Cathode Formation Research Articles

From Bulk to Nanosheet: How Tellurene Can Influence the Performance of Li‐S Batteries on Both Electrodes

AbstractIn the face of growing environmental challenges and the need for alternative energy storage, lithium‐sulfur (Li‐S) batteries stand out for their high theoretical energy density and sulfur's eco‐friendliness. However, the practical application of Li‐S batteries faces significant obstacles, particularly at the cathode and anode. This study explores the transformative impact of 2D tellurene, focusing on how its dimensional variations influence Li‐S battery performance. At the cathode, tellurene not only improves the conductivity and sulfur utilization but also accelerates the conversion of lithium polysulfides (LiPSs). Its reduced size, compared to the bulk counterpart, offers numerous active sites for efficient Li‐ion migration and promotes LiPSs decomposition. At the anode, the protective polytellurosulfides are formed, thereby establishing a stable solid‐electrolyte interphase (SEI) and enhancing reversible lithium deposition. Diminishing the dimensions of tellurene improves its catalytic interface, leading to faster polysulfide conversion kinetics at the cathode and robust SEI formation at the anode. Li‐S batteries equipped with ultra‐thin tellurene‐modified separators demonstrate exceptional performance, exhibiting high areal capacity and significantly reduced capacity decay. Computational simulations further validate the advantages of optimizing tellurene dimensions, confirming its essential role in LiPSs decomposition and overall battery efficiency.

Electrode interface modulation using 1,3-propane sultone functionalized additives for high-performance Zn-MnO2 aqueous batteries

Rechargeable aqueous zinc-manganese dioxide (Zn-MnO2) batteries have gained significant attention in the field of energy storage systems owing to their cost-effectiveness, environmental friendliness, power, and ability to mitigate thermal propagation. However, Zn- MnO2 batteries encounter challenges and limitations, including capacity degradation and voltage hysteresis by the dissolution of Mn ions in the bulk electrolyte. In this study, interfacial stabilization is improved by promoting the decomposition of the 1,3-propane sultone (PS) electrolyte additive, which occurs close to the oxidation decomposition at 1.5 V. This facilitates the formation of a stable cathode–electrolyte interphase (CEI) and effectively suppresses Mn-ion dissolution. Density functional theory (DFT) simulations provide insights into the formation of a CEI layer product structure during cell operation, resulting in the thermodynamically reduced dissolution of Mn (Mn2+) into the electrolyte when a sulfur-based decomposed layer covers MnO2. Consequently, the cathode protection layer ensures high cycle retention, Coulombic efficiency, and high C-rate cell operating conditions for the Zn-MnO2 battery cell. This work presents a promising strategy for designing electrolytes to develop high-performance aqueous zinc-ion batteries.

Critical current in a two-dimensional non-magnetically insulated crossed-field gap with monoenergetic emission

Prior studies have developed theories for the maximum permissible current, or critical current, for one-dimensional planar and cylindrical crossed-field diodes where the magnetic field is below the Hull cutoff, meaning that an electron emitted from the cathode reaches the anode. Here, we develop semi-empirical and analytical models to predict the critical current for a two-dimensional (2D) planar diode with nonzero monoenergetic initial velocity. The semi-empirical method considers the geometry, nonzero initial velocity, and magnetic field as multiplicative corrections to the Child–Langmuir law for space-charge limited current in a one-dimensional planar diode with an initial velocity of zero. These results agree well with 2D particle-in-cell (PIC) simulations using the over-injection method to assess virtual cathode formation for different emission widths, magnetic field strengths, and initial velocities. The analytical solution agrees better with PIC results because it accounts for the coupling of the magnetic field, geometry, and initial velocity that the semi-empirical approach does not.

