Li-ion Diffusion Coefficient Research Articles

Construction of superior performance LiVPO4F/C cathode assisting by a regulating additive NH4F and the “Combination-Protection-Release” mechanism for lithium ion batteries

The commercialization of LiVPO4F/C cathode for lithium ion batteries is hindered by its low electrical conductivity and the presence of Li3V2(PO4)3 impurity. In this work, pure LiVPO4F/C with superior electrochemical performance is successfully prepared by adding regulating additive NH4F in one-step rapid reduction method. N-doped LiVPO4F/C without Li3V2(PO4)3 is synthesized by adding 0.025 mol NH4F, which possesses high electrical conductivity (0.896 S cm−1) and large Li-ion diffusion coefficient (3.65 × 10−10 cm2 s−1). It presents superior capacity of 144.8, 127.5 and 112.7 mAh g−1 at 1, 5 and 15 C and high capacity retention of 85.13% after 300 cycles at 1 C and excellent long term performance after 1000 cycles at 8 C. The in-situ X-ray diffraction analysis reveals the transformation process of the crystal structure of LiVPO4F. The added NH4F can effectively improve the electrochemical performance by adjusting the negative logarithm of the effective hydrogen-ion concentration to refine the grain and serve as nitrogen-doping source, leading to increased Li-ion diffusion coefficient and electrical conductivity. The precipitate LiHF2 is formed after the addition of NH4F, which can suppress the volatilization of fluorine and supplement its loss in the precursor. The “Combination-Protection-Release” mechanism has been proposed to explain the preparation of LiVPO4F/C without impurity Li3V2(PO4)3.

Identifying the positive role of lithium hydride in stabilizing Li metal anodes.

Lithium hydride has been widely identified as the major component of the solid-electrolyte interphase of Li metal batteries (LMBs), but is often regarded as being detrimental to the stabilization of LMBs. Here, we identify the positive and important role of LiH in promoting fast diffusion of Li ions by building a unique three-dimensional (3D) Li metal anode composed of LiMg alloys uniformly confined into graphene-supported LiH nanoparticles. The built-in electric field at the interface between LiH with high Li ion conductivity and LiMg alloys effectively boosts Li diffusion kinetics toward favorable Li plating into lithiophilic LiMg alloys through the surface of LiH. Therefore, the diffusion coefficient of Li ions of the thus-formed 3D structured Li metal anode is 10 times higher than the identical anode without the presence of LiH, and it exhibits a long cycle life of over 1200 hours at 3 mA cm−2 under 5 mA hour cm−2.

Oxygen vacancy-expedited ion diffusivity in transition-metal oxides for high-performance lithium-ion batteries

Rapid capacity decay and inferior kinetics are the vital issues of anodes in the conversion reaction for lithium-ion batteries. Vacancy engineering can efficiently modulate the intrinsic properties of transition-metal oxide (TMO)-based electrode materials, but the effect of oxygen vacancies on electrode performance remains unclear. Herein, abundant oxygen vacancies are in situ introduced into the lattice of different TMOs (e.g., Co3O4, Fe2O3, and NiO) via a facile hydrothermal treatment combined with calcination. Taking Co3O4 as a typical example, results prove that the oxygen vacancies in Co3O4−x effectively accelerate charge transfer at the interface and significantly increase electrical conductivity and pseudocapacitance contribution. The Li-ion diffusion coefficient of Co3O4−x is remarkably improved by two orders of magnitude compared with that of Co3O4. Theoretical calculations reveal that Co3O4−x has a lower Li-insertion energy barrier and more density of states around the Fermi level than Co3O4, which is favorable for ion and electron transport. Therefore, TMOs with rich vacancies exhibit superior cycling performance and enhanced rate capability over their counterparts. This strategy regulating the reaction kinetics would provide inspiration for designing other TMO-based electrodes for energy applications.

