Well-defined Interface Research Articles

Tuning the thermodynamic ordering of strongly correlated protons in ice by angstrom-scale interface modification

The static and dynamic behaviour of strongly correlated many-body protons in nanoscale hydrogen-bond networks plays crucial roles in a wide range of physicochemical, biological and geological phenomena in nature. However, because of the difficulty of probing and manipulating the proton configuration in nanomaterials, controlling the cooperative behaviour of many-body protons remains challenging. By combining proton-order sensitive nonlinear optical spectroscopy and well-defined interface modification at molecular/atomic scale, we demonstrate the possibility of extensively tuning the emergent physical properties of strongly correlated protons beyond the thermodynamic constraints of bulk hydrogen bonds. Focusing on heteroepitaxially grown crystalline ice films as a model of a strongly correlated and frustrated proton system, we show that the emergence and disappearance of a high-Tc proton order on the nano- to mesoscale is readily switched by angstrom-scale interface engineering. These results pave a way to designing and controlling emergent properties of correlated proton systems.

In-situ assembly of 3D VS2/Reduced graphene oxide with superior lithium ion storage performance: The role of heterojunction

VS2 is a potential anode material for lithium-ion batteries (LIBs) due to its advantageous properties. Herein, a novel three-dimensional (3D) VS2/reduced graphene oxide (rGO) heterostructure (VS2-rGO) was fabricated by in-situ assembly of caterpillar-like VS2 nanosheets on rGO. This 3D VS2-rGO with a well-defined heterojunction interface is engineered to mitigate the volumetric expansion of VS2 during Li + intercalation/deintercalation cycles. This optimized design promotes enhanced conductivity across the heterojunction, facilitating efficient electron and ion transport. The VS2-rGO electrode shows higher reversible capacity and better rate performance (644.02 mA h g−1 at 0.1 A g−1 after 140 cycles, 526.66 mA h g−1 at 2 A g−1) as compared to the pure VS2 electrode (433.69 mA h g−1 at 0.1 A g−1 after 140 cycles, 63.91 mA h g−1 at 2 A g−1). Ex-situ XRD analysis suggests that the Li + storage mechanism in the VS2-rGO electrode involves the initial intercalation, followed by intercalation and conversion. The lower Li + diffusion barrier within the VS2-rGO heterojunction (0.183 eV) compared to the VS2 layers (0.225 eV), as predicted by first-principles calculations, resulting the enhanced Li + transport kinetics and improved cycling performance of the VS2-rGO electrode material. This work offers novel perspectives for the influence of heterojunctions on LIBs.

Fabrication of cobalt phosphide/nitride/carbon nanotube composite: An efficient bifunctional catalyst for hydrogen and oxygen evolution

Designing composites with rational structure and composition is a promising approach to obtain efficient electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). In this study, zeolitic imidazolate frameworks-67 (ZIF-67) is employed as a self-sacrificing template to synthesize Co/carbon nanotubes (CNTs) precursor, which is subsequently in-situ nitrided and phosphorized to form cobalt phosphide/nitride/carbon nanotubes (Co2P/Co4N/CNTs) composite. The realized Co2P/Co4N composite exhibits heterogeneous nanoparticle microstucture with an average diameter of approximately 10 nm, encapsulated by carbon nanotubes with a porous dodecahedral array. Moreover, there is a well-defined interface between cobalt phosphide, cobalt nitride phases, and carbon nanotubes species. Benefiting from the synergistic effect of Co4N and Co2P, rich active sites, and high conductivity of CNTs, the composite catalyst demonstrates remarkable HER and OER activities, requiring overpotentials of 228 and 389 mV to support 100 mA cm−2 current density, respectively. This work presents a novel strategy for designing efficient bifunctional catalysts towards HER and OER.

On the Electrochemical Growth of a Crystalline p-n Junction From Aqueous Solutions.

Our society largely relies on inorganic semiconductor devices which are, so far, fabricated using expensive and complex processes requiring ultra-high vacuum equipment. Here we report on the possibility of growing a p-n junction taking advantage of electrochemical processes based on the use of aqueous solutions. The growth of the junction has been carried out using the Electrochemical Atomic Layer Deposition (E-ALD) technique, which allowed to sequentially deposit two different semiconductors, CdS and Cu2S, on an Ag(111) substrate, in a single procedure. The growth process was monitored in situ by Surface X-Ray Diffraction (SXRD) and resulted in the fabrication of a thin double-layer structure with a high degree of crystallographic order and a well-defined interface. The high-performance electrical characteristics of the device were analysed ex-situ and show the characteristic feature of a diode.