Towards rapid formation of electroactive biofilm: insights from thermodynamics and electric field manipulation

Electroactive biofilm (EAB) has garnered significant attention due to its effectiveness in pollutant remediation, electricity generation, and chemical synthesis. However, achieving precise control over the rapid formation of EAB presents challenges for the practical implementation of bioelectrochemical technology. In this study, we investigated the regulation of EAB formation by manipulating applied electric potential. We developed a modified XDLVO model for the applied electric field and quantitatively assessed the feasibility of existing rapid formation strategies for EAB. Our results revealed that electrostatic (EL) force significantly influenced EAB formation in the presence of the applied electric field, with the potential difference between the electrode and the microbial solution being the primary determinant of EL force. Compared to -0.2 V and 0 V vs.Ag/AgCl, EAB exhibited the highest electrochemical performance at 0.2 V vs.Ag/AgCl, with a maximum current density of 6.044 ± 0.10 A/m2, surpassing that at -0.2 V vs.Ag/AgCl and 0 V vs.Ag/AgCl by 1.73 times and 1.31 times, respectively. Furthermore, EAB demonstrated the highest biomass accumulation, measuring a thickness of 25 ± 2 μm at 0.2 V vs. Ag/AgCl, representing increases of 1.67 and 1.25 times compared to -0.2 V vs.Ag/AgCl and 0 V vs.Ag/AgCl, respectively. The strong electrostatic attraction under the anodic potential promoted the formation of a monolayer of biofilm. Additionally, the hydrophilicity and hydrophobicity of the biofilm were altered following inversion culture. The Lewis acid-base (AB) attraction offset the electrostatic repulsion caused by negative charges, it is beneficial for the formation of biofilms. This study, for the first time, elucidated the difference in the formation of cathode and anode biofilm from a thermodynamic perspective in the context of electric field introduction, laying the theoretical foundation for the directional regulation of the rapid formation of typical electroactive biofilms.

Exploring the impact of synergistic dual-additive electrolytes on 5 V-class LiNi0·5Mn1·5O4 cathodes

Tris (trimethylsilyl) phosphate (TMSP) and tris(2,2,2-trifluoroethyl) phosphate (TTFP) was added to carbonate solvent-based electrolytes as dual-additives to enhance the performance of LiNi0·5Mn1·5O4 (LNMO). The X-ray photoelectron spectroscopy results revealed that both TMSP with high oxidation ability and TTFP with high oxidation resistance participated in the formation of cathode–electrolyte interphase (CEI) films. Electrochemical impedance spectroscopy confirmed that the constructed CEI films had excellent electronic insulation and ionic conductivity, reducing the interfacial impedance of the LNMO electrode, and improving the electrochemical performance of LNMO/Li half-cells and LNMO/Li4Ti5O12 full-cells. As measured by the nuclear magnetic resonance, the incorporation of TMSP and TTFP significantly reduced the HF content in the electrolytes. Therefore, both LNMO/Li half-cells (500 cycles with 95.7% capacity retention) and LNMO/Li4Ti5O12 full-cells (200 cycles with 79.9% capacity retention) displayed higher cycling stabilities at 5 C owing to the synergistic effect of TMSP and TTFP. In comparison, capacity retentions of ∼76.5% after 500 cycles and ∼37.2% after 200 cycles were respectively achieved for the LNMO/Li half-cells and LNMO/Li4Ti5O12 full-cells with the standard electrolyte at 5 C. This study provides strong evidence that additive combinations can improve the electrochemical performance of high-energy and high-voltage cathode materials.

A Tutorial on the One-Dimensional Theory of Electron-Beam Space-Charge Effect and Steady-State Virtual Cathode

The space-charge effects of pulsed high-current electron beams are very important to high-power particle beam accelerators and high-power microwave devices. The related physical phenomena have been studied for decades, and a large number of informative publications can be found in numerous scientific journals over many years. This review article is aimed at systematically summarizing most of the previous findings in a logical manner. Using a normalized one-dimensional mathematical model, analytical solutions have been obtained for the space-charge-limited current of both planar diode and drifting space. In addition, in the case of a beam current higher than the space-charge-limited current, the virtual cathode behavior and beam current reflection are quantitively studied. Furthermore, the criteria of steady-state virtual cathode formation are investigated, which leads to the physical understanding of the unstable nature of the virtual cathode. This review article is expected to serve as an integrated source of related information for young researchers and students working on high-power microwaves and pulsed particle beams.

