Interfacial Electronic States Research Articles

Metal-enhanced carbon-nitrogen material for selective detection of hazardous gases: Insights from interface electronic states

In this study, utilizing density functional theory, the C3N1 monolayer modified by Ir, Pd, Pt, and Rh atoms (Ir/Pd/Pt/Rh-C2N1) was chosen for selective adsorption of C2H2 amidst multiple gases (H2O, C2H2, and C4H10O2). According to the results of cohesive energy and ab initio molecular dynamics simulations, it is indicated that precious metal atoms can be stably anchored on the monolayer while enhancing the conductivity of the material The analysis of the electrostatic potential and work function determined the highly active sites and electron release capacity. In addition, the adsorption energy and distance disclosed the gas-solid interface structure of multiple gases on the Ir/Pd/Pt/Rh-C2N1 monolayer. Importantly, C2H2 exhibits strong responses to p-type semiconductor Pt-C2N1 and n-type semiconductor Ir-C2N1, respectively. Crystal Orbital Hamilton Population reveals the difference in adsorption energy due to modifications involving four precious metals. Interestingly, for the first time, the density of states calculation reveals that under the coexistence of multiple gases, the Pt/Ir-C2N1 monolayer effectively eliminates the interference of other gases and has a unique response only to C2H2. In real situations, with the basis of Gibbs free energy and Einstein's law of diffusion, it was determined that Pt-C2N1 and Ir-C2N1 showed excellent hydrophobicity, a wider temperature range, and a low diffusion activation energy barrier. In summary, Pt-C2N1 and Ir-C2N1 detect C2H2 without interference, maintaining fundamental principles, responsiveness, stability, and versatility unaffected by external factors.

Giant Tunneling Electro‐Resistance in Ultrathin Ferroelectric Tunnel Junctions: The Interface Barrier Gain Mechanism

AbstractUltrathin ferroelectric tunnel junctions (FTJs) hold considerable promise for next‐generation, high‐speed, low‐power, and high‐density nonvolatile memory applications. Achieving a substantial tunneling electro‐resistance (TER) remains a challenge as the ferroelectric layer is thinned to nanoscale dimensions, often resulting in a diminished or lost polarization. An innovative interface barrier gain mechanism is introduced, employing interface electronic state modulation to precisely control the size of an additional interface barrier. This strategy lessens the dependency of the tunneling barrier on ferroelectric polarization strength, facilitating a remarkable TER even at ferroelectric thicknesses as minimal as ≈1 nm. The focus is on composite FTJs using In2Se3/MTe2 (M = Mo, W), where the inclusion of an MTe2 monolayer disrupts the asymmetric electrode configuration. The weak ferroelectric polarization reversal of the In2Se3 monolayer effectively modulates the electronic state coupling at the In2Se3/MTe2 interface. This modulation leads to variations in the width and height of the Schottky barrier at the heterojunction‐electrode interface corresponding with the ferroelectric polarization reversal, establishing a beneficial Ohmic contact in the “on” state and resulting in an exponential TER increase up to 5.4 × 106%. This work introduces a universal mechanism to overcome the thickness limitations traditionally associated with enhancing TER, marking a significant advancement in the development of ultrathin ferroelectric nonvolatile devices.

Impedance dynamics in tandem solar cells based on c-Si with upper layers of CsPbBr3 (CsPbI3) perovskite nanocrystals