Mechanism exploration of deep eutectic solvents extraction of indole in wash oil

Deep eutectic solvents (DESs) have gained significant interest for extracting indole from wash oil due to their exceptional characteristics and excellent extraction performance. An in-depth comprehension of the intermolecular interactions within the DES-wash oil system is crucial for developing principles that can guide the design of highly efficient DESs for indole extraction. The intermolecular interactions, molecular associations, and density profile in the DES-wash oil system were investigated using molecular dynamics simulation and FT-IR/1H NMR characterization. The DES was composed of tetraethylammonium chloride and glycerol (TEAC/GLY), which was selected based on its exceptional experimental performance. Both the simulation and spectra results show that indole has strong hydrogen bond with TEAC/GLY. The hydrogen bond promotes indole extraction while van der Waals interactions cause aromatics entrainment. The components in wash oil exhibit two distinct molecular associations before and after the extraction of indole. A well-defined interface is established between the wash oil molecules and DES components, and indole has a preference for accumulating at the interface. The results provide an insight into the mechanism of extracting indole from wash oil using DES.

Structure and topography of the synaptic V-ATPase-synaptophysin complex.

Synaptic vesicles are organelles with a precisely defined protein and lipid composition1,2, yet the molecular mechanisms for the biogenesis of synaptic vesicles are mainly unknown. Here we discovered a well-defined interface between the synaptic vesicle V-ATPase and synaptophysin by in situ cryo-electron tomography and single-particle cryo-electron microscopy of functional synaptic vesicles isolated from mouse brains3. The synaptic vesicle V-ATPase is an ATP-dependent proton pump that establishes the proton gradient across the synaptic vesicle, which in turn drives the uptake of neurotransmitters4,5. Synaptophysin6 and its paralogues synaptoporin7 and synaptogyrin8 belong to a family of abundant synaptic vesicle proteins whose function is still unclear. We performed structural and functional studies of synaptophysin-knockout mice, confirming the identity of synaptophysin as an interaction partner with the V-ATPase. Although there is little change in the conformation of the V-ATPase upon interaction with synaptophysin, the presence of synaptophysin in synaptic vesicles profoundly affects the copy number of V-ATPases. This effect on the topography of synaptic vesicles suggests that synaptophysin assists in their biogenesis. In support of this model, we observed that synaptophysin-knockout mice exhibit severe seizure susceptibility, suggesting an imbalance of neurotransmitter release as a physiological consequence of the absence of synaptophysin.

Lattice Strain and Mott-Schottky Effect of the Charge-Asymmetry Pd1Fe Single-Atom Alloy Catalyst for Semi-Hydrogenation of Alkynes with High Efficiency.

The ideal interface design between the metal and substrate is crucial in determining the overall performance of the alkyne semihydrogenation reaction. Single-atom alloys (SAAs) with isolated dispersed active centers are ideal media for the study of reaction effects. Herein, a charge-asymmetry "armor" SAA (named Pd1Fe SAA@PC), which consists of a Pd1Fe alloy core and a semiconducting P-doped C (PC) shell, is rationally designed as an ideal catalyst for the selective hydrogenation of alkynes with high efficiency. Multiple spectroscopic analyses and density functional theory calculations have demonstrated that Pd1Fe SAA@PC is dual-regulated by lattice tensile and Schottky effects, which govern the selectivity and activity of hydrogenation, respectively. (1) The PC shell layer applied an external traction force causing a 1.2% tensile strain inside the Pd1Fe alloy to increase the reaction selectivity. (2) P doping into the C-shell layer realized a transition from a p-type semiconductor to an n-type semiconductor, thereby forming a unique Schottky junction for advancing alkyne semihydrogenation activity. The dual regulation of lattice strain and the Schottky effect ensures the excellent performance of Pd1Fe SAA@PC in the semihydrogenation reaction of phenylethylene, achieving a conversion rate of 99.9% and a selectivity of 98.9% at 4 min. These well-defined interface modulation strategies offer a practical approach for the rational design and performance optimization of semihydrogenation catalysts.

Facet-Dependent Interfacial Charge Transfer between T-Phase VS2 Nanoflakes and Rutile TiO2 Single Crystals.