Porous Carbon Textile Decorated with VC/V2O3-X Hybrid Nanoparticles: Dual-Functional Host for Flexible Li-S Full Batteries

The polysulfide shuttling at the cathode and lithium dendrite formation at the anode remain as major obstacles to overcome for the realization of high-performance lithium-sulfur (Li-S) batteries. Here, via a facile one-pot synthesis using carbothermic reduction, we prepared a porous and flexible carbon textile uniformly decorated with VC/V2O3-x hybrid nanoparticles, which was used as a robust and flexible host material for both sulfur cathode and Li metal anode. We observed that the defective V2O3-x part traps polysulfides and the conductive VC part catalytically enhances the fragmentation of the polysulfides. Moreover, it was found that the well-distributed VC/V2O3-x nanoparticles act as lithiophilic sites to lead uniform lithium nucleation for a dendrite-free lithium metal anode. The full battery delivered superb rate performance (882 mAh g − 1 at 5 C) and an ultralow decay rate of 0.02% per cycle during 1000 cycles at 1 C. Even with a large sulfur loading of 7.0 mg cm−2, a high areal capacity of 6.29 mAh cm−2 at 0.2 C was obtained. This work provides an effective remedy to simultaneously resolve problems regarding the shuttle effect and the Li dendrite formation for the realization of high-performance flexible Li-S full batteries.

INFLUENCE OF THE METHOD OF FORMING A Pr2CuO4-BASED CATHODE ON THE ELECTROCHEMICAL CHARACTERISTICS OF A PLANAR ELECTROLYTE-SUPPORTED SOFC

The influence of the method of organising the cathode microstructure based on Pr2CuO4 (PCO) on the electrochemical characteristics of a model electrolyte-supported solid oxide fuel cell (SOFC) has been investigated. It is shown that an increase in the thickness of the PCO cathode layer and the introduction of a pore-forming agent contribute to an increase in the power density of the SOFC test cell compared to a sample with an initial unmodified cathode structure, whose power density at 850°C was 34 mW/cm2. It was found that the optimum thickness of the cathode layer to achieve maximum electrochemical performance was in the range of 40-50 μm, while the power density achieved was 116 mW/cm2 at 850°C. At the same time, the transition from a single-phase PCO cathode to a composite of PCO-Ce0.9Gd0.1O1.95 (60/40 wt. %) provides an increase in power density up to 130 mW/cm2 at 850°C, while the dynamics of its decrease with reducing temperature is slower compared to the single-phase cathode. The analysis of the changes in the values of the total electrode polarisation resistance of the model SOFC, determined by impedance spectroscopy, as a function of the method of cathode formation, showed that during the transition from the initial sample to the samples with increased thickness of the cathode layer and the composite cathode, a twofold (in the first case) and threefold (in the second case) decrease in the level of polarisation losses is observed, which correlates with an increase in the power density. The proposed methods of modifying the initial cathode microstructure based on PCO show a positive dynamic of increasing the electrochemical activity of the cathode/electrolyte interface and the power density characteristics of the fuel cell as a whole.

Bifunctional self-assembled molecular layer enables stable Ni-rich cathodes

Ni-rich layered oxides (LiNixCoyMnzO2, x ≥ 0.8, x + y + z = 1) are attractive cathode material candidates for building high-energy-density batteries owing to their higher specific capacity compared to their lower-Ni-content analogues. However, the high nickel content also brings challenges, such as storage instability in ambient conditions and poor cycle life. In this work, we propose a surface chemistry regulation strategy to simultaneously enhance the air storage stability and electrochemical stability of high-nickel cathode materials. A bifunctional ultrathin layer composed of trimethoxy(1H,1H,2H,2H-perfluorodecyl)silane (PFDTMS) was constructed on the surface of single-crystal LiNi0.83Co0.12Mn0.05O2 (NMC811) particles via molecular self-assembly. The passivating PFDTMS layer forms a superhydrophobic surface on the modified NMC811 particles, effectively mitigating deactivation reactions of NMC811 in air, and ensuring an uncompromised electrochemical performance of NMC811-based electrode after storing in air for two weeks. Furthermore, the self-assembled PFDTMS layer contributes to the formation of an electrochemical stable cathode–electrolyte interphase (CEI) on the NMC811 surface, improving the cycling stability of NMC811 at high cut-off voltages. The PFDTMS-based CEI also alleviates the chemical corrosion of NMC811 by the electrolyte, slows down the dissolution of transition metal ions during long term cycling. These findings present a straightforward, effective, eco-friendly, and cost-efficient approach to tackle the stability challenges inherent to Ni-rich layered cathode materials.

