Interfacial Reaction Mechanism Research Articles

Kinetics of the CH4/O2 reaction over supported palladium catalysts on K-doped manganite perovskite: Impact of potassium on the nature of Pd-support interface and related reaction mechanisms

The kinetics of the CH4/O2 reaction, occurring on post-combustion catalysts to treat the exhaust gases of natural gas-powered engines, has been investigated in lean conditions on model Pd catalysts supported on K-doped LaMnO3. Experimental and predicted reaction rates have been compared according to a single site on Pd active sites and dual site reaction mechanism on active sites located at the Pd-perovskite interface. Comparisons with a benchmark Pd/LaMnO3 emphasized significant changes induced by thermal aging at 750 °C in wet atmosphere (10 vol% H2O in 5 vol% O2). Indeed, the contribution of the single site mechanism grows on aged Pd/LaMnO3 emphasizing a deterioration of the Pd-LaMnO3 interface. The opposite trend is observed on Pd/La1−xKxMnO3 with kinetics obeying to a single site mechanism on pre-reduced catalyst and then shifting to a quasi-exclusive dual site mechanism after aging. Such kinetic features have been discussed with respect to bulk and surface physicochemical characterization pointing out the key role of potassium in the stability of the Pd-support interface.

Interfacial reaction characteristics and mechanisms during dissimilar friction stir lap welding of pure copper and Al0.1CoCrFeNi alloy

In order to explore the weldability and widen the applicability of high entropy alloys (HEAs), dissimilar friction stir lap welding of pure copper and Al0.1CoCrFeNi alloy was investigated in this research. The results indicate that a sound dissimilar weld without tunnels and voids is produced, where a ∼20 μm thick interfacial layer is evident at the Cu-HEA interface. The lap joint is fractured at the upper Cu sheet rather than the lap surface during tensile shear test, suggesting an effective bonding of the dissimilar materials. The lap weld roughly consists of three layers along the plate thickness direction, i.e. welds of Cu, HEA and Cu-HEA interface, respectively. The interface of weld, which has experienced the most severe Cu-HEA interaction during welding, is characterized by uniformly distributed and highly recrystallized ultra-fine grains (∼0.79 μm). Meanwhile, intermetallic compounds particles (Al13Cr2 and Al13Co4) ranging in size of 150∼400 nm are generated at the fine grain boundaries. Fast diffusion of Al, Cr and Co elements and easy segregation of these elements during welding result in the formation of the particles. The sufficient DDRX and the pinning effect of particles are responsible for the formation of ultra-fine grains in the weld interface. The present study lays a theoretical foundation for the joining of conventional Cu and the multi-component HEA, which contributes to the improvement of HEA availability in the field of manufacturing industry.

Interfacial reaction mechanism between Y-containing DD5 alloy and Al2O3 ceramic during directional solidification process

This study systematically investigated the influence of varying yttrium(Y) additions on the interfacial reaction mechanism between the DD5 superalloy melt and Al2O3-based ceramic molds during directional solidification. The analysis revealed the formation of a complex multilayer reaction layer at the alloy-ceramic interface. The interfacial products changed from CaO·6Al2O3 to a mixture of various yttrium oxides after Y was added. As the reaction time increased, the sequence of interfacial reaction products observed on the surface of Y-containing alloys progressed as follows: Y2O3, Y4Al2O9, YAlO3, and ultimately Y3Al5O12. Increasing the Y additions promoted the formation of a reaction layer with a higher atomic percentage of Y. The interfacial reaction process between the DD5 superalloy and Al2O3-based ceramic molds involved ceramic decomposition and diffusion, Y element diffusion and displacement reactions, Al2O3 dissolution and further diffusion of the Al element. This process resulted in the formation of different yttrium-aluminum oxides and related to the bidirectional erosion of the Y2O3. These interfacial reactions significantly contributed to the consumption of Y element within the alloy.

Interaction mechanism between DD5 superalloy with different Y content and ceramic molds with Y2O3 layer

DD5 alloys with different Y content were produced by directional solidification (DS) using ceramic molds with the Y2O3 layer. The interaction mechanisms between the corresponding alloys and the Y2O3 layer were discussed. It was found that the Y2O3 layer effectively hindered the direct contact reaction between the active melt and the Al2O3 ceramics, which was conducive to improving the purity of the melt and reducing the loss of Y. Slight dissolution and decomposition of the Y2O3 layer under high temperature melt erosion resulted in the release of Y and O elements into the alloy. The involvement of Y in the melt changed the interfacial reaction mechanism between the Y2O3 layer and the alloy. The interfacial reaction products of melting the DD5 alloy without Y were Al2Y4O9 and Y2O3, while the interfacial reaction product of melting the DD5 alloy with Y was mainly Y2O3.