The hybridizations of two-dimensional (2D) metallic materials with semiconducting transition metal oxides (TMOs) register attractive heterojunctions, which can find various applications in photostimulated circumstances. In this work, we developed an ambient-pressure chemical vapor deposition method to directly grow T-VS2 on atomically smooth rutile TiO2 single crystals with different terminations and thus successfully constructed a heterojunction model of VS2/TiO2 with a well-defined clean interface. Detailed measurements with Kelvin probe force microscopy revealed the facet-dependent charge transfer occurring at the VS2/TiO2 interfaces, seeing variations not only in the amount and direction of the transferred electrons but also in the photoinduced surface potential changes and the dynamics of photogenerated charge carriers under ultraviolet irradiation. Interestingly, ultrathin T-VS2 was found with considerable magnetism at room temperature, disregarding the charge exchange with the TiO2 substrates. These results may bring deep insights into the photoinspired functionalities of the hybridized system combining metallic transition metal dichalcogenides and TMO materials.

Performance analysis of Al stainless steel joints fabricated by friction stir welding: Microstructure, mechanical, and tribology

Hybrid structures, incorporating both aluminum and steel, hold potential for applications in automobile, aerospace, and marine industries. This research delves into the effects of friction stir welding on dissimilar joints (AA2024-T3 and SS304), with a focus on microstructural, mechanical, and tribological aspects. The study identifies optimal welding conditions at (tool rotational speed 710 r/min, traverse speed20 mm/min, tool pin offset1.5 mm towards aluminum, and tilt angle of 1.75 deg) that yield a well-defined joint interface, contrasting with flaws observed at a 40 mm/min traverse speed due to insufficient heat input. Under optimal conditions at 20 mm/min, a well-clean serrated interface, defect-free microstructural evolution, improved surface characteristics; enhanced mechanical performance resulting in higher ultimate tensile strength of 319 MPa with joint efficiency of 72.5 and better tribological performance were achieved with lower wear rate of 1.1607 × 10−5 g/Nm compared to those at 40 mm/min, highlighting the crucial role of optimized friction stir welding parameters in achieving high-quality dissimilar joints with desirable properties.

Electric-Field-Assisted Synthesis of Cu/MoS2 Nanostructures for Efficient Hydrogen Evolution Reaction.

Molybdenum sulfide-oxide (MoS2, MS) emerges as the prime electrocatalyst candidate demonstrating hydrogen evolution reaction (HER) activity comparable to platinum (Pt). This study presents a facile electrochemical approach for fabricating a hybrid copper (Cu)/MoS2 (CMS) nanostructure thin-film electrocatalyst directly onto nickel foam (NF) without a binder or template. The synthesized CMS nanostructures were characterized utilizing energy-dispersive X-ray spectroscopy (EDS), scanning electron microscopy (SEM), X-ray diffraction (XRD), and electrochemical methods. The XRD result revealed that the Cu metal coating on MS results in the creation of an extremely crystalline CMS nanostructure with a well-defined interface. The hybrid nanostructures demonstrated higher hydrogen production, attributed to the synergistic interplay of morphology and electron distribution at the interface. The nanostructures displayed a significantly low overpotential of -149 mV at 10 mA cm-2 and a Tafel slope of 117 mV dec-1, indicating enhanced catalytic activity compared to pristine MoS2.This research underscores the significant enhancement of the HER performance and conductivity achieved by CMS, showcasing its potential applications in renewable energy.

CoFe2O4 on Mica Substrate as Flexible Ethanol Gas Sensor in Self-Heating Mode.

In this study, a novel flexible ethanol gas sensor was created by the deposition of a CoFe2O4 (CFO) thin film on a thin mica substrate using the pulsed laser deposition technique. Transition electron microscopy (TEM) investigations clearly demonstrated the successful growth of CFO on the mica, where a well-defined interface was observed. Ethanol gas-sensing studies showed optimal performance at 200 °C, with the highest response of 19.2 to 100 ppm ethanol. Operating the sensor in self-heating mode under 7 V applied voltage, which corresponds to a temperature of approximately 200 °C, produced a maximal response of 19.2 to 100 ppm ethanol. This aligned with the highest responses observed during testing at 200 °C, confirming the sensor's accuracy and sensitivity to ethanol under self-heating conditions. In addition, the sensor exhibited good selectivity to ethanol and excellent flexibility, maintaining its high performance after bending and tilting up to 5000 times. As this is the first report on flexible self-heated CFO gas sensors, we believe that this research holds great promise for the future development of high-quality sensors based on this approach.

Spatially and Temporally Resolved Dynamic Response of Co-Based Composite Interface during the Oxygen Evolution Reaction.

