Li–S batteries. During the preparation of NZG, deamination of the ZIF8A induces the incorporation of abundant N-containing moieties into rGO (pyridinic and pyrrolic N), which results in providing favorable active sites for polysulfides confinement and their rapid conversion via physiochemical interactions. Additionally, hierarchical pores with large surface area and interconnected conductive pathways in the as-prepared multifunctional layer accelerate the catalytic conversion kinetics of polysulfide species, leading to high sulfur utilization and enhanced Li–S battery electrochemical performance. This work suggests an efficient approach for designing multifunctional layers to achieve high-performance Li–S batteries.

Measuring the interlaminar fracture toughness of thin carbon fiber/polyamide6 composites using adhesively bonded stiffeners

The present work investigates the interlaminar fracture toughness of a thin unidirectional carbon fiber-reinforced/polyamide6 (CF/PA6) composite laminate. Aluminum (Al) stiffening beams are adhesively bonded on both sides of the thin laminate to avoid undesirable large deformations during the subsequent double cantilever beam tests. Experimentation with various surface treatment techniques and different adhesives is presented, from which it is concluded that the mode I fracture toughness of the CF/PA6 laminate is always higher than the fracture toughness of the adhesives used. Consequently, the crack initiates at the Al–composite interface. A finite element (FE) model is proposed, and quantitative results for the fracture toughness of the laminate are provided (e.g., GIc,ini=2.1N/mm). Overall, the study highlights the challenges in the adhesive joining of stiffening beams to CF/PA6 surfaces, ways to improve adhesion, and the FE simulation as an alternative to determining the interlaminar fracture toughness of such thin laminates.

Insights into nano-mechanical degradation behavior of Ag/Ti2AlC composite under different arc erosion stages

Serious arc erosion is the main reason for premature failure of the Ag-matrix composite electrical contact materials in actual service. Clarifying the structure and property degradation process is crucial for creating eco-friendly Ag/MAX electrical contacts and upgrading high-performance materials for low-voltage switch applications. In this study, the representative Ag/Ti2AlC electrical contacts were designed into three arc erosion stages (from 1 to 5610 cycles) by ex-situ arc discharging experiment, and the nanoindentation technique was then applied to in-depth analyze the evolution behavior of nano-mechanical properties by comparing nano hardness, modulus, creep, continuous stiffness, elastic/plastic deformation, and NanoBlitz 3D Mapping indentation results in different erosion stages. Finally, the inherent relationship among the structural dissociation of Ti2AlC, and compositional changes of Ag/Ti2AlC interface and nano-mechanical properties of composite was revealed, and the material degradation model and anti-arc erosion mechanism were proposed. This work further elucidates the intrinsic source of excellent arc erosion resistance and degradation process of Ag/Ti2AlC composite from the nano-mechanical perspective and lays a theoretical foundation for the future design and optimization of this material system.

Investigation of Interface Discharge Characteristics for Cable Accessories After Moisture Penetration Into the XLPE–SiR Interface

For cable accessories, environmental moisture inevitably gradually diffuses into the XLPE-SiR composite interface. The penetrated moisture always causes interface insulation degradation and failure. In this paper, to investigate the discharge characteristics at the interface insulation, a composite interface discharge experimental unit is performed, and the insulation deterioration when the interface remains dry or becomes damped are discussed and analyzed. Combined with optical tests, discharge signal tests, SEM and EDS tests, the interface discharge characteristics are studied. In addition, several analysis models are established, and the discharge processes of the interface insulation are discussed in detail. Moreover, several field cases are discussed and compared to better understand the interface discharge. It is found that the discharge trace is mainly concentrated in one channel when the insulation remains dry. Moisture-induced early deterioration of the interface insulation is characterized by the emergence of non-conductive regions and weak dendritic discharge. As the interfacial water content increases, weak dendritic discharge turns into a macroscopic one. The occurrence and development of discharge after interface wetting can be attributed to two main factors. On one hand, interface discharge is related to the interface electric field distribution and interface contact morphology. On the other hand, the discharge performance is strongly influenced by the electric field distortion caused by water droplets, size of the dry area between water droplets, and increase in electrical losses ascribed to the invading moisture. The ultimate damage to the interface insulation takes two forms: continuous thermal breakdown that erodes the insulation, and instantaneous arc breakdown at the interface.