Inducing lattice defects in calcium ferrite anode materials for improved electrochemical performance in lithium-ion batteries

Enhancing the electrical conductivity of electrode materials via a cationic substitution strategy was recognized as an effective way of improving the electrochemical performance of Li-ion batteries. Thus, LixCa1-xFe2O4 nanoparticles were synthesized via a facile inexpensive process at low temperature. XRD peaks refer to the formation of an orthorhombic structure with the Pnma space group. HR-TEM investigations reveal orthorhombic-like shape for pure CaFe2O4, nanoplatelet-like morphology for Li0.05Ca0.95Fe2O4 and irregular distorted crystals for Li0.1Ca0.9Fe2O4. Voids and pores in Li-doped CaFe2O4 were confirmed by FESEM and BET measurements. XPS spectra of O1s prove that Li-doped CaFe2O4 have higher conductivity due to the created lattice defects and oxygen species. Li-doped CaFe2O4 anodes exhibit great improvement in their initial discharge capacities ∼1219 and 1606 mAhg−1 upon substitution of Ca with 5% and 10% Li, respectively. Furthermore, 10% Li-doped CaFe2O4 anode displays the highest Li-ions diffusion coefficient and exchange current density due to the enhanced Li+ ions mobility. Moreover, the DC activation energies for the LixCa1-xFe2O4 nanoparticles decreased with increasing Li content.

Constructing zigzag-like hollow mesoporous nanospheres MoO2/C with superior lithium storage performance

Hollow mesoporous nanospheres MoO2/C are successfully constructed through metal chelating reaction between molybdenum acetylacetone and glycerol as well as the Kirkendall effect induced by diammonium hydrogen phosphate. MoO2 nanoparticles coupled by amorphous carbon are assembled to unique zigzag-like hollow mesoporous nanosphere with large specific surface area of 147.7 m2 g−1 and main pore size of 8.7 nm. The content of carbon is 9.1%. As anode material for lithium-ion batteries, the composite shows high specific capacity and excellent cycling performance. At 0.2 A g−1, average discharge capacity stabilizes at 1092 mAh g−1. At 1 A g−1 after 700 cycles, the discharge capacity still reaches 512 mAh g−1. Impressively, the composite preserves intact after 700 cycles. Even at 5 A g−1, the discharge capacity can reach 321 mAh g−1, exhibiting superior rate capability. Various kinetics analyses demonstrate that in electrochemical reaction, the proportion of the surface capacitive effect is higher, and the composite has relatively high diffusion coefficient of Li ions and fast faradic reaction kinetics. Excellent lithium storge performance is attributed to the synergistic effect of zigzag-like hollow mesoporous nanosphere and amorphous carbon, which improves reaction kinetics, structure stability and electronic conductivity of MoO2. The present work provides a new useful structure design strategy for advanced energy storage application of MoO2.

Facile synthesis of carbon and oxygen vacancy co-modified TiNb6O17 as an anode material for lithium-ion batteries.

Titanium niobium oxides (TNOs), benefitting from their large specific capacity and Wadsley–Roth shear structure, are competitive anode materials for high-energy density and high-rate lithium-ion batteries. Herein, carbon and oxygen vacancy co-modified TiNb6O17 (A-TNO) was synthesized through a facile sol–gel reaction with subsequent heat treatment and ball-milling. Characterizations indicated that A-TNO is composed of nanosized primary particles, and the carbon content is about 0.7 wt%. The nanoparticles increase the contact area of the electrode and electrolyte and shorten the lithium-ion diffusion distance. The carbon and oxygen vacancies decrease the charge transfer resistance and enhance the Li-ion diffusion coefficient of the obtained anode material. As a result of these advantages, A-TNO exhibits excellent rate performance (208 and 177 mA h g−1 at 10C and 20C, respectively). This work reveals that A-TNO possesses good electrochemical performance and has a facile preparation process, thus A-TNO is believed to be a potential anode material for large-scale applications.

Three-dimensional flexible molybdenum oxynitride thin film as a high capacity anode for Li-ion batteries

With the fast development of flexible wearable electronics, mobile electronic equipment, electric tool and electric vehicles, high specific capacity, superior cycle stability and excellent fast-charge performance are required for lithium-ion batteries (LIBs). Nevertheless, commercial graphite with the limited theoretical capacity (372 mAh g−1) and short lifespan is difficult to satisfy the requirements of the new generation of LIBs. In this work, the three-dimensional flexible molybdenum oxynitride (MNO) thin films with non-binder were prepared by magnetron sputtering approach. The charge transfer resistance and Li-ion diffusion coefficient were measured by electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV), and the results show that molybdenum nitride is helpful to increase the diffusion and electron transfer of Li-ion. The MNO thin film annealed at 300 °C with irregular aggregate matrix structure shows a discharge capacity of 413 mAh g−1 after 180 cycles at 1 A g−1. The outstanding rate performance and cycle stability suggest that these binder-free thin film electrodes, especially nitrides, offer great opportunity for energy storage systems with fast-charge capabilities.