Interfacial interaction dictates the overall catalytic performance and catalytic behavior rules of the composite catalyst. However, understanding of interfacial active sites at the microscopic scale is still limited. Importantly, identifying the dynamic action mechanism of the "real" active site at the interface necessitates nanoscale, high spatial-time-resolved complementary-operando techniques. In this work, a Co3O4 homojunction with a well-defined interface effect is developed as a model system to explore the spatial-correlation dynamic response of the interface toward oxygen evolution reaction. Quasi in situ scanning transmission electron microscopy-electron energy-loss spectroscopy with high spatial resolution visually confirms the size characteristics of the interface effect in the spatial dimension, showing that the activation of active sites originates from strong interfacial electron interactions at a scale of 3 nm. Multiple time-resolved operando spectroscopy techniques explicitly capture dynamic changes in the adsorption behavior for key reaction intermediates. Combined with density functional theory calculations, we reveal that the dynamic adjustment of multiple adsorption configurations of intermediates by highly activated active sites at the interface facilitates the O-O coupling and *OOH deprotonation processes. The dual dynamic regulation mechanism accelerates the kinetics of oxygen evolution and serves as a pivotal factor in promoting the oxygen evolution activity of the composite structure. The resulting composite catalyst (Co-B@Co3O4/Co3O4 NSs) exhibits an approximately 70-fold turnover frequency and 20-fold mass activity than the monomer structure (Co3O4 NSs) and leads to significant activity (η10 ∼257 mV). The visual complementary analysis of multimodal operando/in situ techniques provides us with a powerful platform to advance our fundamental understanding of interfacial structure-activity relationships in composite structured catalysts.

Spin coating epitaxial heterodimensional tin perovskites for light-emitting diodes.

Environmentally friendly tin (Sn) perovskites have received considerable attention due to their great potential for replacing their toxic lead counterparts in applications of photovoltaics and light-emitting diodes (LEDs). However, the device performance of Sn perovskites lags far behind that of lead perovskites, and the highest reported external quantum efficiencies of near-infrared Sn perovskite LEDs are below 10%. The poor performance stems mainly from the numerous defects within Sn perovskite crystallites and grain boundaries, leading to serious non-radiative recombination. Various epitaxy methods have been introduced to obtain high-quality perovskites, although their sophisticated processes limit the scalable fabrication of functional devices. Here we demonstrate that epitaxial heterodimensional Sn perovskite films can be fabricated using a spin-coating process, and efficient LEDs with an external quantum efficiency of 11.6% can be achieved based on these films. The film is composed of a two-dimensional perovskite layer and a three-dimensional perovskite layer, which is highly ordered and has a well-defined interface with minimal interfacial areas between the different dimensional perovskites. This unique nanostructure is formed through direct spin coating of the perovskite precursor solution with tryptophan and SnF2 additives onto indium tin oxide glass. We believe that our approach will provide new opportunities for further developing high-performance optoelectronic devices based on heterodimensional perovskites.

Molecular insights into the water dissociation and proton dynamics at the β-TaON (100)/water interface.

Understanding the dynamic nature of the semiconductor-water interface is crucial for developing efficient photoelectrochemical water splitting catalysts, as it governs reactivity through charge and mass transport. In this study, we employ ab initio molecular dynamics simulations to investigate the structural and dynamical properties of water at the β-TaON (100) surface. We observed that a well-defined interface is established through the spontaneous dissociation of water and the reorganization of surface chemical bonds. This leads to the formation of a partially hydroxylated surface, accompanied by a strong network of hydrogen bonds at the TaON-water interface. Consequently, various proton transport routes, including the proton transfer through "low-barrier hydrogen bond" path, become active across the interface, dramatically increasing the overall rate of the proton hopping at the interface. Based on our findings, we propose that the observed high photocatalytic activity of TaON-based semiconductors could be attributed to the spontaneous water dissociation and the resulting high proton transfer rate at the interface.

Twinned crystal Cd0.9Zn0.1S/MoO3 nanorod S-scheme heterojunctions as promising photocatalysts for efficient hydrogen evolution.