Study on Ground Settlement Patterns and Prediction Methods in Super-Large-Diameter Shield Tunnels Constructed in Composite Strata

This study focuses on investigating the surface settlement characteristics induced by the construction of a super-large-diameter shield tunnel in composite strata. By utilizing a combination of field monitoring and numerical simulation analysis, the surface settlement patterns encountered during the construction process in horizontally distributed typical soil–rock composite strata were summarized based on the 16.03 m super-large-diameter shield tunnel project in the southerly extension of He’ping Avenue in Wuhan. In addition, the collected data were used to enhance the Peck empirical formula. The results of the study show the following: (1) Significant non-uniform settlement occurs along the tunneling direction when the shield machine passes through soil–rock composite strata. The range of non-uniform settlement is approximately 3.1 times the tunnel diameter (D) in soil sections and 1.9 times the tunnel diameter (D) in rock sections. (2) The impact of composite strata on the maximum settlement is greater than its effect on the settlement trough width, with a larger impact within the soil sections compared to the rock sections. (3) The Peck correction formula, which takes into account the distance between the monitoring cross-section and the composite interface, provides more accurate predictions than the original Peck empirical formula.

Investigating the Influence of Diffusion on the Cohesive Zone Model of the SiC/Al Composite Interface.

Modeling metal matrix composites in finite element software requires incorporating a cohesive zone model (CZM) to represent the interface between the constituent materials. The CZM determines the behavior of traction-separation (T-S) in this region. Specifically, when a diffusion zone is formed due to heat treatment, it becomes challenging to determine experimentally the equivalent mechanical properties of the interface. Additionally, understanding the influence of heat treatment and the creation of a diffusion zone on the T-S law is crucial. In this study, the molecular dynamics approach was employed to investigate the effect of the diffusion region formation, resulting from heat treatment, on the T-S law at the interface of a SiC/Al composite in tensile, shear, and mixed-mode loadings. It was found that the formation of a diffusion layer led to an increase in tensile and shear strengths and work of separation compared with the interfaces without heat treatment. However, the elastic and shear moduli were not significantly affected by the creation of the diffusion layer. Moreover, the numerical findings indicated that the shear strength in the diffusion region was higher when compared with the shear strength of the {111} slip plane within the fcc aluminum component of the composite material. Therefore, in the diffusion region, crack propagation did not occur in the pure shear loading case; however, shear sliding was observed at the aluminum atomic layers.

Double Effects of Oxidative Aging on Carbon Nanotube-Asphalt Nanocomposite Interfaces: Enhancement and Deterioration.

Understanding the mechanisms of oxidative aging effects on the carbon nanotube (CNT)-asphalt nanocomposite interface has long been a challenge, as there are two opposing effects: enhancement and deterioration. In this study, a multiscale coupling method is proposed to analyze the dual effect of oxidative aging on the CNT-asphalt nanocomposite. The method is based on density functional theory (DFT) and molecular dynamics (MD) simulations, supported by microscopic interface observation and macroscopic property testing with a focus on the composite interface. The results show that oxidative aging has a resetting effect on benzene ring stacking at the interface and enhances the binding energy of CNT-asphalt. Meanwhile, oxidative aging enhanced the interfacial charge transfer, but no chemical reaction occurred between CNT-aged asphalt. This is also verified by Fourier Transform Infrared Spectroscopy (FTIR). Enhancement and degeneration effects of oxidative aging occur via distinct mechanisms. Oxidative aging enhanced the interfacial shear barrier by approximately 5% and the energy barrier by 44.87%, which increased the high-temperature deformation resistance of the CNT-asphalt nanocomposites. However, molecular oxidation was not responsible for the decline in the fatigue resistance. According to scanning electron microscopy (SEM) and atomic force microscopy (AFM) results, oxidative aging elevates the content of polar molecules, leading to an increase in the solid properties of asphalt and a 39.6% decrease in surface adhesion. This disrupts the three-dimensional network of the CNT and ultimately leads to a reduction in crack resistance. This study clarifies the mechanism underlying the dual effect of oxidative aging and provides fundamental support for understanding asphalt aging behavior and the interfacial behavior of composites.