Sputtering Coating of Lithium Fluoride Film on Lithium Cobalt Oxide Electrodes for Reducing the Polarization of Lithium-Ion Batteries.

Lithium cobalt oxide (LCO) is the most widely used cathode materials in electronic devices due to the high working potential and dense tap density, but the performance is limited by the unstable interfaces at high potential. Herein, LiF thin film is sputtered on the surface of LCO electrodes for enhancing the electrochemical performance and reducing the voltage polarization. The polarization components are discussed and quantified by analyzing the relationship between electrochemical polarization and charger transfer resistance, as well as that between concentration polarization and Li-ion diffusion coefficients. In addition, the decreased charge transfer resistance, increased lithium-ion diffusion coefficients, and stabilized crystal structure of LiF-coated LCO are confirmed by various electrochemical tests and in-situ XRD experiments. Compared to that of pristine LCO, the capacity and cycling performance of LiF-coated LCO is improved, and the overpotential is reduced upon cycling. This work provides reference for quantifying the various polarization components, and the strategy of coating LiF film could be applied in developing other analogous cathode materials.

A new boundary condition forging the unprecedented self-consistence of galvanostatic intermittent titration technique

Galvanostatic Intermittent Titration Technique (GITT) is widely applied to undertake the measurement of Li ion diffusion coefficient D in solid phase of electrode materials. However, various parameters adopted in GITT lead to considerable gaps of values of D in previous researches, making the measurement less rigorous. This work tries to introduce an indicator, the first derivative of ∆Eτ (or Eτ) vs t, to sift out the start of time region for the quasi-steady state. Further, by the introduction of a new boundary condition in GITT model, an enabler based on the slope ratio of ∂E/∂t at various titration currents is developed to reveal a more appropriate time region, realizing the high self-consistence of results calculated from GITT with different parameters. Particularly, the time region for Li+ diffusion in solid phase optimized from the enabler is even several orders of magnitude later than time constants derived from equivalent circuits. Based on the optimization of time region, the calculation of D via GITT achieves an unprecedented self-consistence within different titration currents over the un-optimized one. Such optimization may set a standard for calculate ion of Li+ diffusion in electrode materials.

Effects of long-term fast charging on a layered cathode for lithium-ion batteries

Fast charging, which aims to shorten recharge times to 10–15 min, is crucial for electric vehicles (EVs), but battery capacity usually decays rapidly if batteries are charged under such severe conditions. Revealing the failure mechanism is a prerequisite to improving the charging performance of lithium (Li)-ion batteries. Previous studies have focused less on cathode materials while also mostly focusing on their early changes. Thus, the cumulative effect of long-term fast charging on cathode materials has not been fully studied. Here, we study the changes in a layered cathode material during 1000 cycles of 6C charging based on 1.6 Ah LiCoO2/graphite pouch cells. Postmortem analysis reveals that the surface structure, charge transfer resistance and Li-ion diffusion coefficient of the cathode degenerate during repeated fast charging, causing a large increase in polarization. This polarization-induced poor utilization of the Li inventory is an important reason for the rapid capacity fading of batteries. These findings deepen the understanding of the aging mechanism for cells undergoing fast charging and can be used as benchmarks for the future development of high-capacity, fast-charging layered cathode materials.

Enhancing capacity and transport kinetics of C@TiO2 core–shell composite anode by phase interface engineering

