Interfacial Reaction Mechanism Research Articles

Nano-sized gold particles driven interfacial reaction for the enhanced electrochemical nitrite sensing

Nitrite is a typical food additive and chemical fertilizer, which could pose toxicity to human and aquatic organisms when it is excessive. Therefore, it is meaningful to develop reliable analytical methods for nitrite detection. In this work, an innovative electrochemical nitrite sensor has been fabricated using In2O3 decorated with high-activity nano-sized Au particles (Au/In2O3), which were synthesized through a two-step synthetic method combining hydrothermal reaction and deposition-precipitation, resulting in an excellent sensing performance for the nitrite. Specifically, the electrochemical nitrite sensor based on Au/In2O3 exhibits high sensitivity with a linear detection range from 10 μM to 5 mM at pH 7.38. Additionally, the Au/In2O3 based nitrite sensor shows a detection limit of 0.46 μM and presents impressive selectivity and stability. The extraordinary nitrite sensing performance can be attributed to the excellent catalytic activity of nano-sized Au particles and the strong interfacial reaction between Au/In2O3 and nitrite. Furthermore, theoretical calculations reveal the interfacial reactions mechanism driven by Au particles, which enhance the charge transfer between Au/In2O3 and nitrite and thus improve its electrochemical sensing performance. This work presents a novel approach towards fabricating high-performance electrochemical nitrite sensor and reveals the enhanced interfacial reaction mechanism of nano-sized Au particles.

Electrical monitoring of single-event protonation dynamics at the solid-liquid interface and its regulation by external mechanical forces

Detecting chemical reaction dynamics at solid-liquid interfaces is important for understanding heterogeneous reactions. However, there is a lack of exploration of interface reaction dynamics from the single-molecule perspective, which can reveal the intrinsic reaction mechanism underlying ensemble experiments. Here, single-event protonation reaction dynamics at a solid-liquid interface are studied in-situ using single-molecule junctions. Molecules with amino terminal groups are used to construct single-molecule junctions. An interfacial cationic state present after protonation is discovered. Real-time electrical measurements are used to monitor the reversible reaction between protonated and deprotonated states, thereby revealing the interfacial reaction mechanism through dynamic analysis. The protonation reaction rate constant has a linear positive correlation with proton concentration, whereas the deprotonation reaction rate constant has a linear negative correlation. In addition, external mechanical forces can effectively regulate the protonation reaction process. This work provides a single-molecule perspective for exploring interface science, which will contribute to the development of heterogeneous catalysis and electrochemistry.

Interface Stability and Reaction Mechanisms of Li3YCl5Br with High-Voltage Cathodes and Li Metal Anode: Insights from Ab Initio Simulations.

Recent advancements in battery technology emphasize the critical role of solid electrolytes in enhancing the performance and safety of next-generation batteries. In this study, we investigate the interface stability and reaction mechanisms of Li3YCl5Br, a promising halide-based solid electrolyte, in contact with high-voltage Ni-Mn-Co (NMC) cathodes and a Li metal anode using ab initio molecular dynamics simulations. Our findings reveal that Li3YCl5Br reacts with charged NMC cathodes. This reaction involves changes in the oxidation states of Br- anions in Li3YCl5Br and d-element cations in NMC, as well as the diffusion of Li ions from the solid electrolyte to the cathode to maintain charge balance. The reaction is confined to the interface, suggesting bulk stability. Conversely, the Li/Li3YCl5Br interface exhibits significant instability, with a chemical reaction that results in substantial structural changes and the formation of LiCl and LiBr at the solid electrolyte surface and metallic Y at the Li anode surface. These insights provide valuable information for optimizing interfacial design, aiming at improving the performance and reliability of all-solid-state batteries using halide solid electrolytes.

Gas-liquid interfacial reaction mechanisms of typical small α-dicarbonyls in the neutral and acidic droplets: Implications for secondary organic aerosol formation

Small α-dicarbonyls (SαDs) are well-known as the important precursors of secondary organic aerosol (SOA). Hence, it is imperative to understand the atmospheric chemistry of SαDs to contribute to SOA formation. In this work, we investigated the interfacial chemistry of typical SαDs, including methylglyoxal (MG) and biacetyl (BA) in the neutral and acidic droplets by combined molecular dynamics and quantum chemical calculations. The trans configurations of MG and BA are found to be the favorable configurations at the interfaces and are prone to stay at the gas-liquid interface of the acidic droplet. The C=O group exhibits a preferential uptake orientation towards the interface because the carbonyl-O atom has a strong interaction with interfacial H2O. The uptakes and accumulations of MG and BA at the interfaces are promoted by the acidic condition. Subsequent interfacial hydrations of MG and BA in the acidic droplet are beneficial to yield diols, which can engage in oligomerization in the droplet interior to contribute SOA formation. Our results provide the theoretical insight into the interfacial chemistry of SαDs and their role in SOA formation.