The application of an additional nanoparticle layer is a common practice for enhancing the optical and electrical properties of third-generation solar cells. In this study, we present the results of impedance spectroscopy (IS) for modified solar cells using Nyquist and Bode diagrams. The structure investigated consists of a conventional double junction based on crystalline silicon (c-Si) coated with thin films of inorganic perovskite nanocrystals (NC) of lead halides CsPbI3 and CsPbBr3. The latter are characterized by a significant phonon disorder, which leads to unique electron-phonon interactions and dielectric responses. The IS results indicate that, under the same conditions, the measured Nyquist plots align well with the simulated ones. An equivalent circuit model is proposed, featuring ohmic resistance, recombination resistance, and geometric capacitance. These elements arise due to charge accumulation, charge transfer resistance, and/or additional interfacial electronic states. The study finds that the introduction of a CsPbI3 layer enhances the photoresponse under bias conditions, but this photoresponse leads to a decrease in DC conductivity. In contrast, the addition of a CsPbBr3 layer obstructs the photoresponse under bias while slightly improving the photoresponse in the absence of an applied voltage. The results obtained contribute to the improvement of tandem solar cell characteristics featuring top layers of perovskite nanocrystals.

Selective Phosphate Adsorption Using Topologically Regulated Binary-Defect Metal-Organic Frameworks: Essential Role of Interfacial Electron Mobility.

Metal-organic framework (MOF)-modified biochars (BC) have gained recognition as potent adsorbents for phosphate. However, essential insights into the electronic interfacial state of the MOFs remain lacking. In this study, we propose a novel topological transformation strategy to directionally regulate the interfacial electronic states of BC/MOFs composites. The optimized BC/MOFs exhibited an excellent selective phosphate adsorption capacity of 188.68 mg·g-1, coupled with rapid sorption kinetics of 6.81 mg·(g·min0.5)-1 in simulated P-laden wastewater. When challenged with real bioeffluent, such efficacy was still maintained (5 mg·L-1, 25.92 mg·g-1). This superior performance was due to the Fe(III) → Fe(II) transition, promoting electron mobility and leading to the anchoring of Mg(II) to form specific coordination unsaturated sites (Mg-CUS) for phosphate adsorption. Importantly, the simultaneous regulation of binary defects further enhances electron mobility, resulting in the formation of sp3 unequal hybrid orbitals with a stronger internal coupling capability between Mg 3s in Mg-CUS and O 2p in phosphate. Furthermore, the high electron affinity of Mg effectively promotes electron cycling, endowing BC/MOFs with a distinct self-healing capability to facilitate phosphate desorption. The outcomes of this study provide novel perspectives for electronic regulated phosphate adsorption.

Interfacial Electronic States of GeC/g-C3N4 van der Waal Heterostructure with Promising Photocatalytic Activity via Hydrogenation.

The bandgap of most known two-dimensional materials can be tuned by hydrogenation, although certain 2D materials lack a sufficient wide bandgap. Currently, it would be perfect to design non-toxic, low-cost, and high-performance photocatalysts for photocatalytic water splitting via hydrogenation. We systematically examine the impact of hydrogenation on the optical and electronic characteristics of GeC/g-C3N4 vdW heterostructures (vdWHs) with four different stacking patterns using first-principles calculations. The phonon spectra, interlayer distance, binding energies and ab initio molecular dynamics calculations show the kinetic, mechanical, and thermal stability of GeC/g-C3N4 vdWH after hydrogenation at 300, 500 and 800 K and possesses anisotropic Poisson's ratio, Young's and bulk modulus, suggesting that it's a promising candidate for experimental fabrication. According to an investigation of its electronic properties, GeC/g-C3N4 vdWH has a bandgap of 1.28 eV, but hydrogenation dramatically increases it to 2.47 eV. As a result of interface-induced electronic doping, the electronic states in g-C3N4 might be significantly adjusted by coming into contact with hydrogenated GeC sheets. The vdWH exhibits a type-II semiconductor, which can enhance the spatial separation of electron-hole pairs and has a strong red-shift of absorption coefficient than those of the constituent monolayers. The high potential drop caused by the significant valence and conduction band offsets effectively separated the charge carriers. The absorption coefficient of GeCH2/g-C3N4 vdWH is highly influenced by a biaxial compressive strain more than the biaxial tensile strain. Our theoretical research implies that the hydrogenated GeCH2/g-C3N4 vdWH possesses tunable optical and electronic behaviour for use as a hole-transport material in solar energy harvesting, nanoelectronic and optoelectronic devices.

