Material Architecture Research Articles

Nanometer-Scale 1D Negative Differential Resistance Channels in Van Der Waals Layers.

Negative differential resistance (NDR) is the key feature of resonant tunneling diodes exploited for high-frequency and low-power devices and recent studies have focused on NDR in van der Waals heterostructures and nanoscale materials. Here, strong NDR confined along a 1-nm-wide 1D channel within a van der Waals layer 1T-TaS2 is reported. Using scanning tunneling microscopy, a double 1D NDR channel formed along the sides of a charge-density-wave domain wall of 1T-TaS2 is found. The density functional theory calculation elucidates that the strong local band-bending at the domain wall and the interlayer orbital overlap cooperate to bring about 1D NDR channels. Furthermore, the NDR is well controlled by changing the tunneling junction distance. This result would be important for nanoscale device applications based on strong nonlinear resistance within van der Waals material architectures.

Enhancing the photovoltaic performance of dithienobenzodithiophene based polymer donors through backbone fluorination and radical polymer additives

Unveiling the corresponding relationship between the molecular architecture of organic semiconductor materials and the morphology within the active layer of the organic solar cells (OSCs) is essential for the innovation of novel optical materials and the refinement of device optimization strategies to overcome the bottlenecks in efficiency. In this work, three dithieno[3,2-b]benzo[1,2-b;4,5-b’]dithiophene(DTBDT)-alt-benzothiadiazole (BT) based polymer donors (PDTBDT-F-BT, PDTBDT-F-FBT, and PDTBDT-F-2FBT) with varying fluorine atom content within their acceptor segments were designed and synthesized, and the photovoltaic performances of these polymers when blended with Y6 were meticulously investigated. Incorporating fluorine atoms into the BT segment was observed to not only incrementally increase the optical bandgap, lower the HOMO energy level, and bolster the self-aggregation of the polymer, but also effectively reduce the surface energy of the resulting polymer, thereby altering the donor-acceptor (D-A) interfacial spacing and the phase separation in the blend films as illustrated by molecular dynamic simulations and morphology characterization. As a result, the OSCs fabricated using PDTBDT-F-FBT, which incorporates a single fluorine substitution in the BT unit, demonstrated the highest power conversion efficiency (PCE) of 9.92 %. More importantly, this blend film's morphology is likely to be more conducive to the incorporation of the radical polymer additive, GDTA. This has resulted in a notable reduction in voltage loss, ultimately achieving a higher PCE of 11.55 % for the PDTBDT-F-FBT:Y6 based OSCs. This research uncovered a synergistic impact of backbone fluorination and the incorporation of radical polymer additives, which contributed to reducing the energy loss and enhancing the efficiency of OSCs from DTBDT-based polymer donors.

On-chip warped three-dimensional InGaN/GaN quantum well diode with transceiver coexistence characters

Featured with light emission and detection coexistence phenomenon, nitride-based multiple-quantum-well (MQW) diodes integrated chip has been proven to be an attractive structure for application prospects in various fields such as lighting, sensing, optical communication, and other fields. However, most of the recent reports are based on planar structures. Three-dimensional (3D) structures offer extra advantages in direction and polarization and absorption modulation and may start a new way to make the same thing over and over with interesting properties. In this paper, we designed and fabricated a single-cantilever InGaN/GaN MQW diode with warped 3D microstructure via standard microfabrication technology. Experimental results indicate that the strain architecture of the multi-layer materials is the key principle for the self-warped device. The planar structure will bear greater compressive stress while the warped beam part has less stress, resulting in differences in the optical and electrical performance. The strain-induced band bending highly influences the emission and detection properties, while the warped structure will introduce direction selectivity to the 3D device. As an emitter, 3D structures have a directional emission with lower turn-on voltage, higher capacitance, increased luminous intensity, higher external quantum efficiency (EQE), high -3dB bandwidth, and redshifted peak wavelength. Besides, it can serve as an emitter for directional-related optical communication. As a receiver, 3D structures have lower dark-current, higher photocurrent, and red-shifted response spectrum and also show directional dependence. These findings not only deepen the understanding of the working principle of the single-cantilever GaN devices but also provide important references for device performance optimization and new applications in visible light communication (VLC) technology.