In situ formed partially disordered phases as earth-abundant Mn-rich cathode materials

AbstractEarth-abundant cathode materials are urgently needed to enable scaling of the Li-ion industry to multiply terawatt hours of annual production, necessitating reconsideration of how good cathode materials can be obtained. Irreversible transition metal migration and phase transformations in Li-ion cathodes are typically believed to be detrimental because they may trigger voltage hysteresis, poor kinetics and capacity degradation. Here we challenge this conventional consensus by reporting an unusual phase transformation from disordered Li- and Mn-rich rock salts to a new phase (named δ), which displays partial spinel-like ordering with short coherence length and exhibits high energy density and rate capability. Unlike other Mn-based cathodes, the δ phase exhibits almost no voltage fade upon cycling. We identify the driving force and kinetics of this in situ cathode formation and establish design guidelines for Li- and Mn-rich compositions that combine high energy density, high rate capability and good cyclability, thereby enabling Mn-based energy storage.

Fast Lithium Intercalation Mechanism on Surface‐Modified Cathodes for Lithium‐Ion Batteries

AbstractEnhancing the understanding of fast lithium intercalation on cathode surfaces modified by oxides is crucial for the development of electrode materials that offer high‐power and long‐life operation. Herein, lithium transfer is elucidated by directly observing the structural changes within the cathode, through the interface, and into the electrolyte using in situ neutron reflectometry (NR). Two films are studied—a Li2ZrO3‐modified and an unmodified LiCoO2 film—and it is found that the modified film exhibits a superior rate capability. In situ NR studies indicate that the surface modification facilitates the formation of a dense cathode–electrolyte interphase (CEI), primarily composed of inorganic species. In contrast, the unmodified surface is covered by a relatively sparse and electrolyte‐impregnated CEI. These structural observations suggest that lithium desolvation during intercalation primarily occurs on the CEI and LiCoO2 surfaces for the modified and unmodified films, respectively. Fast desolvation of lithium on the CEI may contribute to the superior rate capability of the surface‐modified cathodes. This suggests a mechanism of fast intercalation achieved by surface modification of low ionically conductive oxides. Simultaneous chemical composition and morphological information is a powerful way to elucidate the dynamics at cathode/liquid electrolyte interfaces suitable for high‐power operation.

Uniform space-charge-limited current for a two-dimensional planar emitter with nonzero monoenergetic initial velocity

While characterizing space-charge-limited current (SCLC) is important for numerous applications, no analytical solutions for SCLC with monoenergetic initial velocity exist for two-dimensional (2D) geometries. Here, we derive approximate closed-form solutions for uniform SCLC with monoenergetic emission of electrons in a 2D planar diode, where emission is restricted to a long patch of width W for electrodes separated by a distance D. We also derive a semiempirical approach for estimating the SCLC for these cases by treating the geometric and velocity correction factors as multiplicative corrections to the SCLC for a one-dimensional vacuum diode given by the Child–Langmuir (CL) law. We show that the SCLC for a finite patch with nonzero velocity can exceed the CL law by three orders of magnitude. The theoretically calculated SCLCs for various emission widths and initial velocities in the 2D diode agree well with particle-in-cell simulations using the over-injection method in XOOPIC; they agree with the semiempirical relationship for lower initial velocities. In the limit of high initial velocity, the geometry and velocity corrections to the CL law cannot be decoupled, invalidating the assumption of the semiempirical approach and causing it to diverge from the theoretical solution and XOOPIC simulations. These results provide valuable estimates for determining the onset of virtual cathode formation for photocathodes and thermionic cathodes, which operate in the over-injection regime to avoid beam quality degradation.

Nonuniform electron distributions in a solenoidal ioniser

Solenoidal ionisers are a new class of highly efficient helium detectors that are increasingly important for high resolution atom scattering, molecular scattering and scanning helium microscopy. They operate via electron ionisation, where the electrons are trapped by the magnetic field of a solenoid and additional electrostatic potentials. Their ionisation efficiency scales with the electron population they contain, motivating large devices with high emission currents. However, these detectors typically become unstable at high electron densities, constraining their performance improvement. Through imaging the electron population at the exit of the ioniser, we demonstrate that these instabilities arise from non-uniformities in the electron distribution. Considering the ioniser as a non-neutral plasma leads to the proposal of the formation of a virtual cathode and a plasma instability as the origins of the non-uniformity.