Local symmetry-driven interfacial magnetization and electronic states in (ZnO)n/(w-FeO)n superlattices.

Superlattices constructed with the wide-band-gap semiconductor ZnO and magnetic oxide FeO, both in the wurtzite structure, have been investigated using spin-polarized first-principles calculations. The structural, electronic and magnetic properties of the (ZnO)n/(w-FeO)n superlattices were studied in great detail. Two different interfaces in the (ZnO)n/(w-FeO)n superlattices were identified and they showed very different magnetic and electronic properties. Local symmetry-driven interfacial magnetization and electronic states can arise from different Fe/Zn distributions at different interfaces or spin ordering of Fe in the superlattice. The local symmetry-driven interfacial magnetization and electronic states, originating either from different Fe/Zn distribution across interfaces I and II, or by spin ordering of Fe in the superlattice, can be identified. It was also found that, in the case of the ferromagnetic phase, the electrons are more delocalized for the majority spin but strongly localized for the minority spin, which resulted in interesting spin-dependent transport properties. Our results will pave the way for designing novel spin-dependent electronic devices through the construction of superlattices from semiconductors and multiferroics.

Interfacial electronic state between hexagonal ZnO and cubic NiO.

The interface of two dissimilar materials gives rise to a myriad of interesting structural, magnetic, and electronic properties that may be utilized to produce novel materials with unique characteristics and functions. In particular, growing a cubic oxide film on top of a hexagonal oxide substrate results in such unique properties due to the conflict of their respective stabilization mechanisms within the interface layer. This study aims to elucidate the electronic properties of the interface between hexagonal ZnO and cubic NiO by analyzing the interface electronic states within epitaxial NiO films grown on ZnO substrates, expressed in the form of ultraviolet photoemission spectroscopy (UPS) for valence band structure and X-ray absorption spectroscopy (XAS) spectra for conduction band structure. This is accomplished through a modeling approach in which the film, substrate, and interface signals are assumed to be related to each other by a set of mathematical equations, and then rearranging and modulating the equations to obtain unique UPS and XAS spectra that depict the interface electronic states.

Spatially modulated interface states in a two-dimensional potential: Single-layer RbI on Ag(111)

Alkali halides are known to exhibit interface electronic states (IES) when deposited on metal surfaces with ultra-thin coverage. Here, we examine the IES formed by sub-monolayer RbI growth on Ag(111), which exhibits spatial variations in electronic structure in surprising contrast to the results previously obtained for other alkali halides. We find that this spatially dependent behavior can be qualitatively modeled by using a two-dimensional cosine potential commensurate with the moiré superstructure, where the IES is constructed from the well-known analytical solutions to the Mathieu equation. Our results indicate this potential is more corrugated than for similar potentials reported for other alkali halides, a result of substrate–adlayer charge transfer interactions that are stronger for RbI. This two-dimensional effective potential leads to anisotropy in the effective electron mass, in surprising contrast to previous results for other alkali halides, which report a single isotropic mass.

Interfacial electronic states and self-formed asymmetric Schottky contacts in polar α-In2Se3/Au contacts

In recent years, the two-dimensional (2D) semiconductor α-In2Se3 has great potential for applications in the fields of electronics and optoelectronics due to its spontaneous iron electrolysis properties. Through ab initio electronic structure calculations and quantum transport simulations, the interface properties and transport properties of α-In2Se3/Au contacts with different polarization directions are studied, and a two-dimensional α-In2Se3 asymmetric metal contact design is proposed. When α-In2Se3 is polarized upward, it forms an n-type Schottky contact with Au. While when α-In2Se3 is polarized downward, it forms a p-type Schottky contact with Au. More importantly, significant rectification effect is found in the asymmetric Au/α-In2Se3/Au field-effect transistor. The carrier transports under positive and negative bias voltages are found to be dominated by thermionic excitation and tunneling, respectively. These findings provide guidance for the further design of 2D α-In2Se3-based transistors.