In nanocomposite electrodes, besides the synergistic effect that takes advantage of the merits of each component, phase interfaces between the components would contribute significantly to the overall electrochemical properties. However, the knowledge of such effects is far from being well developed up to now. The present work aims at a mechanistic understanding of the phase interface effect in C@TiO2 core–shell nanocomposite anode which is both scientifically and industrially important. Firstly, amorphous C, anatase TiO2 and C@anatse-TiO2 electrodes are compared. The C@anatase-TiO2 shows an obvious higher specific capacity (316.5 mAh g−1 at a current density of 37 mA g−1 after 100 cycles) and Li-ion diffusion coefficient (4.0 × 10–14 cm2 s−1) than the amorphous C (178 mAh g−1 and 2.9 × 10–15 cm2 s−1) and anatase TiO2 (120 mAh g−1 and 1.6 × 10–15 cm2 s−1) owing to the C/TiO2 phase interface effect. Then, C@anatase/rutile-TiO2 is obtained by a heat treatment of the C@anatase-TiO2. Due to an anatase-to-rutile phase transformation and diffusion of C along the anatase/rutile phase interface, additional abundant C/TiO2 phase interfaces are created. This endows the C@anatase/rutile-TiO2 with further boosted specific capacity (409.4 mAh g−1 at 37 mA g−1 after 100 cycles) and Li-ion diffusion coefficient (3.2 × 10–13 cm2 s−1), and excellent rate capability (368.6 mAh g−1 at 444 mA g−1). These greatly enhanced electrochemical properties explicitly reveal phase interface engineering as a feasible way to boost the electrochemical performance of nanocomposite anodes for Li-ion batteries.

Rapid Determination of the Li-Ion Diffusion Coefficient in Intercalation Electrodes by Intermittent Current Interruption

The galvanostatic intermittent titration technique (GITT) has long been regarded as the go-to method for determining the diffusion coefficient of Li-ions in the intercalation electrode materials at various states of charge (SoC). However, the GITT is a stand-alone technique and notoriously time-consuming. Here, we present an efficient alternative to GITT: the intermittent current interruption (ICI) method. From Fick’s laws, it is demonstrated that the ICI method renders the same information as GITT. Both GITT and ICI are experimentally benchmarked by electrochemical impedance spectroscopy (EIS) in a half-cell of lithium nickel-manganese-cobalt oxide (NMC 811). The results from the three employed methods match each other where the assumption of semi-infinite diffusion applies, thereby demonstrating the applicability of using a more efficient technique to determine the lithium diffusivity. Moreover, the nondisruptive nature and the compatibility with galvanostatic cycling make the ICI method ideal for online diagnoses and operando characterization of Li-ion batteries.Figure: Diffusion coefficient (D) of Li-ions in NMC 811 plotted against the potential (E) in measurements employing GITT and ICI methods. Figure 1

Graphite Anode of Lithium-Ion Batteries for Fast Charging Application

The rapid growth of electric vehicle (EV) market has demanded lithium-ion batteries (LIBs) with fast charging capability. During fast charging application, the anode plays a crucial role in determining the performance of LIBs. In this report, four graphite materials with particle sizes ranged from 5 to 22.4 μm were investigated as anodes of LIBs. The properties of pristine graphite materials, including crystal phase, morphology, particle size and surface area, were evaluated through X-ray diffraction (XRD), scanning electron microscope (SEM) and nitrogen adsorption. Assembled into cells, these graphite materials were evaluated through a fast charging test protocol. The electrochemical measurements demonstrate that the rate capability of LIBs increases when the particle size of graphite anode decreases, and LIBs with 5 mm graphite exhibits the highest capacity retention of 74% at 2C and 65% at 4C, respectively. Further, 80% capacity is retained in 5 mm graphite anode after 120 cycles. Measurements from galvanostatic intermittent titration technique (GITT) reveal that the particle size has negligible effect on Li-ion diffusion coefficient in graphite materials studied in this project. In further, lower resistance were observed at the surface of graphite with smaller particles, although a thicker solid electrolyte interface (SEI) film was formed. Therefore, all these observations suggest that the particle size is a very important parameter that should be considered for graphite anode for fast charging LIBs. Keywords: Graphite, Particle Size, Fast charging, Li-Ion Batteries

Intimately-coordinated carbon nitride-metal sulfide with high π-d conjugation for efficient battery performance

In this investigation, a hybrid of metal sulfide and carbon nitride (CN) is synthesized by in-situ chemical conversion between metallic species and a single precursor of carbon, nitrogen and sulfur elements through a strong π-d conjugation approach. It is observed that the local chemical alteration in the vicinity of N atom in the CN template triggers the formation of a highly π-conjugated CN system and efficient π-d hybridization at heterointerface. This is accelerated by partial substitution of the Fe atom for Mn ions in the MnS phase which significantly enhances the battery performance, delivering 2031 mA h g−1 after 500 cycles with inverse capacity growth. Via systematic in-depth characterizations, it is found that the gradual increase of Li-ion diffusion coefficients and charge transfer kinetics for repeated cycling is ascribed to the highly dispersed and uniform particles that are confined within the CN template through a strong π-d hybridization.