Wetting behavior of Ti-Ni-xNb filler alloy on (HfTaZrNbTi)C high-entropy carbide ceramic

Exploring the wetting behavior of active filler alloys on high-entropy ceramic is critical to clarifying the solid/liquid interface reaction mechanism and guiding the preparation of high-performance composites. The wetting and spreading behaviors of the molten Ti-Ni-xNb filler alloys, both without and with different Nb concentrations, on (HfTaZrNbTi)C high-entropy carbide (HEC) ceramic were investigated at 1330 °C under a vacuum atmosphere using a sessile drop method. The wetting process of the Ti-Ni-xNb filler alloys was characterized by four distinct stages: (i) adhesion stage, (ii) rapid decreasing stage, (iii) sluggish spreading stage, and (iv) final equilibrium stage. The Ti-Ni-xNb filler alloys all exhibited good wettability on the HEC ceramic, with the final contact angle remaining around 47-48°. The interfacial structure was identified as a sequence of HEC/Ti-based HEC’ diffusion layer/TiCx reaction layer/Ti2Ni layer/alloy droplet in all wetting systems. Notably, the introduced Nb element participated in the interfacial reactions between HEC and the filler alloy, modifying the morphology of the solidified droplet and accelerating the rapidly decreasing stage of the alloys on the ceramic. Nb atoms replaced some of the Ti atoms in the TiCx reaction layer, which restrained the atomic diffusion, leading to the formation of thinner reaction layers. The spreading kinetics were initially governed by interfacial reactions and later by the diffusion of Ti and Ni into the ceramic substrate, exhibiting a transition from reaction-controlled to diffusion-controlled spreading.

Interfacial characteristics and thermal stability of polymer-derived SiCf/Ti composite fabricated by powder hot isostatic pressing

The novel SiCf/Ti composite is prepared by hot isostatic pressing (HIP) with polymer-derived (PD) SiC fiber and powder titanium alloy as raw materials in this work. The interfacial characteristics and thermal stability of the PD SiCf/Ti composite have been systematically investigated. The interfacial properties of the PD SiCf/Ti composites are quantified to discuss the interfacial reaction mechanisms and kinetics. The results show that with the proposed HIP process, the powder matrix can be near-fully dense, and the matrix and SiC fiber are well bonded with a uniform interfacial layer. The major interfacial products are C-Ti compounds and Si-Ti compounds, which are formed by atomic diffusion reaction. During subsequent thermal exposure conditions, the interfacial layer growth is temperature-dependent and diffusion-controlled, following the parabolic relation and Arrhenius law. The frequency factor k0 is 102–103 times lower than that in the chemical vapor deposition (CVD) SiCf/Ti composites, showing better interfacial thermal stability. After thermal exposure, the element diffusion becomes significant, and the microhardness of the near-interface zone is noticeably greater than the matrix microhardness because of the atomic diffusion of C. The microhardness of both the matrix and near-interface zone reaches the highest value after 900 °C/9 h thermal exposure. It is concluded that the PD SiCf/Ti composites with good thermal stability can be successfully fabricated by powder HIP.

Influential mechanism of water occurrence states of waste-activated sludge: Specifically focusing on the pore characteristics dominated by cation-organic interactions

The solid pore characteristics are commonly considered as the important influential factors on waste-activated sludge (WAS) dewaterability, and should be related to the cohesive force of bio-flocs dominated by cation-organic interactions at solid-water interface. This study aimed to establish an approach for regulating the solid pore structure of WAS by cationic regulation. The influential mechanism of WAS dewaterability was accordingly explored from the perspective of the pore characteristics dominated by cation-organic interactions. Primarily, with the gradient removal or addition of bivalent cations, the varying pore structure of WAS flocs was tracked by in-situ synchrotron X-ray computed microtomography imaging technique (CMT). The three-dimensional visual model was established to quantify the pore structure parameters of WAS flocs. Following the visualization analysis, the artificial intelligence means, the gradient-weighted class activation mapping (Grad CAM) of three-dimensional convolutional neural network (3D-CNN), was applied for the first time to explore the linkages among solid surface properties, solid pore structure, water occurrence states and sludge dewaterability. It was found that the number and volume of isolated pores jointly determined the mobility and the fractions of vicinal water and interstitial water (p-value ≤ 0.02); also, the decreasing polar or acid-based interfacial free energy with the cationic addition was accompanied with the decreasing isolated pore mean-volume (Pearson coefficient=-0.77, p-value < 0.01). These results indicated that the pore structure characteristics determined the water occurrence states, but the solid porosity strongly depended on the interfacial properties. Accordingly, the molecular docking was applied to explore the interfacial reaction mechanism between Ca2+/Mg2+ and solid compositions in terms of complexation sites, molecular dynamics and free energy calculations. As a result, how the cation-organic interactions affected the pore characteristics through solid surface modification could be clarified, which is expected to serve as theoretical foundation for the development of novel sludge conditioning technologies, i.e., more efforts should be devoted to increasing the dense degree of sludge particles through weakening the hydration repulsion of solid surface.