Design method of immiscible dissimilar welding (Mg/Fe) based on CALPHAD and thermodynamic modelling

Joining dissimilar metals is a major challenge in joining technology; the weldability of immiscible systems is especially challenging. In this study, a design methodology for dissimilar welding is suggested. The Miedema model and Toop model are developed to calculate the thermodynamics of quaternary alloy systems (Mg-Fe-Al-Cu). Finite element modelling (FEM) of temperature fields and the calculation of phase diagrams (CALPHAD) are combined to provide prerequisite information for modelling. As a test subject, laser welded lap configuration joints of AZ31B magnesium alloy and DP590 steel with a copper coating were put into the design scheme. The interfacial elemental diffusion and formation of intermetallics (IMCs) along the interface during the welding process are predicted. This simulation design scheme predicts the interfacial reaction kinetics and identifies whether the intermediate element works or not. The effects of the Cu coating thickness on the weld constitution, interfacial microstructures and mechanical properties were studied. Cu coating promotes the weld formation fostering the metallurgical reaction of the fusion zone (FZ) with the steel brazing interface. The mechanism of interfacial reactions during the welding-brazing process has been clarified. The Vickers hardness distribution across the interface shows that the Cu-IMCs are ductile.

Atomic-Resolution Interfacial Reaction Mechanism between Bi2Te3-Based Alloys and Ni Electrodes.

Interdiffusion and solid-solid phase reaction at the interface between thermoelectric (TE) materials and the electrode critically influence interfacial transport properties and the overall energy conversion efficiency during service. Here, the microstructural evolution and diffusion mechanisms at the interfaces between the most widely used Bi2Te3-based TE materials, n-type Bi2Te2.7Se0.3 (BTS) and p-type Bi0.5Sb1.5Te3 (BST), and Ni electrodes were investigated at atomic resolution using spherical aberration-corrected scanning transmission electron microscopy (STEM). The BTS(0001)/Ni and BST(0001)/Ni interfaces were constructed by depositing Ni nanoparticles on mechanically exfoliated BTS and BST bulk materials and subsequent annealing. The interfacial reaction is initially dominated by Ni diffusion into the TE matrix to form NiAs-type NiM intermetallics, while Ni trans-quintuple-layer diffusion only occurs in Sb-rich BST. The Bi-rich BTS is more influenced by the Ni-Te preferential reaction, resulting in NiM abnormal grain growth and the formation of tilted and rotated interfaces. Bi diffusion into the BTS matrix forms a Bi double layer at the interface or Bi2[Bi2(Te,Se)3] as the annealing temperature increases, while Bi diffusion into the Ni thin film greatly accelerates the interfacial reaction rate, as elucidated by in situ heating STEM. The results provide essential structural details to understand and prevent the degradation of TE device performance.

Dual electron microregion with oxygen vacancy of Fe0.8La/MCM-48 in bridging peracetic acid and ozonation: Taking the pathway of free radical or nonradical generation?

Efficient tetracycline hydrochloride (TCH) degradation and interface reaction mechanism were investigated by constructing nonradical pathways in heterogeneous peracetic acid coupling with ozonation (O3/PAA) process. Ball-milling assisted Fe–La anchoring MCM-48 catalysts with dual electron microregion was designed to trigger 1O2-dominated non-radical for strong immunity to environment interference. Results exhibited that 83.4% degradation efficiency of TCH was achieved by Fe0.8La/MCM-48/O3/PAA system in only 2 min and 94% TCH was degraded in a 12-hour continuous flow experiment. La with oxygen vacancy regulated the local atomic environment and electron structure of Fe sites, which could initiate peracetic acid activation to promote 1O2 production by surface adsorbed atomic oxygen (*Oad) reaction and this process overcame a lower reaction energy barrier than the binding of surface *Oad to O3. This work offers a reasonable interpretation for Fe–La synergy for inducing non-free radical route, which furnishes theoretical support and practical application for heterogeneous O3/PAA.