Leveraging solar energy through photocatalytic hydrogen production from water stands out as one of the most promising approaches to address the energy and environmental challenges. The choice of catalyst profoundly influences the outcomes of photocatalytic reactions, and constructing heterojunctions has emerged as a widely applied strategy to overcome the limitations associated with single-phase photocatalysts. MoO3, renowned for its high chemical stability, encounters issues such as low photocatalytic efficiency and fast recombination of photogenerated electrons and holes. To tackle these challenges, the morphology of MoO3 has been controlled to form nanorods, simultaneously suppressing the aggregation of the catalyst and increasing the number of surface-active sites. Moreover, to facilitate the separation of photogenerated charge carriers, Cd0.9Zn0.1S nanoparticles with a twin crystal structure are deposited on the surface of MoO3, establishing an S-scheme heterojunction. Experimental findings demonstrate that the synergistic effects arising from the well-defined morphology and interface interactions extend the absorption range to visible light response, improve charge transfer activity, and prolong the lifetime of charge carriers. Consequently, Cd0.9Zn0.1S/MoO3 S-scheme heterojunctions exhibit outstanding photocatalytic hydrogen production performance (3909.79 μmol g-1 h-1) under visible light irradiation, surpassing that of MoO3 by nearly nine fold.

Structure, dynamics, and functional properties of hybrid alginate-pectin gels dually crosslinked by Ca2+ and Zn2+ ions designed as a delivery device for self-emulsifying systems for lipophilic phytotherapeutics

Alginate gels are outstanding biomaterials widely applicable in food and pharmaceutical industries. This contribution provides comprehensive insight into the design of advanced hybrid alginate/pectin co-networks double crosslinked by Ca2+/Zn2+ ions encapsulating self-emulsifying systems (SES). The tunable mucoadhesive properties, structural stability, integrity, dissolution profiles, and enhanced in-vivo bioavailability make the synthesized hybrid systems ideal vehicles for the delivery of lipophilic phytotherapeutics, allowing the long-term site-specific treatment of intestinal inflammation. This work also provides a thorough understanding of the structure-property relationships of alginate-pectin gels at the atomic resolution level. It was found out that SES molecules form well-distributed, phase-separated microparticles that interact with the polysaccharide matrix through a well-defined interface. The hybrid alginate-pectin gel is highly cross-linked, with both types of polysaccharides participating in the network formation. The observed surface interactions of SES droplets increase the intrinsic mobility of the network. The plasticizing effect can be regulated by the amount of pectin macromolecules, whose interaction with alginate chains enables a strengthening of the polysaccharide network. Overall, the domain-like architecture of hybrid alginate-pectin gels synthesized by external ionic gelation is revealed; the key structural motifs responsible for their properties are discovered; and the pathways allowing their regulation are identified. Biological in-vivo tests then confirmed positive effects of the synthesized systems in living organisms. The strategy presented thus offers a new perspective for the rational design of alginate-based materials for the microencapsulation of bioactive compounds for advanced orally administered delivery systems or controlled-release decontaminators applicable in the food and nutraceutical processing industries.

Monolayer Organic Crystals for Ultrahigh Performance Molecular Diodes.

Molecular diodes are of considerable interest for the increasing technical demands of device miniaturization. However, the molecular diode performance remains contact-limited, which represents a major challenge for the advancement of rectification ratio and conductance. Here, it is demonstrated that high-quality ultrathin organic semiconductors can be grown on several classes of metal substrates via solution-shearing epitaxy, with a well-controlled number of layers and monolayer single crystal over 1mm. The crystals are atomically smooth and pinhole-free, providing a native interface for high-performance monolayer molecular diodes. As a result, the monolayer molecular diodes show record-high rectification ratio up to 5 × 108 , ideality factor close to unity, aggressive unit conductance over 103 S cm-2 , ultrahigh breakdown electric field, excellent electrical stability, and well-defined contact interface. Large-area monolayer molecular diode arrays with 100% yield and excellent uniformity in the diode metrics are further fabricated. These results suggest that monolayer molecular crystals have great potential to build reliable, high-performance molecular diodes and deeply understand their intrinsic electronic behavior.

Structural, Dielectric, Complex Impedance and Magnetoelectric Properties of the (1-x) KNbO3 - xMgFe2O4 Composites

Ferrite-ferroelectric nanoparticle composites have a promising potential for a wider range of applications for the manufacturing of new-generation devices due to the tenability of their electric and magnetic orders. In this present work, room-temperature magnetoelectric (ME) coupling studies of KNbO3/MgFe2O4 composites having a general formula (1-x) KNbO3 - xMgFe2O4 (where x = 0, 0.1, 0.3, 0.5, 0.7, 0.9, 1) is presented. The presence of the cubic spinel-ferrite phase of MgFe2O4 and the orthorhombic ferroelectric phase of KNbO3 were confirmed by the structural analysis which was employed using X-ray diffraction (XRD), Raman spectroscopy, and morphology and grain size using Transmission electron microscopy (TEM). Magnetization versus magnetic field (M-H) measurements conform to ferromagnetic ordering and show improved magnetization with the increase in the ferrite phase. The existence of coupling between ferroelectric and ferromagnetic ordering was performed using a lock-in amplifier ME measurement setup. All the composite samples show good linear magnetoelectric coupling that increases with increasing ferrite content. This composite nanostructure with a well-defined interface provides the possibility of an ideal model of room temperature ME coupling which is significant from the technological point of view for a variety of miniaturized next-generation device applications. 