Heterojunction-structured Ni0.85Se/CoSe nanoparticles anchored on holey graphene for performance-enhanced sodium-ion batteries

Graphene-based metal selenides, are increasingly recognized for their potential in sodium-ion battery applications due to their superior electrochemical properties. The unique structure of graphene facilitates rapid in-plane transport of sodium ions, but the interlayer diffusion remains a significant challenge. The Ni0.85Se@CoSe heterojunctions, strategically grown adjacent to the graphene pores, offer a novel solution by creating in-plane holes that serve as direct channels for vertical ion transport, thereby enhancing cross-layer sodium ion permeation. The incorporation of Ni0.85Se@CoSe heterojunctions with holey graphene (NCS/HG) significantly enhances the reaction dynamics between sodium ions and anode material. These heterojunctions not only promote easier sodium ion insertion/extraction process by reducing the Na+ adsorption energy, but also improve the electrical conductivity by adjusting the band gap. The configuration supports high current density applications (573.5 mAh/g at 5.0 A/g), and ensures robust cycle stability with a capacity retention rate of 97 % after 1000 cycles at 2.0 A/g. Therefore, the development and etching techniques employed in engineering the Ni0.85Se@CoSe/HG graphene-based anodes exemplify a significant advancement in anode material design, highlighting the importance of material architecture in the development of high-performance energy storage devices.

Lift-Out Specimen Preparation and Multiscale Correlative Investigation of Li-Ion Battery Electrodes Using Focused Ion Beam-Secondary Ion Mass Spectrometry Platforms.

Advanced characterization is paramount to understanding battery cycling and degradation in greater detail. Herein, we present a novel methodology of battery electrode analysis, employing focused ion beam (FIB) secondary-ion mass spectrometry platforms coupled with a specific lift-out specimen preparation, allowing us to optimize analysis and prevent air contamination. Correlative microscopy, combining electron microscopy and chemical imaging of a liquid electrolyte Li-ion battery electrode, is performed over the entire electrode thickness down to subparticle domains. We observed a distinctive remnant lithiation among interparticles of the anode at the discharge state. Furthermore, chemical mapping reveals the nanometric architecture of advanced composite active materials with a lateral resolution of 16 nm and the presence of a solid electrolyte interface on the particle boundaries. We highlight the methodological advantages of studying interfaces and the ability to conduct high-performance chemical and morphological correlative analyses of battery materials and comment on their potential use in other fields.

Ar[formula omitted]i-Textile composites: Role of weave architecture on mode-I fracture energy in woven composites

This paper investigates the impact of weave architectures on the mechanics of crack propagation in fiber-reinforced woven polymer composites under quasi-static loading. Woven composites consist of fabrics/textiles containing fibers interwoven at 0 degrees (warp) and 90 degrees (weft) bound by a polymer matrix. The mechanical properties can be tuned by weaving fiber bundles with single or multiple materials in various patterns or architectures. Although the effects of uniform weave architectures, like plain, twill, satin, etc. on in-plane modulus and fracture energy have been studied, the influence of patterned weaves consisting of a combination of sub-patterns, that is, architected weaves, on these behaviors is not understood. We focus on identifying the mechanisms affecting crack path tortuosity and propagation rate in composites with architected woven textiles containing various sub-patterns, hence, Arχi(ar.kee)-Textile Composites. Through compact tension tests, we determine how architected weave patterns compared to uniform weaves influence mode-I fracture energy of woven composites due to interactions of different failure modes. Results show that fracture energy increases at transition regions between sub-patterns in architected weave composites, with more tortuous crack propagation and higher resistance to crack growth than uniform weave composites. We also introduce three geometrical parameters — transition, area, and skewness factors — to characterize sub-patterns and their effects on in-plane fracture energy. This knowledge can be exploited to design and fabricate safer lightweight structures for marine and aerospace sectors with enhanced damage tolerance under extreme loads.