Stable anode interface regulation of solid sodium battery through oxygen potential regulation

Solid sodium ion batteries (SSIBs) is the potential development direction of the next generation of energy storage technology owing to their low cost and superior safety. However, a series of problems such as high interfacial resistance and dendrites growth during the cycling process seriously hinder its practical application. Herein, a novel stable composite interface consisting of Ce0.8Gd0.2O1.9 (CGO) and Na5YSi4O12 (NYS) was constructed by a facile screen-printing method. The CGO with high oxygen fugacity can conduct oxygen ions to fill the oxygen vacancies due to interfacial reactions, homogenize the electric-field distribution, and impede electron conduction, thus inhibiting interfacial side reactions and dendrite growth. Therefore, the Na/NYS/Na symmetric battery can cycle stably for 3000 h at 0.1 mA cm−2 without short circuit and the NVP/NYS/Na full cell also exhibits a good electrochemical performance. This work makes an important contribution to the future development of safe and stable solid-state sodium battery systems.

Atomic pins bridging integrated surface to assist high-rate stability for Co-free Li-rich cathode

Li- and Mn-rich oxides (LMR) have emerged as promising cathode materials for next-generation Li-ion batteries due to their cost effectiveness, impressive capacity, and high energy density. However, the poor electrochemical kinetics and structural instability in hostile interface environments have result in continuous voltage/capacity decay and undesirable rate performance, impeding the large-scale commercial application of LMR materials. In this study, we introduce an atomic pins-assisted integrated surface reconstruction (AISR) strategy to address the interfacial degradation and instability issues. Utilizing the bidirectional diffusion effect of the aluminum-containing intermediate layer during the heat treatment process, we employ aluminum atoms as bridging centers to in situ construct a composite interface structure. This approach capitalizes on the element diffusion reaction and anchoring effect to achieve multifunctional modification through the Al-based ionic conductor network constructing and near-surface Al doping for LMR material. Intriguingly multiple kinetic investigations and calculations reveal that the epitaxial ionic conductor layer suppresses interfacial side reactions, enhances ionic conductivity, and improves electronic conductivity by regulating cationic/anionic redox activity through Al surface doping.Impressively, the modified electrodes exhibited an increased reversible capacity at both 0.1C/5C rates (0.1C, 2 ∼ 4.8 V, from 264.2 mAh∙g−1 to 274 mAh∙g−1; 5C, 2 ∼ 4.6 V, from 145.5 mAh∙g−1 to 197.9 mAh∙g−1) and improved capacity retention after 250 cycles at 1C/5C rates (2 ∼ 4.6 V: 1C, from 69.46% to 81.92%; 5C from 57.73% to 81.35%). We systematically summarized the rate-dependent failure mechanism and the corresponding integrated interface reconstruction principle. These key findings offer valuable insights for the development of high-energy–density and long-life lithium-ion batteries in commercial applications.

A three-dimensional in-situ self-electrolysis system based on Ni3(HITP)2/graphene-based composite aerogel particle electrodes for efficient deep removal of phenol from coking wastewater

Herein, a Ni3(HITP)2/graphene-based composite aerogel (Ni3(HITP)2/GA) particle electrode is developed for the oxidation removal of phenol with three-dimensional electrode technology. The as-constructed three-dimensional electrode system possesses high in-situ self-electrolysis capacity and achieves highly efficient degradation of phenol, completely removed within 15 min with a decomposition rate constant of 0.3283 min−1. Ni3(HITP)2 in Ni3(HITP)2/GA and the tetradentate Ni–N2O2 coordination bond generated at the composite interface produce H2O2 highly selectively via the 2e- ORR pathway. The graphene layer converts H2O2 into •OH by using the 1e- of Ni3(HITP)2 excitation and the microelectrode action of the particle electrode. Furthermore, the simultaneous generation of •OH and O2•- in the system greatly reduces the dependence on acidic environment and broadens the scope of utilization. The present work provides a new strategy for the efficient construction of particle electrodes in 3D electrode systems, which allows their potential application in the purification of coking wastewater.