Arbitrary Digital DNA Computing: A Programmable Molecular Perceptron Driven by Lambda Exonuclease for Lighting up Concatenated Circuits.

DNA circuits, as a type of biochemical system, have the capability to synchronize the perception of molecular information with a chemical reaction response and directly process the molecular characteristic information in biological activities, making them a crucial area in molecular digital computing and smart bioanalytical applications. Instead of cascading logic gates, the traditional research approach achieves multiple logic operations which limits the scalability of DNA circuits and increases the development costs. Based on the interface reaction mechanism of Lambda exonuclease, the molecular perceptron proposed in this study, with the need for only adjusting weight and bias parameters to alter the corresponding logic expressions, enhances the versatility of the molecular circuits. We also establish a mathematical model and an improved heuristic algorithm for solving weights and bias parameters for arbitrary logic operations. The simulation and FRET experiment results of a series of logic operations demonstrate the universality of molecular perceptron. We hope the proposed molecular perceptron can introduce a new design paradigm for molecular circuits, fostering innovation and development in biomedical research related to biosensing, targeted therapy, and nanomachines.

Surface complexation adsorption of Tl(III) by Fe and Mn (hydr)oxides

Thallium(III) (Tl(III)) is mobile in acidic environments and under ligand complexation, posing a potential threat to the environment and human health. The adsorption of Tl(III) on manganese and iron (hydr)oxides will affect its environmental mobility and engineering removal efficiency. However, the adsorption behavior and interfacial reaction mechanism of Tl(III) remain largely unknown. This study is the first to elucidate the surface complexation mechanism of Tl(III) on Fe/Mn (hydr)oxides and to investigate the adsorption behavior of Tl(III) under the influence of typical environmental ligands. Deprotonation of surface hydroxyl groups contributes to the increase in adsorption capacity for Tl(III) (δ-MnO2, 1619.93 mg g−1; α-FeOOH, 48.25 mg g−1; and α-Fe2O3, 58.66 mg g−1 from Langmuir thermodynamic fitting). Surface complexation modeling reveals tridentate complexation of Tl(III) on birnessite and monodentate complexation on iron (hydr)oxides. The anionic ligand strongly inhibits the adsorption of Tl(III) (up to 16.0 %–40.0 %) by complexing with Tl(III) and occupying the adsorption sites. In addition, HA also reduces the adsorption of Tl(III) by 8.2 %–23.2 % by exacerbating the aggregation and surface coating of the adsorbent particles. New insights into the binding mechanism of Tl(III) on Fe/Mn oxides can help to guide the development of efficient Tl(III) removal adsorbents.

Selective Recovery of Battery-Grade Li2CO3 from Spent NCM Cathode Materials Using a One-Step Method of CO2 Carbonation Recovery Without Acids or Bases.

The recovery of spent lithium-ion batteries by traditional acid leaching is limited by serious pollution, complicated technology, and the low purity of Li2CO3. To address the problems of the traditional acid leaching process and increasing demand for decarbonization, a technique for the selective carbonation leaching of Li and the recovery of battery-grade Li2CO3 by a simple concentration precipitation process without acids or bases was developed. The coupling of CO2 and reducing agents could effectively promote the precipitation of MCO3 (M=Ni/Co/Mn) and the selective leaching of Li by decreasing the reducing capability needed for transition metals and decreasing the pH of the solution. The optimal selective leaching process of Li was obtained under 1 MPa CO2 with 20 g/L Na2S2O3 at an L/S ratio of 30 mL/g for 1.5 h. FT-IR, XRD, ICP-MS and other methods were used to reveal the multiphase interfacial reaction mechanism of the carbonation reduction of layered cathode materials, which indicated that the reducing agent Na2S2O3 could promote lattice distortion of the cathode materials and effective separation of Li. In summary, a green and economical method for the selective recovery of battery-grade Li2CO3 using a one-step method of CO2 carbonation recovery in a near-neutral environment was proposed.

Interfacial Metal-Support Interaction and Catalytic Performance of Perovskite LaCrO3-Supported Ru Catalyst.