Emerging Zinc‐Ion Capacitor Science: Compatible Principle, Design Paradigm, and Frontier Applications

AbstractThe development of high energy/power density and long lifespan device is always the frontier direction and attracts great research attention in the energy storage fields. Zinc‐ion capacitors (ZICs), as an integration of zinc‐ion batteries and supercapacitors, have been widely regarded as one of the viable future options for energy storage, owing to their variable system assembly method and potential performance improvement. However, the research of ZICs still locate at initial stage until now, and how to construct the suitable systems for different condition is still challenging. Herein, the recent advance in the rational design of ZICs is reviewed in order to construct related theory including compatible principle and design paradigm. It starts with a systematically summary of the fundamental theory as well as the motivation. Then, the electrode materials are classified into capacitor‐type and battery‐type based on the storage mechanism, and the design strategies and progress of these two‐type candidates are comprehensively discussed, aiming to reveal the inherent relationship between the performance of devices and the component as well as architecture of electrode materials. Beyond that, the future perspectives in this emerging field are also given, expecting to guide the construction of high‐performance ZICs for practical applications and boost its development.

Growth of VO2-ZnS thin film cavity for adaptive thermal emission

Low-weight, passive, thermal-adaptive radiation technologies are needed to maintain an operable temperature for spacecraft while they experience various energy fluxes. In this study, we used a thin film coating with the Fabry–Pérot (FP) effect to enhance emissivity contrast (Δε) between VO2 phase-change states. This coating utilizes a hybrid material architecture that combines VO2 with a mid- and long-wave infrared transparent chalcogenide, zinc sulfide (ZnS), as a cavity spacer layer. We simulated the design parameter space to obtain a theoretical maximum Δε of 0.63 and grew prototype devices. Using x-ray diffraction, Raman spectroscopy, and Fourier transform infrared spectroscopy (FTIR), we determined that an intermediate buffer layer of TiO2 is necessary to execute the crystalline growth of monoclinic VO2 on ZnS. Through temperature-dependent FTIR measurements, our fabricated devices demonstrated FP-cavity enhanced adaptive thermal emittance.

Heteroatom Immobilization Engineering toward High-Performance Metal Anodes.

Heteroatom immobilization engineering (HAIE) is becoming a forefront approach in materials science and engineering, focusing on the precise control and manipulation of atomic-level interactions within heterogeneous systems. HAIE has emerged as an efficient strategy to fabricate single-atom sites for enhancing the performance of metal-based batteries. Despite the significant progress achieved through HAIE in metal anodes for metal-based batteries, several critical challenges such as metal dendrites, side reactions, and sluggish reaction kinetics are still present. In this review, we delve into the fundamental principles underlying heteroatom immobilization engineering in metal anodes, aiming to elucidate its role in enhancing the electrochemical performance in batteries. We systematically investigate how HAIE facilitates uniform nucleation of metal in anodes, how HAIE inhibits side reactions at the metal anode-electrolyte interface, and the role of HAIE in promoting the desolvation of metal ions and accelerating reaction kinetics within metal-based batteries. Finally, we discuss various strategies for implementing HAIE in electrode materials, such as high-temperature pyrolysis, vacancy reduction, and molten-salt etching and anchoring. These strategies include selecting appropriate heteroatoms, optimizing immobilization methods, and constructing material architectures. They can be utilized to further refine the performance to enhance the capabilities of HAIE and facilitate its widespread application in next-generation metal-based battery technologies.

Direct Ink Write 3D Printing of Fully Dense and Functionally Graded Liquid Metal Elastomer Foams

AbstractLiquid metal (LM) elastomer composites offer promising potential in soft robotics, wearable electronics, and human‐machine interfaces. Direct ink write (DIW) 3D printing offers a versatile manufacturing technique capable of precise control over LM microstructures, yet challenges such as interfilament void formation in multilayer structures impact material performance. Here, a DIW strategy is introduced to control both LM microstructure and material architecture. Investigating three key process parameters–nozzle height, extrusion rate, and nondimensionalized nozzle velocity–it is found that nozzle height and velocity predominantly influence filament geometry. The nozzle height primarily dictates the aspect ratio of the filament and the formation of voids. A threshold print height based on filament geometry is identified; below the height, significant surface roughness occurs, and above the ink fractures, which facilitates the creation of porous structures with tunable stiffness and programmable LM microstructure. These porous architectures exhibit reduced density and enhanced thermal conductivity compared to cast samples. When used as a dielectric in a soft capacitive sensor, they display high sensitivity (gauge factor = 9.0), as permittivity increases with compressive strain. These results demonstrate the capability to simultaneously manipulate LM microstructure and geometric architecture in LM elastomer composites through precise control of print parameters, while maintaining geometric fidelity in the printed design.