Hybrid Metal-Ligand Interfacial Dipole Engineering of Functional Plasmonic Nanostructures for Extraordinary Responses of Optoelectronic Properties.

Programmable manipulation of inorganic-organic interfacial electronic properties of ligand-functionalized plasmonic nanoparticles (NPs) is the key parameter dictating their applications such as catalysis, photovoltaics, and biosensing. Here we report the localized surface plasmon resonance (LSPR) properties of gold triangular nanoprisms (Au TNPs) in solid state that are functionalized with dipolar, conjugated ligands. A library of thiocinnamate ligands with varying surface dipole moments were used to functionalize TNPs, which results in ∼150 nm reversible tunability of LSPR peak wavelength with significant peak broadening (∼230 meV). The highly adjustable chemical system of thiocinnamate ligands is capable of shifting the Au work function down to 2.4 eV versus vacuum, i.e., ∼2.9 eV lower than a clean Au (111) surface, and this work function can be modulated up to 3.3 eV, the largest value reported to date through the formation of organothiolate SAMs on Au. Interestingly, the magnitude of plasmonic responses and work function modulation is NP shape dependent. By combining first-principles calculations and experiments, we have established the mechanism of direct wave function delocalization of electrons residing near the Fermi level into hybrid electronic states that are mostly dictated by the inorganic-organic interfacial dipole moments. We determine that both interfacial dipole and hybrid electronic states, and vinyl conjugation together are the key to achieving such extraordinary changes in the optoelectronic properties of ligand-functionalized, plasmonic NPs. The present study provides a quantitative relationship describing how specifically constructed organic ligands can be used to control the interfacial properties of NPs and thus the plasmonic and electronic responses of these functional plasmonics for a wide range of plasmon-driven applications.

MXene-based Materials for Water Splitting: Synthesis and Modification.

With abundant metal site and tunable electronic structure, MXene is considered as a promising electrocatalyst for the conversion of energy molecules. In this review, the latest research progress on inexpensive MXene-based catalysts for water electrolysis is summarized. Typical preparation and modification methods and their advantages and disadvantages are briefly discussed, with a focus on the regulation and design of the surface interface electronic states, which improve the electrocatalytic performance of MXene-based materials. The main strategies for the electronic state modification include end-group modification, heteroatom doping, and heterostructure construction. Some limitations of MXene-based materials, which should be considered in the rational design of advanced MXene-based electrocatalyst, are also discussed. Finally, prospects for the rational design of Mxene-based electrocatalysts is proposed.

Local Built-In Field at the Sub-nanometric Heterointerface Mediates Cascade Electrochemical Conversion of Lithium-sulfur Batteries.

Heterogeneous catalytic mediators have been proposed to play a vital role in enhancing the multiorder reaction and nucleation kinetics in multielectron sulfur electrochemistry. However, the predictive design of heterogeneous catalysts is still challenging, owing to the lack ofin-depth understanding of interfacial electronic states and electron transfer on cascade reaction in Li-S batteries. Here, a heterogeneous catalytic mediator based on monodispersed titanium carbide sub-nanoclusters embedded in titanium dioxide nanobelts is reported. The tunable catalytic and anchoring effects of the resulting catalyst are achieved by the redistribution of localized electrons caused by the abundant built-in fields in heterointerfaces. Subsequently, the resulting sulfur cathodes deliver an areal capacity of 5.6 mAh cm-2 and excellent stability at 1 C under sulfur loading of 8.0mg cm-2 . The catalytic mechanism especially on enhancing the multiorder reaction kinetic of polysulfides is further demonstrated via operando time-resolved Raman spectroscopy during the reduction process in conjunction with theoretical analysis.