An analytical model for anchor-mortar interface bonding based on electrochemical impedance spectroscopy

Corrosion can lead to deterioration of the bonding properties at anchor-mortar interfaces, affecting the durability of the anchored structures. Therefore, it is essential to establish an accurate analytical model of the anchor-mortar interface bond to estimate the interface bond strength under corrosion. Steel corrosion occurs via electrochemical reactions, that is, anode and cathode formation in different potential zones on the steel surface, resulting in an electrical potential difference that facilitates constant cation migration and the generation of corrosion products with anions. In this study, electrochemical impedance spectroscopy, taking into account electrochemical theory, was carried out to analyse the kinetics of the electrode processes. Based on electrochemical parameters such as pore solution resistance and charge transfer resistance, a function relating electrochemical parameters to the material properties was established. The traditional theoretical model of a thick-walled cylinder was modified to obtain an analytical model of the bond strength of the anchor-mortar interface in pull-out damage mode under the effect of corrosion. The accuracy of the estimated values of the analytical model was verified via pull-out test results. The estimated values obtained from the analytical model were in good agreement with the test values, indicating that the model was able to describe the corrosion state at the anchor-mortar interface and estimate the interfacial bond without damaging the specimen.

Controlled crystal growth and electrode formation of single crystalline Li(Ni,Mn)2O4 spinel cathodes

To promote the practical application of single crystalline (SC) cathode materials, it is essential tailoring the electrochemically active crystal phase with specific surface growth favored to the Li+ transport. Additionally, the electrode formation should be adjusted accordingly for the corresponding polygonal shape SC particles, which significantly affects the overall physical/electrochemical properties for the given cathode materials. Herein, we present optimal crystal synthesis and cathode formation for the spinel LiNi0.5Mn1.5O4 SC particles and evaluate the electrochemical performances. The resultant particles are uniform octahedral shape with the (111) and (100) planes preserving stable surface conditions grown in Li2MoO4 flux. We can also realize the porosity-controlled cathode formation using the corresponding SC particles is important in alleviating the severe capacity fade under high voltage and current densities, which was confirmed by the degree of lithiation and delithiation during the cycle reactions in conjunction with the spectroscopy analysis such as Laser Induced Breakdown Spectroscopy.

More than Just a Binder: Versatile Block Copolymer Enhances the Electrochemical Performance of a Nickel-Rich Cathode

Nickel-rich layered cathodes (for example, NCM811) hold great promise for practical applications in high-energy density lithium-ion battery technology. However, a nickel-rich cathode has poor cyclic stability because of the structure degradation induced by repeated cycles and excessive formation of thick cathode–electrolyte interface (CEI) layers. Poly(vinylidene difluoride) (PVDF) is a typical binder used to form a positive electrode, which nevertheless lacks the functionality to suppress structure degradation and control CEI layer formation. A new concept is proposed in this work to use a multi-functional block copolymer of poly(ether imide)-block-poly(dimethyl siloxane) (PEI-b-PDMS; abbreviated as PEMS) as the binder for the nickel-rich cathode. Unlike the conventional PVDF binder, the PEMS binder is capable of inhibiting crack formation within the NCM811 particles to retard structure degradation over cycles because of its elastomeric feature. The PEMS binder also enables tuning the composition of the CEI layer and inhibits the formation of overly thick CEI layers because the carbonate solvent molecules are excluded from the solvation sheath by the PEMS binder. Enhanced electrolyte affinity is exhibited by the electrode with the PEMS binder as evidenced by the contact angle measurement. Improved carbon black dispersion within the electrode is achieved by the PEMS binder because the PEI aromatic chain has strong affinity toward the carbon black particles. Both the cycling and rate performance of the NCM811 cathode is improved with the PEMS binder compared to the PVDF binder. In detail, the capacity retention is increased from 63.9 to 80.6% after 200 cycles at 0.5 C (1 C = 205 mAh g–1) when the PVDF binder is replaced by the PEMS binder. The rate performance at current densities of 2 and 5 C is increased significantly due to enhanced electrochemical kinetics.