Digital composite lattice materials for fast but robust assembly

The unique and complex architecture of lattice materials enable their excellent mechanical properties and multifunctionality, but how to realize their efficient production remains a challenge for large-scale structural application. In this study, a discrete assembly strategy was developed for lattice materials with planar elements (termed as clips) and a newly proposed joint design inspired by Chinese traditional mortise and tenon art. The clips were prepared through conventional mechanical cutting or additive manufacturing, and the assembled lattice materials were respectively tested. Different failure modes were observed in the clips but joint failure rarely occurred. Future application of the assembled digital lattice composites for emergency rescue scenarios was examined, where their portability and shape customization advantages fully revealed.

Mechanical properties and fracture phenomena in 3D-printed helical cementitious architected materials under compression

The mechanical response and fracture behavior of two architected 3D-printed hardened cement paste (hcp) elements, ‘lamellar’ and ‘Bouligand’, were investigated under uniaxial compression. A lab-based X-ray microscope was used to characterize the post-fracture crack pattern. The mechanical properties and crack patterns were analyzed and compared to cast hcp. The role of materials architecture and 3D-printing-induced weak interfaces on the mechanical properties and fracture behavior are discussed. The pore architecture that inadvertently forms in the design of solid architected materials dictated the overall mechanical response and fracture behaviors in both 3D-printed architected materials. While no specific crack pattern or microcracking was observed in the cast element, lamellar architecture demonstrated a crack pattern following weak vertical interfaces. Bouligand architectures, on the other hand, exhibited a helical crack pattern with distributed interfacial microcracking aligned with the helical orientation of filaments. As a result, the bouligand architected elements showed a significant 40% increase in work-of-failure compared to cast counterparts. The enhanced energy absorption was obtained without sacrificing the strength and was attributed to higher fractured surface and microcracking, both of which follow the weak helical interfaces.

Geometric symmetry and mechanical behavior of Topologically Interlocked Material systems from skewed building blocks

Architectured materials are engineered materials with specific geometries and arrangements to exhibit desired mechanical properties. One class of architectured material is the Topologically interlocked material (TIM) system. In TIM systems, a plurality of convex particles is assembled under specific geometric constraints such that a load-carrying structure is obtained without the need for an adhesive bond between building blocks. Past investigations have considered TIM systems with building blocks and assemblies with a high degree of symmetry. Here the geometric constraints commonly imposed on the geometry of the system are relaxed. Two new types of skewed building blocks are introduced: one with only a rotational symmetry and no mirror symmetry, and one without rotational or mirror symmetry. These blocks are used to build even and odd-numbered assemblies and to create TIM systems with both mirror and rotational symmetry, rotational symmetry only, and no symmetry. A vector field representing the material architecture is introduced and demonstrated to connect architecture and mechanical behavior. It is demonstrated that load transfer patterns in the TIM system closely match the geometric symmetry. This allows for the demonstration of achiral and chiral mechanical behavior as represented by the presence of reaction moments for the centrally loaded square TIM assembly. The chirality of the building blocks manifests itself in the mechanical behavior of the TIM system only once the deflection of the system opens the contacts between building blocks such that building blocks accommodate deformation. Chiral building blocks diffuse the load from the central load path dominant in the TIM systems built from achiral blocks. This construction concept allows for simultaneous improvements in mechanical properties (strength and stiffness) solely from geometry.

A Multiscale Computational Modeling Framework to Quantify Microstructural Effects on Nucleation of Li Metal on Carbon Scaffold Architectures

Carbon materials with scaffold architecture have been shown to mitigate the non-uniform Li plating/stripping issues during cycling, which is critical for achieving significantly enhanced energy densities and improved safety of Li metal batteries. However, optimal design of the architecture and microstructure of the carbon materials requires fundamental understanding of the Li metal nucleation behavior at different length scales. In this poster, we present a multiscale computational modeling framework to quantify the microstructural effects of carbon materials on the tendency of Li metal nucleation during plating by integrating atomic-scale simulation, mesoscale microstructure-based homogenization, continuum-scale electrochemistry modeling, and classical nucleation theory. We modeled the architecture of the carbon scaffold and the electrochemistry of Li transport across the electrode and electrolyte by finite element simulation to determine boundary conditions for our mesoscale models. We then generated different porous microstructures of various carbon materials by stochastic and physics-based simulations informed from experiments and performed multiphysics-based simulations at mesoscale to identify the electro-chemo-mechanical hotspots which are sensitive to the microstructure morphology. We calculated the energy barriers for Li to form clusters on graphene surfaces as a function of local Li concentrations and electric fields by ab initio molecular dynamics simulations. The synergistic deployment of different models across scales allows us to theoretically estimate the Li metal nucleation tendency based on a modified classical nucleation theory for different microstructures under various electroplating conditions. Comparison of the theoretical predictions and experimental results will be briefly discussed. The insights obtained from this multiscale framework offer new understanding and strategies for the design of carbon scaffold architectures to mitigate the non-uniformity of Li plating and issues in Li metal anode deployment in solid-state batteries.This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344 and 22-ERD-043.