Chemical and electronic properties of interfaces between RuO2 and Hf0.5Zr0.5O2 studied by x-ray photoelectron spectroscopy

Recently, the extensive study of the platinum group metal oxide electrodes for TiN replacement in Hf0.5Zr0.5O2 (HZO)-based ferroelectric memory stacks began. In this work, we use high sensitivity of x-ray photoelectron spectroscopy to the interface chemical and electronic states to investigate the chemistry and band alignment between HZO and RuO2, which is one of the most suitable noble metal oxide electrodes. We report that RuO2 is easily reduced to metallic Ru during the atomic layer deposition (ALD) of HZO because of the chemical reaction between the oxygen stored in RuO2 and metallic precursors used for HZO deposition. This process makes it impossible to use RuO2 as a bottom electrode, when HZO is grown by the conventional thermal ALD process (with H2O as a reactant). At the same time, RuO2 may be effectively conserved if one uses more active oxygen reactants for the HZO growth because of the re-oxidation of the newly formed Ru. RuO2 is also effectively conserved at the top interface, at least within the thermal budget of the growth of all functional layers. We also report the detailed investigation of the band alignment between RuO2 and HZO in both type of stacks (with reduced and conserved RuO2) and both interfaces with HZO (top and bottom), which may be useful for the understanding of the ferroelectric properties of the related stacks in the future. In addition, the potential of RuO2 utilization for the reliability improvement of HZO-based stacks is discussed.

Interfacial Electronic and Photovoltaic Performance of a Novel Lead‐Free Z‐Scheme CsSnBr3/MoSe2 Perovskite Heterostructure: A Theoretical and Experimental Study

Sn‐based perovskite materials with nontoxic, low cost, and unique structure have attracted much attention. However, their efficiency only reaches 14.09% due to the higher carrier recombination rate and short carrier lifetime in photovoltaic applications. Herein, the interfacial electronic structure, optical absorption, interfacial charge transfer mechanism, and photovoltaic performance of the CsSnBr3/MoSe2 perovskite heterostructure are systematically investigated by theoretical calculation and experimental observation. The results indicate that the strong coupling and hybridization of interfacial electronic states can lead to a narrowing bandgap, which induces an excellent optical absorption of the CsSnBr3/MoSe2 perovskite heterostructure in the visible spectrum. Excitingly, the charge transfer at the interface forms a built‐in electric field, which can effectively promote the interfacial charge transfer between CsSnBr3 (001) and MoSe2 monolayer, complying with a Z‐scheme mechanism. Moreover, the photovoltaic performance of the CsSnBr3/MoSe2 heterostructure significantly enhances due to excellent light absorption and Z‐scheme system for extending carrier lifetime. An effective strategy for designing highly efficient Sn‐based perovskite solar cells is reported.

Organic Heterocyclic Strategy for Precisely Regulating Electronic State of Palladium Interface to Boost Alcohol Oxidation

AbstractExploring highly‐efficient palladium (Pd)‐based electrocatalysts for the alcohol oxidation reaction (AOR) is crucial yet challenging for chemists due to the vague Pd interface with an uncontrollable electronic environment. Herein, an organic heterocyclic strategy is used for the first time to modulate the electronic state of Pd electrocatalysts by anchoring Pd nanoparticles to conjugated microporous polymers (CMPs) with varied S‐, N‐, O‐, or S, N‐heterocycles. Among these CMPs, the S, N‐containing thiazole heterocyclic polymer SNC with Pd catalyst exhibits highly‐efficient current densities of 1575.0 mA mgPd−1 for methanol oxidation and 1071.0 mA mgPd−1 for ethanol oxidation, which are among the highest performance in the heterocyclic modulated Pd systems and surpass the commercial Pd black catalyst. Detailed theory calculations suggest that although the furan (O‐heterocycle) polymer OC has the strongest charge transfer (0.057 |e|) with the Pd cluster, the moderate electron transfer (0.041 |e|) of the Pd/SNC heterojunction with an S···N···Pd noncovalent interaction shows the best catalytic reaction kinetics. Moreover, the d‐band of the Pd/SNC system is closer to the volcano vertex than its counterparts. These results indicate that appropriate electron transfer intensity regulation of Pd electronic state by well‐defined heterocyclic structures may significantly improve AOR activity.