Analysis of the virtual cathode and floating potential of a thermionic emissive probe operating in the space-charge-limited regime

This paper analyses by this and characterizes a thermionic emissive probe operating in both the temperature-limited current regime (T-region) and the space-charge-limited current regime (S-region) characterized by the formation of a virtual cathode. For this last case, we obtain the potential profile, the emitted current that overcomes the virtual cathode, as well as the thickness and depth of the potential well in front of the probe for different probe temperatures, plasma electron temperatures and neutral gas pressures. From these results, we obtain the I–V curves and the floating potential. Depending on the probe radius, when the floating potential is reached in the S-region, its value saturates, becoming almost independent of the probe temperature and the electron temperature.

Dual Role of Bis(borate) Additive in Electrode/Electrolyte Interface Layer Construction for High-Voltage NCM 523 Cathode

Increasing the working voltage of a layered oxide cathode is an efficient way to lift the energy density of lithium-ion batteries. However, uncontrollable side reactions and excessive electrolyte decomposition take place at high voltage. Bulk cathode structure degradation and formation of a high working voltage induce excessive growth of the solid-electrolyte interface (SEI) layer and overconsumption of the electrolyte. Construction of a high-voltage stable SEI layer is crucial to enhance the electrochemical performance. In this work, trimethylene borate (TMEB) as a borate ester additive is used to improve the cycled stability of NCM523 cells at 4.5 V charging-cutoff voltage. On one hand, TMEB can be preferentially decomposed during cycling and participate in the film formation process on the surfaces of both anode and cathode. On the other hand, TMEB can tune the solvation sheath by expelling the carbonate solvent molecules out of the solvation sheath to suppress decomposition of the electrolyte. The cells cycled with the 0.5 wt % TMEB-containing electrolyte exhibit improved cycling stability after 200 cycles with the capacity retention of 90.9% indicating TMEB to be an effective additive to improve the lithium-ion batteries at higher charging-cutoff voltage.

Effect of q-Nonextensively Distributed Plasma Electrons on Double Sheath Characteristics and Virtual Cathode Formation Associated With Electron Emitting Surfaces

A double sheath characteristics and virtual cathode formation in a plasma containing <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$q$</tex-math> </inline-formula> -nonextensive distributed electrons, thermally emitted or secondary emitted electrons from the cathode wall, and ions are studied numerically. The distribution of primary (plasma) electrons is taken to be nonextensive, as per Tsallis statistics. The electric field at the cathode, the ratio of ion to electron current density and the velocity of ions are evaluated and the results are compared with the case of electrons having Boltzmann distribution. The variation of the electric potential, space charge density, and sheath thickness are analyzed for the cases of different nonextensivity <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$q$</tex-math> </inline-formula> . The electric field at the cathode becomes zero at a lower value of electron beam current density, and hence the formation of the virtual cathode takes place earlier for the case of super-extensive distributed electrons as compared to that of the Boltzmann-distributed electrons. For super extensively distributed electrons, the electric potential drops slowly to a minimum, the velocity of positive ions increases inside the sheath, and an increase in the sheath thickness is observed.

Enhancement of Light Extraction Efficiency and Suppression of Roll‐Off Characteristics of Thermally Activated Delayed Fluorescence Organic Light‐Emitting Diodes by Inserting Nanoscale Pixel‐Defining Layer

AbstractThermally activated delayed fluorescence (TADF) organic molecules are considered the most suitable for blue organic light‐emitting diodes (OLEDs) after extensive research; however, they are plagued by issues of internally guided light and the roll‐off characteristics contributed by triplet exciton‐utilized emission. Thus, this study leverages exciton diffusion guidance and energy extraction to simultaneously achieve optical efficiency enhancement and roll‐off characteristic suppression of mixed‐host blue TADF OLEDs. The array of nanopixels, defined by the inserted nanoscale pixel‐defining layer (nPDL), spatially separates the excitons and polarons, resulting in the exacerbation of triplet quenching by securing exciton diffusion. Furthermore, through the formation of a metal cathode with a corrugated profile, nonradiative energy transfer to the surface plasmon polaritons is capitalized via Bragg diffraction, thereby boosting the emission efficiency. The structure of the nPDL is judiciously determined by finite‐difference time‐domain computational analysis. Consequently, the device with the optimized nPDL demonstrates 88.4%, 118.8%, and 108.8% improvements in external quantum, current, and power efficiencies, respectively, compared to the reference. Moreover, the critical luminance, which quantifies the degree of roll‐off, is improved by 83.7%. This pioneering demonstration of hybridizing the material combination and nanopatterning techniques is expected to provide new insights for designing high‐performance OLEDs.