(Invited) Probing Electrochemical Interfaces in Catalytic and Energy Materials and Process Using Operando Soft X-Ray Spectroscopy

Advanced energy technology arises from the understanding in fundamental science, thus rest in large on in-situ/operando characterization tools for observing the physical and chemical interfacial processes. Synchrotron based X-ray spectroscopic techniques offers unique characterization in many important energy materials of energy conversion, energy storage and catalysis in regards to the functionality, complexity of material architecture, chemistry and interactions among constituents within. However, it is challenging to reveal the real mechanism of the chemical processes.In the operando soft X-ray spectroscopy characterization of interfacial phenomena in energy materials and devices, it has been found that the microstructure and composition of materials as well as the microstructure evolution process have a great influence on performances in a variety of fields, e.g., energy conversion and energy storage materials, chemical and catalytic processes. This presentation will show how to best use the in-situ/operando soft X-ray spectroscopy characterization techniques, including soft x-ray absorption spectroscopy (XAS) and resonant inelastic soft X-ray scattering (RIXS) to investigate the real electrochemical mechanism during the operation. The experimental results show how in-situ/operando soft X-ray spectra characterization techniques uncover the phase conversion, chemical and environmental change of elements and other very important information of solid/gas and solid/liquid interfaces in real time, thus further enhance the understanding of real reaction mechanism.

Frequency-band programmable piezoelectric energy harvesters with variable substrate material, tip mass and fractal architectures: Experimental and numerical investigations

To automate the approach of assessing the health and efficacy of large structural systems globally through structural health monitoring systems, a vast network of sensors that must be mounted throughout the entire structure and connected to a continuous power supply is necessary. Clusters of wires need to be placed throughout the structures to support the network, or batteries must be changed frequently, adding to the network’s high maintenance expenses. The present study investigates the scope of powering such low-energy devices with a localized renewable energy source based on smart piezoelectric components such as PZT-patched energy harvesting systems. This paper analyses the performance of the PZT patch mounted on different structures that are predominantly activated in d 31 mode. A vibration testing rig is manufactured to perform experiments for investigating the effect of material properties, natural frequencies, vibrating structural mass, and their interaction with the output power of a PZT transducer. Optimal mass, material, and structural configurations are attempted to be identified experimentally. The hypothesis, predictions, and results are evaluated further based on a converged finite element model. Subsequently, we introduce a novel concept of chiral fractal substrates in piezoelectric energy harvesters, wherein a significant improvement is noticed in the energy output along with increased frequency-band programmability. The power output of such architected and optimized energy harvesters holds the potential to serve as a reliable and sustainable alternative to conventional batteries, effectively providing a renewable source of power to energize and sustain low-power micro-electro-mechanical systems (MEMS) and devices.

Inverted optical functionality of phase change material surfaces through Mie resonances of VO2@Si core–shell structures

Vanadium dioxide (VO2) has attracted extensive attention due to its reversible transition from the insulator to metal phase at a critical temperature of 68°C. Below the critical temperature VO2 transmits the infrared radiation in the insulator phase, whereas above the critical temperature VO2 reflects the infrared portion of the incident radiation. However, smart surface interfaces for high-temperature emitter surfaces require the opposite functionality within the 1–3 µm spectral range. Here, we demonstrate that a core–shell structure, composed of VO2@Si, which is deposited on a thin layer of Ag, achieves the inverted optical functionality within the 1–3 µm spectral range, making it ideal as smart interfaces for radiative heat applications as high-temperature emitters. The proposed material architecture also increases the thermal stability of VO2 in addition to enhancing its optical properties in near-infrared region. The results were obtained using numerical simulations. Our results indicate that in its metallic state, the core–shell structure with metallic underlayer promotes efficient absorption in the near-infrared spectrum. On the other hand, in its insulating state dielectric resonances within the core–shell structure along with the metallic underlayer, resulting in increased reflection, offer inverse optical functionalities. Our findings present a significant step toward designing dynamic filters that can efficiently capture and respond to changing conditions in the near-infrared spectrum.