Interfacial metal-support interaction (MSI) significantly affects the dispersion of active metals on the surface of the catalyst support and impacts catalyst performance. Understanding MSI is crucial for developing highly active and stable catalysts with a low metal loading, particularly for noble metal catalysts. In this work, we synthesized LaRuxCr1-xO3 catalysts with low Ru loading (x = 0.005, 0.01, and 0.02) using the sol-gel self-combustion method. We found that all of the Ru atoms immediately above or below the metal-support interface are closely bonded to the perovskite LaCrO3 surface lattice through Ru-O bonds, enhancing the MSI via interfacial reaction and charge transfer mechanisms. We identified a variety of Ru species, including small 3D Ru nanoparticles, 2D dispersed Ru surface atoms, and even 0D Ru single atoms. These highly dispersed Ru species exhibit high activity and stability under dry reforming of methane (DRM) conditions. The LaRu0.01Cr0.99O3 catalyst with very low Ru loading (0.42 wt %) was stable over a 50 h DRM test and the carbon deposition was negligible. The CH4 and CO2 conversions at 750 °C reached 83 and 86%, respectively, approaching the theoretical thermodynamic equilibrium values.

Cobalt single-atom catalyst tailored ceramic membrane for selective removal of emerging organic contaminants

Water reuse is an effective way to solve the issues of current wastewater increments and water resource scarcity. Ultrafiltration, a promising method for water reuse, has the characteristics of low energy consumption, easy operation, and high adaptability to coupling with other water treatment processes. However, emerging organic contaminants (EOCs) in municipal wastewater cannot be effectively intercepted by ultrafiltration, which poses significant challenges to the effluent quality and sustainability of ultrafiltration process. Here, we develop a cobalt single-atom catalyst-tailored ceramic membrane (Co1-NCNT-CM) in conjunction with an activated peroxymonosulfate (PMS) system, achieving excellent EOCs degradation and anti-fouling performance. An interfacial reaction mechanism effectively mitigates membrane fouling through a repulsive interaction with natural organic matter. The generation of singlet oxygen at the Co-N3-C active sites through a catalytic pathway (PMS→PMS∗→OH∗→O∗→OO∗→1O2) exhibits selective oxidation of phenols and sulfonamides, achieving >90% removal rates. Our findings elucidate a multi-layered functional architecture within the Co1-NCNT-CM/PMS system, responsible for its superior performance in organic decontamination and membrane maintenance during secondary effluent treatment. It highlights the power of integrating Co1-NCNT-CM/PMS systems in advanced wastewater treatment frameworks, specifically for targeted EOCs removal, heralding a new direction for sustainable water management.

Carbon structural evolution and interfacial reaction mechanism investigation of the green anode in kneading and baking via ReaxFF-MD and force-biased Monte Carlo

ABSTRACT Baking is the most costly and critical process in anode preparation, and the study from the microscopic scale is conducive to the optimisation of anode baking process. In this research, a hybrid simulation method of reactive force field molecular dynamics (ReaxFF-MD) and force-biased Monte Carlo (fbMC) was proposed to understand the interaction mechanism between coal tar pitch (CTP) and calcined petroleum coke (CPC) during kneading and baking processes, and to explore the optimal ratio of CTP from the molecular scale. Results showed that the CTP content of 14 wt.% was beneficial for anode production. The mechanism of anode coking behaviour at high temperatures was also analyzed. The carbonisation of CTP during high-temperature baking broke the carbon rings and formed straight chains, exposing active carbon atoms that can bond with the remaining layers. As the high-temperature simulation progresses, the carbon chains at the bonding sites became increasingly cyclized and aromatised, which made the layered structure of the baked block similar to that of graphite. The generation of various volatile hydrocarbons during the baking process was observed, namely CH4, C2H4, C2H2, C2H6, and C3H6. This work provides theoretical basis for process optimisation.

Surface Decoration of TiC Nanocrystals onto the Graphite Anode Enables Fast-Charging Lithium-Ion Batteries.

To significantly reduce the charging time of commercial lithium-ion batteries (LIBs), it is essential to control the surface properties of graphite anodes because the charging process involves sluggish interfacial kinetics between graphite and the electrolyte. For the effective surface modification of graphite, herein we demonstrate the surface decoration with titanium carbide (TiC) nanocrystals onto graphite particles via a simple wet-coating process. The high electrical conductivity, low Li+ adsorption energy, and small surface diffusion barrier of the TiC nanocrystals facilitate fast Li+ adsorption and migration in the graphite surface by reducing the overpotential upon the charging process. The feasibility of the TiC nanocrystal-decorated graphite (TiC@AG) anode is thoroughly examined with an in-depth understanding of the interfacial reaction mechanism. Furthermore, the full-cell with a commercial cathode (LiNi0.8Co0.1Mn0.1O2) and TiC@AG anode demonstrates an impressive capacity retention (94.5%) after 300 cycles under fast-charging condition (3 C-charging and 1 C-discharging) without any sign of Li plating. The charging time of the TiC@AG full-cell was estimated at 16.2 min (80% of state of charge), which is substantially shorter than that of the artificial graphite full-cell. Our findings offer practical insights into the design principles of advanced graphite anodes, contributing to the realization of fast-charging LIBs.