Nitrogen-doped iron-manganese porous carbon particle electrodes for electrocatalytic degradation of tetracycline: Interfacial reaction mechanisms

In this study, nitrogen-doped porous carbon-supported iron-manganese microspheres (FeMn@NC-700) were successfully synthesized and employed as three-dimensional particle electrodes (3DPE) for electro-oxidative of tetracycline (TCH) in water. FeMn@NC-700 exhibited stable catalytic activity and effective TCH removal capabilities under complex water quality conditions and varying pH levels. Under optimized conditions, the 3D/FeMn@NC-700 system reduced the TCH concentration from an initial 20 mg/L to 0.96 mg/L within 60 min, achieving a 95.23 %removal efficiency with an energy consumption of only 10.05 kWh/m3. The outstanding electrocatalytic activity of the 3D/FeMn@NC-700 system was attributed to the dynamic redox cycling between the Fe and Mn species on the 3DPE surface. Radical quenching experiments and electron paramagnetic resonance (EPR) analysis identified the predominant role of singlet oxygen (1O2), effectively removing TCH with the assistance of hydroxyl radicals (·OH) and superoxide anions (O2·-). The degradation pathways of major intermediate products of TCH were proposed, along with a toxicity assessment. In conclusion, the 3D/FeMn@NC-700 system represents a reliable and cost-effective technology for TCH wastewater treatment.

Advances and Challenges of Porous Structure on Solid–Liquid Interfaces in Polyanionic Sodium‐Ion Batteries

AbstractThe sodium‐ion batteries (SIBs) are expected to be the substitute for lithium‐ion batteries (LIBs) because of their low cost, high abundance, and similar working mechanism. Among them, polyanion‐type electrodes show great application prospects due to their superior ion diffusion channels and structural stability. However, there are still many scientific issues that need to be thoroughly investigated, especially the formation mechanism, structural stability, and interface impedance of solid–liquid interfaces. Therefore, it is of great significance to systematically study the mechanism of interface reaction and the electrochemical behavior, to promote the further practical application of SIBs. Fortunately, the polyanionic electrodes can effectively improve the transport dynamics and the interfacial stability of the solid–liquid interfaces through constructing the porous structure, surface modification, and electrolyte strategies, thus improving the cycle and rate performance. This review discusses the characteristics and formation mechanisms of electrode/electrolyte interface (EEI), as well as their electrochemical behavior in porous structures with different dimensions. Furthermore, this review covers the application of porous materials in improving transport kinetics and EEI. In particular, it highlights the various strategies employed to comprehend the interplay among structure, chemistry, preparation methods, and the mechanisms of porous electrodes that ultimately affect the electrochemical properties of SIBs.

Tracing the Cross‐Talk Phenomenon of Vinylethylene Carbonate to Unveil its Counterintuitive Influence as an Electrolyte Additive on High‐Voltage Lithium‐Ion Batteries

AbstractThe formation of effective interphases is crucial to enable high‐performance lithium‐ion batteries. This can be facilitated by the introduction of electrolyte additives, ensuring improved stability and transport properties. The identification of proper additives requires a comprehensive understanding of the fundamental mechanisms of interfacial reactions governing interphase formation. This study presents a detailed investigation of widely known and less conventional interphase‐forming additives in high‐voltage LiNi0.6Mn0.2Co0.2O2, NMC622||artificial graphite cells. The electrochemical characterization shows that cells containing vinylethylene carbonate (VEC) significantly outperform all other investigated electrolyte formulations. Surprisingly, gas chromatography‐mass spectroscopy measurements of the electrolyte composition after cycling indicate the formation of an ineffective solid‐electrolyte interphase (SEI) in the presence of VEC. A thorough analysis of the interfacial composition via operando shell‐isolated nanoparticle‐enhanced Raman spectroscopy (SHINERS) and surface‐enhanced Raman spectroscopy elucidates rather the formation of an effective cathode‐electrolyte interphase (CEI). This phenomenon results from the reductive reaction of VEC on the anode, followed by the product transfer and electro‐polymerization of reaction products on the cathode. Additionally, focused ion beam secondary ion mass spectrometry (FIB‐SIMS) with a time of flight (ToF)‐detector is used to analyze the elemental spatial distribution of Li‐species and Mn in the respective SEIs.

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.