Double Bubble Electrospinning: Patents and Nanoscale Interface.

Bipolymeric nanofibers have gained significant attention in various fields due to their enhanced functionality, improved mechanical properties, and controlled release capabilities. However, the fabrication of these composite fibers with a well-defined polymer-polymer interface remains a challenging task. The double bubble electrospinning setup was developed and simulated using Maxwell 3D to analyze the electric field. PVP and PVA polymers were electrospun simultaneously to create bipolymer nanofibers with an interface. The resulting nanofibers were compared with nanofibers made from pure PVA, PVP, and a PVA/PVP blend. The characterization of the nanofibers was performed using scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), and thermogravimetric analysis (TGA). The SEM images showed the formation of PVA/PVP interfacial nanofibers aligned side by side, with a diameter of a few thousand nanometers on each side. By increasing the voltage from 20 kV to 40 kV during electrospinning, the diameter of the nanofibers on the PVA and PVP sides was successfully reduced by 60.8% and 66.3%, respectively. FTIR analysis confirmed the presence of both PVA and PVP in the bipolymeric interfacial nanofibers. TGA analysis demonstrated a weight retention of 14.28% compared to PVA, PVP, and the PVA/PVP blend even after degradation at 500°C. The Maxwell simulation of double bubble electrospinning revealed a stronger and more uniform electric field pattern at 40 kV compared to 20 kV. The study has demonstrated the potential of double bubble electrospinning for the fabrication of bipolymer nanofibers with an interface, opening new avenues for the development of functional nanofibers.

Electrolyte Reactivity on the MgV2O4 Cathode Surface.

Predictive understanding of the molecular interaction of electrolyte ions and solvent molecules and their chemical reactivity on electrodes has been a major challenge but is essential for addressing instabilities and surface passivation that occur at the electrode-electrolyte interface of multivalent magnesium batteries. In this work, the isolated intrinsic reactivities of prominent chemical species present in magnesium bis(trifluoromethanesulfonimide) (Mg(TFSI)2) in diglyme (G2) electrolytes, including ionic (TFSI-, [Mg(TFSI)]+, [Mg(TFSI):G2]+, and [Mg(TFSI):2G2]+) as well as neutral molecules (G2) on a well-defined magnesium vanadate cathode (MgV2O4) surface, have been studied using a combination of first-principles calculations and multimodal spectroscopy analysis. Our calculations show that nonsolvated [Mg(TFSI)]+ is the strongest adsorbing species on the MgV2O4 surface compared with all other ions while partially solvated [Mg(TFSI):G2]+ is the most reactive species. The cleavage of C-S bonds in TFSI- to form CF3- is predicted to be the most desired pathway for all ionic species, which is followed by the cleavage of C-O bonds of G2 to yield CH3+ or OCH3- species. The strong stabilization and electron transfer between ionic electrolyte species and MgV2O4 is found to significantly favor these decomposition reactions on the surface compared with intrinsic gas-phase dissociation. Experimentally, we used state-of-the-art ion soft landing to selectively deposit mass-selected TFSI-, [Mg(TFSI):G2]+, and [Mg(TFSI):2G2]+ on a MgV2O4 thin film to form a well-defined electrolyte-MgV2O4 interface. Analysis of the soft-landed interface using X-ray photoelectron, X-ray absorption near-edge structure, electron energy-loss spectroscopies, as well as transmission electron microscopy confirmed the presence of decomposition species (e.g., MgFx, carbonates) and the higher amount of MgFx with [Mg(TFSI):G2]+ formed in the interfacial region, which corroborates the theoretical observation. Overall, these results indicate that Mg2+ desolvation results in electrolyte decomposition facilitated by surface adsorption, charge transfer, and the formation of passivating fluorides on the MgV2O4 cathode surface. This work provides the first evidence of the primary mechanisms leading to electrolyte decomposition at high-voltage oxide surfaces in multivalent batteries and suggests that the design of new, anodically stable electrolytes must target systems that facilitate cation desolvation.