Interfacial polymerization mechanisms assisted flame retardancy process of low-flammable electrolytes on lithium anode

Thermal runaway is a hazardous risk, occurring more readily in high-energy–density lithium-ion batteries (LIBs), which leads to a rapid temperature rise and even combustion or explosion when using flammable electrolyte systems. Flame retardants (FRs), such as trimethyl phosphate (TMPa) and triethyl phosphate (TEP), are commonly utilized due to their effective flame suppression, low toxicity, and excellent thermal stability. However, the lack of in-depth understanding of the flame retardancy mechanism and solid electrolyte interphase (SEI) formation process has made the development of functional electrolytes difficult at present. In this study, we clarified the flame retardancy and interfacial reaction mechanisms of low-flammable TMPa localized high-concentration electrolytes (LHCE) using hybrid ab initio and reactive force field (HAIR) schemes. Long-term HAIR simulation reveals that phosphorous radicals produced by the decomposition of TMPa capture carbon radicals, encouraging their polymerization into low-flammable oligomers, while fluorine-containing solvents in the electrolyte capture hydrogen radicals and produce nonflammable hydrofluoric acid (HF). This synergistic flame retardancy mechanism provides essential atomic-level insights for the rational design of high-safety electrolytes in the future.

In-situ surface enhanced Raman spectroscopy revealing the role of metal–organic frameworks on photocatalytic reaction selectivity on highly sensitive and durable Cu-CuBr substrate

Photocatalytic reactions using copper-based nanomaterials have emerged as a new paradigm in green technology. Selective photocatalysis is very important for improving energy utilization efficiency, and in order to directional improve catalytic selectivity, it is necessary to understand the mechanism of interfacial reactions at the molecular level. Therefore, a unique bifunctional Cu-CuBr substrate is first fabricated via an electrochemical method, which overcomes the instability of traditional copper-based materials and endows high surface-enhanced Raman spectroscopy (SERS) sensitivity and photocatalytic performance and can be stored stably for more than a year. Further modification of the surface with Metal-Organic Frameworks (MOFs) containing carboxyl functional groups can significantly tune the surface properties of the substrate. This increases the adsorption of cationic dyes to improve the SERS effect, and 10−10 M methylene blue can easily be detected with this substrate. Surprisingly, in-situ SERS monitoring of the interfacial photocatalytic dehalogenation reaction of aromatic halides through its intrinsic SERS effect reveal two competing selective reaction pathways, self-coupling and hydrogenation. Typically, the SERS spectra reveal that the latter's selectivity was greatly enhanced after MOFs modification, and the yield rate of the hydrogenated product increased from 27.6 % to 46.9 % (selectivity increased from 32.7 % to 51.5 %). This proves that the surface properties of catalysts, especially the affinity for reaction intermediates, can effectively regulate catalytic selectivity.

Enhancing SERS Sensitivity in N‐Graphene Hydrangea by Synergistic Charge‐Transfer and Excitation Light Absorption

Surface‐enhanced Raman scattering (SERS) is a versatile spectroscopic technique, which plays a crucial role in enhancing analytical sensitivity, investigating interfacial reaction mechanisms, enabling biosensing, and fostering efficient catalysis. Currently, the common SERS substrates are primarily metal nanostructures, which entail high manufacturing costs, complex processes, and the metal surface undergo change over time and with environmental conditions. These issues limit the development of SERS technology. In this work, a nitrogen‐doped graphene (N‐graphene) hydrangea was synthesized on a silicon (Si) substrate using plasma‐assisted chemical vapor deposition (PACVD), forming an N‐graphene hydrangea/Si hybrid structure as a SERS substrate. This substrate offers the advantages of high stability, ultra‐sensitivity, and reusability. The three‐dimensional nano‐cavity structure of graphene can increase the interaction between light and graphene, resulting in an increased localized electric field. Combining theoretical simulation analysis, the introduction of nitrogen (N) elements adjusts the Fermi level of graphene, promoting efficient charge transfer. In practical scenarios, Di(2‐ethylhexyl) phthalate (DEHP), a commonly used plasticizer, has raised concerns due to its potential as an endocrine disruptor and carcinogen. The as‐prepared SERS substrate achieves a remarkable detection limit of as low as 10−8 m for DEHP, providing significant support for environmental conservation and human health.