Identifying and Removing the Interfacial States in Metal-Oxide-Semiconductor Schottky Si Photoanodes for the Highest Fill Factor.

A critical bottleneck for realizing an efficient Schottky type Si photoelectrode is minimizing the charge extraction losses across the heterointerface via reducing the unfavorite defects. This requires a clear microscopic insight into the correlation between interfacial features and photoconversion. Herein, by taking the n-Si/oxide (MOx)/Ni as the prototype, the heterointerface with the different characteristics and its effects on charge transportation and the corresponding photoelectric/photoelectrochemical (PEC) behaviors were clarified. An ultra-thin AlOx layer can effectively diminish the interfacial pinning of n-Si/Ni and significantly facilitate the photoconversion; meanwhile, it results in some unexpected donor-like deep defects at around 0.59 eV below the conduction band of n-Si, which could be ionized under a reverse bias and cause about 10% photogenerated charge recombination. Fortunately, these deep defects can be further eliminated by cooperating AlOx with a thin Au layer. The AlOx/Au dual-interlayer can remove almost all unexpected defects and maximize the efficiency of the electric field for charge extraction from semiconductor Si for the surface catalytic reaction. Eventually, the n-Si/SiOx/AlOx/Au/Ni/NiFeOx photoanode exhibited a record fill factor of 0.75 for the corresponding photoelectric device and an applied bias photon-to-current efficiency of 3.71% for PEC water oxidation. This study provides definite insights into interfacial electronic states and elaborates their crucial role in solar photoelectric conversion.

First-Principles Calculation of the Bonding Strength of the Al2O3-Fe Interface Enhanced by Amorphous Na2SiO3.

In this paper, the interfacial adhesion work (Wad), tensile strength, and electronic states of the Fe-amorphous Na2SiO3-Al2O3 and Fe-Al2O3 interfaces are well-investigated, utilizing the first-principles calculations. The results indicate that the Fe-amorphous Na2SiO3-Al2O3 interface is more stable and wettable than the interface of Fe-Al2O3. Specifically, the interfacial adhesion work of the Fe-amorphous Na2SiO3 interface is 434.89 J/m2, which is about forty times that of the Fe-Al2O3 interface, implying that the addition of amorphous Na2SiO3 promotes the dispersion of Al2O3 particle-reinforced. As anticipated, the tensile stress of the Fe-amorphous Na2SiO3-Al2O3 interface is about 46.58 GPa over the entire critical strain range, which is significantly greater than the Fe-Al2O3 interface control group. It could be inferred that the wear resistance of Al2O3 particle-reinforced is improved by adding amorphous Na2SiO3. To explain the electronic origin of this excellent performance, the charge density and density of states are investigated and the results indicate that the O atom in amorphous Na2SiO3 has a bonding action with Fe and Al; the amorphous Na2SiO3 acts as a sustained release. This study provides new ideas for particle-reinforced composites.

Activation of H2O Tailored by Interfacial Electronic States at a Nanoscale Interface for Enhanced Electrocatalytic Hydrogen Evolution.