Nitrogen and Oxygen Codoped Carbon Anode Fabricated Facilely from Polyaniline Coated Cellulose Nanocrystals for High-Performance Li-Ion Batteries

A facile approach was developed to fabricate nitrogen/oxygen (N/O) codoped carbon anodes by direct carbonization of cellulose nanocrystal/polyaniline (CNC/PANi) nanocomposites which were prepared by in situ growth of PANi onto CNCs. The carbonized CNC/PANi (c-CNC/PANi) anode delivered a high reversible capacity of 470 mAh g–1 at 200 mA g–1 over 100 cycles, which was almost two times higher than those for c-CNC. Moreover, it presented a better rate performance and higher Li-ion diffusion coefficient than c-CNC and c-PANi anodes. The c-CNC/PANi anode also exhibited a distinguished cycling stability with high Coulombic efficiency around 100% at a high current density of 1000 mA g–1 even after 2000 cycles. The significant improvement in the electrochemical performance should be attributed to the larger specific area and uniform N/O dual heteroatoms codoping which can provide sufficient active sites for Li ions storage and induce superior diffusion kinetics of Li ions. This work provided a facile strategy to fabricate N/O codoping carbon derived from the renewable resource of CNC, and it is expected to be a promising candidate anode material for Li-ion batteries application.

Three-dimensional Li-ion transportation in Li2MnO3-integrated LiNi0.8Co0.1Mn0.1O2

Ni-rich layered cathodes (LiNixCoyMnzO2) have recently drawn much attention due to their high specific capacities. However, the poor rate capability of LiNixCoyMnzO2, which is mainly originated from the two-dimensional diffusion of Li ions in the Li slab and Li+/Ni2+ cation mixing that hinder the Li+ diffusion, has limited their practical application where high power density is needed. Here we integrated Li2MnO3 nanodomains into the layered structure of a typical Ni-rich LiNi0.8Co0.1Mn0.1O2 (NCM811) material, which minimized the Li+/Ni2+ cationic disordering, and more importantly, established grain boundaries within the NCM811 matrix, thus providing a three-dimensional diffusion channel for Li ions. Accordingly, an average Li-ion diffusion coefficient (DLi+) of the Li2MnO3-integrated LiNi0.8Co0.1Mn0.1O2 (NCM811-I) during charge/discharge was calculated to be approximately 6*10−10 cm2 S−1, two times of that in the bare NCM811 (3*10−10 cm2 S−1). The capacity delivered by the NCM811-I (154.5 mAh g−1) was higher than that of NCM811 (141.3 mAh g−1) at 2 C, and the capacity retention of NCM811-I increased by 13.6% after 100 cycles at 0.1 C and 13.4% after 500 cycles at 1 C compared to NCM811. This work provides a valuable routine to improve the rate capability of Ni-rich cathode materials, which may be applied to other oxide cathodes with sluggish Li-ion transportation.

FeNb11O29, anode material for high-power lithium-ion batteries: Pseudocapacitance and symmetrisation unravelled with advanced electrochemical and in situ/operando techniques

In the last years of research on new anode materials for advanced Lithium-Ion Batteries (LIBs), niobium-based oxides are raising growing attention due to very high theoretical capacities and high working potential that can prevent the formation of lithium dendrites, ensuring the safety of the batteries. Most of them crystallizes in open Wadsley–Roth shear structures, which show large Li-ion diffusion coefficients and promising applications in energy storage systems. In this paper, the complex structural and electrochemical features of FeNb11O29 are unravelled with in situ Raman Spectroscopy, operando X-Ray Diffraction and electrochemical techniques. The intrinsic pseudocapacitance shown by the iron niobate is correlated to large channels in its structure that cause weak Li+-host interactions and very little charge-transfer resistances. The symmetrisation of the octahedral framework that occurs after the reduction of Nb5+ cations, detected for the first time, seems to be the key of the electrochemistry of FeNb11O29, which shows excellent features for advanced high-power density LIBs.