Porous‐structured vermiculite/polybutylene adipate terephthalate composite films: The morphology, mechanical properties, and nonisothermal degradation kinetics

AbstractTo examine the impact of vermiculite (VMT) on the environmental and physical aspects of polybutylene terephthalate (PBAT), the thermal degradation behavior of VMT/polybutylene terephthalate polyadipate (VMT/PBAT) composite films was investigated by using the thermogravimetric analysis (TGA). To ensure precise calculation of the specific activation energy values of VMT/PBAT composite films in thermal degradation performance experiments, the Kissinger method (K‐method) and Flynn–Wall–Ozawa method (FWO method) were utilized. Additionally, the reaction mechanism was analyzed using the Coats–Redfern equation (CR equation). The introduction of VMT into the PBAT co‐polyester structure leads to an increase in the thermal degradation activation energy Ek of composite films.; the apparent activation energies were calculated by the Coats–Redfern method for different reaction mechanisms, and the interfacial diffusion reaction mechanism of the composite film was determined, with a thermal degradation reaction principle properties of g(α) = [1 − (1 − α)]2 and the number of reaction steps of 2.Highlights VMT/PBAT composite films prepared using a simple method. Analyzing nonisothermal degradation kinetics using K‐method and FWO method. Analyzing the degradation mechanisms using the Coats–Redfern equation. Addition of VMT enhances the thermal degradation properties of composite films. Addition of VMT reduces the mechanical properties of the composite film.

Photocatalytic NO x removal and recovery: progress, challenges and future perspectives.

The excessive production of nitrogen oxides (NO x ) from energy production, agricultural activities, transportation, and other human activities remains a pressing issue in atmospheric environment management. NO x serves both as a significant pollutant and a potential feedstock for energy carriers. Photocatalytic technology for NO x removal and recovery has received widespread attention and has experienced rapid development in recent years owing to its environmental friendliness, mild reaction conditions, and high efficiency. This review systematically summarizes the recent advances in photocatalytic removal, encompassing NO x oxidation removal (including single and synergistic removal and NO3 - decomposition), NO x reduction to N2, and the emergent NO x upcycling into green ammonia. Special focus is given to the molecular understanding of the interfacial nitrogen-associated reaction mechanisms and their regulation pathways. Finally, the status and the challenges of photocatalytic NO x removal and recovery are critically discussed and future outlooks are proposed for their potential practical application.

Crystal Orientation-Dependent Interface Compatibility in the Oxide Composite Cathode by in Situ Heating Transmission Electron Microscopy

All-solid-state batteries (ASSBs) with oxide-based solid electrolytes are getting prominence as a forthcoming battery system capable of overcoming the drawbacks of current lithium-ion batteries by satisfying the expanding demand for high energy density and safety. However, the poor interfacial contact between cathode active materials and solid electrolytes, at which lithium ions diffuse and the charge transfer occurs, is a major concern for practical utilization. Although the co-sintering process at high temperatures is essential to achieve an intimate interface contact, excessive thermal energy reversely accelerates the interfacial degradation reaction, of which the mechanism has been still unexplored. Here, using an epitaxial model system in which the crystal orientations of the Li(Ni1/3Co1/3Mn1/3)O2 cathode and Li3xLa(2/3)-x⎕(1/3)-2xTiO3 solid electrolyte are controlled, we directly probe the interfacial reaction in real-time during heating by in situ heating transmission electron microscopy, and investigate the impact of the crystal orientation at the interface on the interfacial reaction mechanism and kinetics. In situ observation reveals that the interfacial reactions are highly dependent on the crystal orientation at the interface involving the onset temperature of the reaction, the diffusion behavior of lithium ions, the intermediate states, and the overall degradation mechanism between the active material and the solid electrolyte. The interfacial degradation during heating increases the charge transfer resistance between the cathode active material and the solid electrolyte, and the increasing tendency of the resistance is closely related to the crystal orientation-dependent interfacial degradation.