Despite the fundamental and practical significance of the hydrogen evolution reaction (HER), the reaction kinetics at the molecular level are not well-understood, especially in basic media. Here, with ZIF-67-derived Co-based carbon frameworks (Co/NCs) as model catalysts, we systematically investigated the effects of different reaction parameters on the HER kinetics and discovered that the HER activity was directly dependent not on the type of nitrogen in the carbon framework but on the relative content of surface hydroxyl and water (OH–/H2O) adsorbed on Co active sites embedded in carbon frameworks. When the ratio of the OH–/H2O was close to 1:1, the Co/NC nanocatalyst showed the best reaction performance under the condition of high-pH electrolytes, e.g., an overpotential of only 232 mV at a current density of 10 mA cm–2 in the 1 M KOH electrolyte. We unambiguously identified that the structural water molecules (SWs) in the form of hydrous hydroxyl complexes absorbed on metal centers {OHad·H2O@M+} were catalytic active sites for the enhanced HER, where M+ could be transition or alkaline metal cations. Different from the traditional hydrogen bonding of water, the hydroxyl (hydroxide) groups and water molecules in the SWs were mainly bonded together via the spatial interaction between the p orbitals of O atoms, exhibiting features of a delocalized π-bond with a metastable state. These newly formed surface bonds or transitory states could be new weak interactions that synergistically promote both interfacial electron transfer and the activation of water (dissociation of O–H bonds) at the electrode surface, i.e., the formation of activated H adducts (H*). The capture of new surface states not only explains pH-, cation-, and transition-metal-dependent hydrogen evolution kinetics but also provides completely new insights into the understanding of other electrocatalytic reductions involving other small molecules, including CO2, CO, and N2.

Enhancing catalytic activity of Fe3O4 for electrochemical water oxidation via the coupling of OER-inert Au

Interfacial charge transfer efficiency and electronic states of active sites are two essential issues to restrict catalytic activity of electrocatalysts for oxygen evolution reaction (OER). In this work, we show that although Au is recognized to be inert towards OER, the catalytic activity of Fe3O4 catalyst for OER was highly boosted by coupling Fe3O4 with Au to address these two issues. Here, Au nanoparticles were attached to hierarchical Fe3O4 microsphere through electrochemical deposition, a mild and rapid approach that can be accomplished within 3 min and requires no sophisticated equipment. With the coupling of Au, interfacial charge transfer resistance of Fe3O4 declined remarkably. On the other hand, oxidability of Fe sites and electron accepting capability of Au sites was elevated due to strong interaction between Au and Fe3O4. Owing to these two merits induced by Au, Fe3O4 exhibited enhanced catalytic activity for OER. The potential of Fe3O4 to obtain 10 mA/cm2 decreased by 640 mV, the current density was amplified up to 2.5 fold at the potential of 2 V (vs SCE), and the Tafel slop was reduced by 146 mV/dec.

Simultaneous interfacial interaction and built-in electric field regulation of GaZnON@NG for high-performance lithium-ion storage

Interfacial interaction and built-in electric field regulation strategy is developed to construct (Ga1−xZnx)(N1−xOx) (GaZnON) nanoparticles coupled with nitrogen-doped graphene (NG) (GaZnON@NG) via a simple and facile method. Advanced structural characterization and density functional theory (DFT) analysis reveals the strong bridging bonds (Ga–N/N–C) and the interfacial charge transfer in GaZnON@NG. This interfacial interaction can subtly regulate the interfacial electronic state and improve the surface electron density and charge transport kinetics for efficient lithium-ion storage. As a proof-of-concept study, this well-designed GaZnON@NG heterostructure anode shows an enhanced lithium-ion storage performance of 1073.6 mA h g−1 at 0.1 A g−1 after 200 cycles. Even at 5.0 A g−1, the reversible capacity is still maintained at 338.6 mA h g−1 after 2000 cycles. Electrochemical kinetic analysis corroborates the enhanced pseudocapacitive contribution and lithium-ion reaction kinetics in the GaZnON@NG anode. Furthermore, XRD and XPS analysis of the GaZnON@NG heterostructure reveals good structural stability and reversible lithium-ion intercalation mechanism. DFT analysis further reveals that this GaZnON@NG heterostructure anode possesses lower lithium-ion adsorption energy and higher charge and discharge rates. This interfacial interaction strategy can open opportunities for advanced energy storage applications and beyond.