Review of Compensation Topologies Power Converters Coil Structure and Architectures for Dynamic Wireless Charging System for Electric Vehicle

The increasing demand for wireless power transfer (WPT) systems for electric vehicles (EVs) has necessitated advancements in charging solutions, with a particular focus on speed and efficiency. However, power transfer efficiency is the major concern in static and dynamic wireless charging (DWC) design. Design consideration and improvements in all functional units are necessary for an increase in overall efficiency of the system. Recently, different research works have been presented regarding DWC at the power converter, coil structure and compensators. This paper provides a comprehensive review of power converters incorporating high-order compensation topologies, demonstrating their benefits in enhancing the DWC of EVs. The review also delves into the coupling coil structure and magnetic material architecture, pivotal in enhancing power transfer efficiency and capability. Moreover, the high-order compensation topologies used to effectively mitigate low-frequency ripple, improve voltage regulation, and facilitate a more compact and portable design are discussed. Furthermore, optimal coupling and different techniques to achieve maximum power transfer efficiency are discussed to boost magnetic interactions, thereby reducing power loss. Finally, this paper highlights the essential role of these components in developing efficient and reliable DWC systems for EVs, emphasizing their contribution to achieving high-power transfer efficiency and stability.

One-Pot Self-Assembly of Sequence-Controlled Mesoporous Heterostructures via Structure-Directing Agents.

Multimaterial heterostructures have led to characteristics surpassing the individual components. Nature controls the architecture and placement of multiple materials through biomineralization of nanoparticles (NPs); however, synthetic heterostructure formation remains limited and generally departs from the elegance of self-assembly. Here, a class of block polymer structure-directing agents (SDAs) are developed containing repeat units capable of persistent (covalent) NP interactions that enable the direct fabrication of nanoscale porous heterostructures, where a single material is localized at the pore surface as a continuous layer. This SDA binding motif (design rule 1) enables sequence-controlled heterostructures, where the composition profile and interfaces correspond to the synthetic addition order. This approach is generalized with 5 material sequences using an SDA with only persistent SDA-NP interactions ("P-NP1-NP2"; NPi = TiO2, Nb2O5, ZrO2). Expanding these polymer SDA design guidelines, it is shown that the combination of both persistent and dynamic (noncovalent) SDA-NP interactions ("PD-NP1-NP2") improves the production of uniform interconnected porosity (design rule 2). The resulting competitive binding between two segments of the SDA (P- vs D-) requires additional time for the first NP type (NP1) to reach and covalently attach to the SDA (design rule 3). The combination of these three design rules enables the direct self-assembly of heterostructures that localize a single material at the pore surface while preserving continuous porosity.

Surface reconstructed layer with bulk high-valence Mo doping to achieve long-life LiMn2O4 cathode material

Mo doping plays a striking role in the stability enhancement of LiMn2O4 cathode materials. However, the underlying microscopic mechanism is still unclear. Here, we elucidate that the relationship between the atomic position of Mo doping in LiMn2O4 and the stability enhancement of Mo-doped LiMn2O4 by utilizing the spherical aberration-corrected scanning transmission electron microscopy (Cs-STEM). It exhibits that the part of Mo6+ ions occupy empty Mn 16c site to form a surface reconstructed layer of rock-salt like phase on the outermost surface and other Mo6+ ions dope into the Mn octahedral 16d sites to form LiMoxMn2-xO4 in bulk, which is beneficial for inhibiting the parasitic side reactions. Concomitantly, this dual modification of bulk structure and surface can significantly enhance electrode reversibility and Li+ diffusion. As a result, excellent long cycling stability of the as-designed optimal LiMo0.01Mn1.99O4 after 1500 cycles with 61.61 % capacity retention at 10 C (1 C = 148 mAh g−1) is presented, with an initial discharge capacity of 88.30 mAh g−1. Our research provides a clever approach for regulating the surface structure/bulk architecture in LiMn2O4 cathode materials.