Highly-concentrated electrolyte incorporating Li-ion solvation sheath interphase for encapsulation-free organic electrochromic devices

Electrolytes play an essential role in boosting the performance of electrochromic devices (ECDs), nevertheless, the detailed impact of highly-concentrated electrolytes (HCEs) on electrochromism remains elusive. In this work, we creatively report an eco-friendly, aqueous HCE based on lithium bis (trifluoromethanesul-phonyl)-imide (TFSILi), and investigate the potential of developed electrolyte for ECD applications through combining experimental and molecular dynamic simulation approaches. The radial distribution function calculations reveal that the primary solvation sheath of Li-ion is greatly alterd by the concentration of electrolyte. The formation of Li-ion solvation sheath containing TFSI− in electrolyte protects the electrochromic (EC) layer from being destroyed by free water. Mean squared displacement shows that the diffusion coefficient of Li-ion in 15 M HCE reaches up to 8.5 × 10−11 m2/s, indicating that high ion mobility enables faster charge transfer and efficient transport of Li-ion promotes interfacial reaction kinetics, which correlates-well with the experimental conductivity results. These findings demonstrate that HCEs can substantially improve the performance of organic ECDs, especially in terms of device stability, optical memory and switching rate. Notably, the solvation sheath nature of the developed HCE enables the development of encapsulation-free devices, which is greatly attractive for the industrialization of EC technology.

Excellent electrochemical properties, Li ion dynamics and room temperature work function of Li2MnO3 cathode thin films

We report on excellent electrochemical properties, Li ion diffusion coefficient and work function of Li2MnO3 thin films fabricated by RF sputtering technique. The x-ray diffraction study confirms the formation of Li2MnO3 thin film in layered structure. The x-ray photoelectron spectroscopy study confirms the existence of Li and Mn ions and their appropriate oxidation states in Li2MnO3 thin film. Work function of the Li2MnO3 thin film has been measured using scanning Kelvin probe microscopy and is found to be 5.51 eV. Electrochemical studies show that the Li2MnO3 thin film exhibits oxidation and reduction peaks at 2.98 V and 2.81 V respectively with the discharging capacity of 10 μAh cm−2 in the first cycle and 9 μAh cm−2 in the 100th cycle at a C rate of 25 μA cm−2. Electrochemical stability of Li2MnO3 thin film is probed by measuring the charge discharge profile with high sweep rate of 500 mV s−1. Li ion diffusion coefficient value is seen to 1.6 × 10−14 cm2 s−1 and 2.56 × 10−14 cm2 s−1 before and after the cycling respectively. Electrochemical studies indicate that Li2MnO3 thin films can be utilized as a promising cathode layer in all-solid thin film battery fabrication.

Hierarchically porous nanofibers comprising multiple core–shell Co3O4@graphitic carbon nanoparticles grafted within N-doped CNTs as functional interlayers for excellent Li–S batteries

Hierarchically porous nanofibers (NFs) comprising multiple core–shell Co3O4@graphitic carbon (GC) nanoparticles grafted within N-doped carbon nanotubes (CNTs) (Co3O4@GC/N-CNT NF) were rationally designed as functional interlayers for excellent Li–S batteries (LSBs). The well-grafted N-doped CNTs (N-CNTs) and high-conductivity GC layer coated on Co3O4 nanoparticles provided conductive channels for fast ionic/electronic transfer during charging–discharging. The Co3O4 nanoparticles inside the GC layer served as active polar sites for efficient anchoring of dissolved lithium polysulfides and ensured their reuse during redox reactions via fast charge transfer processes. Consequently, the assembled Li–S cell featuring a Co3O4@GC/N-CNT NF-coated separator and a pure sulfur electrode (70 wt% and 2.0 mg cm−2 loading) presented an excellent electrochemical performance, namely a high-rate capability and stable cycling performance at C-rates of 0.1, 0.5, and 1.0C. In addition, the Li-ion diffusion coefficient of the assembled Li–S cell (10−8 cm2 s−1) was one order of magnitude higher than those of the assembled Li–S cells featuring bare Co3O4 NF-coated and pristine separators (10−9 cm2 s−1). The remarkable overall cell performance was attributed to the combination of highly conductive N-CNTs, GC layer, and polar Co3O4 nanoparticles, which effectively trapped polysulfides. Therefore, we believe that the proposed unique nanostructure synthesis method can provide new insights into the development of sustainable and highly conductive polar materials as functional interlayers for advanced LSBs.