High Ion Research Articles

A Novel Hydrated Iron Vanadate Cathode Material for Advanced Aqueous Nickel-Ion Batteries.

Aqueous nickel-ion batteries (ANIBs) as an emerging energy storage device attracted much attention owing to their multielectron redox reaction and dendrite-free Ni anode, yet their development is hindered by the divalent properties of Ni2+ and the lack of suitable cathode materials. Herein, a hydrated iron vanadate (Fe2V3O10.5∙1.5H2O, FOH) with a preferred orientation along the (200) plane is innovatively proposed and used as cathode material for ANIBs. The FOH cathode exhibits a remarkable capacity of 129.3 mAh g-1 at 50mA g-1 and a super-high capacity retention of 95% at 500mA g-1 after 700 cycles. The desirable Ni2+ storage capacity of FOH can be attributed to the preferentially oriented and tunnel structures, which offer abundant reaction active planes and a broad Ni2+ diffusion path, the abundant vacancies and high specific surface area further increase ion storage sites and accelerate ion diffusion in the FOH lattice. Furthermore, the Ni2+ storage mechanism and structural evolution in the FOH cathode are explored through ex situ XRD, ex situ Raman, ex situ XPS and other ex situ characteristics. This work opens a new way for designing novel cathode materials to promote the development of ANIBs.

Determination of High Concentration Copper Ions Based on Ultraviolet—Visible Spectroscopy Combined with Partial Least Squares Regression Analysis

With the rapid development of industrialization, the problem of concentration determination based on the copper production process has been widely concerned, and the accurate determination of high-concentration copper ions (Cu2+) is of great significance for enterprise production, resource utilization, and pollution prevention. The characteristics of different spectrophotometric methods for the determination of Cu2+ are discussed, and it is found that these methods are suitable for the determination of trace or low concentration of Cu2+ (0.5 μg/L–5 mg/L), whereas for the determination of high Cu2+ concentration pre-treatments such as dilution, complexation, and coloring are required. In this study, a method based on ultraviolet-visible spectroscopy (UV-Vis) combined with partial least squares regression analysis (PLS) was proposed for the determination of high copper ions (>100 mg/L), which performs rapid and accurate determination of high Cu2+ concentration by preprocessing and feature extraction of UV-Vis spectral data, followed by model construction with PLS analysis, which is easy to operate and applicable to a wide range of concentrations. The correlation coefficient (R2), mean relative error (MRE), and root mean square error (RMSECV) of the model prediction of Cu2+ concentrations were 0.99946, 0.006343, and 11.237 mg/L, respectively, indicating that the accuracy of the model prediction is very high. This study not only provides an efficient method for the precise determination of high Cu2+ concentration but also enables the simultaneous determination of Cu2+, Co2+, and Ni2+ ions, which provides a new technical means for environmental monitoring and pollution prevention.

Chaotropic Ions Mediated Polymer Gelation for Thermal Management.

Energy and environmental issues have increasingly garnered significant attention for sustainable development. Flexible and shape-stable phase change materials display great potential in regulation of environmental temperature for energy saving and human comfort. Here, inspired by the water absorption behavior of salt-tolerant animals and plants in salinity environment and the Hofmeister theory, highly stable phase change salogels (PCSGs) are fabricated through in situ polymerization of hydrophilic monomers in molten salt hydrates, which can serve multiple functions including thermal management patches, smart windows, and ice blocking coatings. The gelation principles of the polymer in high ion concentration solution are explored through the density functional theory simulation and verified the feasibility of four types of salt hydrates. The high concentration chaotropic ions strongly interacted with polymer chains and promoted the gelation at low polymer concentrations which derive highly-stable and ultra-moisturizing PCSGs with high latent heat (> 200 J g-1). The synergistic adhesion and transparency switching abilities accompanied with phase transition enable their smart thermal management. The study resolves the melting leakage and thermal cycling stability of salt hydrates, and open an avenue to fabricate flexible PCM of low cost, high latent heat, and long-term durability for energy-saving, ice-blocking, and thermal management.

Ultrathin Ionic Diodes with Electrostatically Heterogeneous Hybrid Interfaces of Nanoporous SiO2 Nanofilms and Polymer Layer-by-Layer Multilayers.

Nanofluidic ionic diodes have attracted much attention due to their unique functions as unidirectional ion transportation ability and promising applications from molecular sensing, and energy harvesting to emerging neuromorphic devices. However, it remains a challenge to fabricate diode-like nanofluidic systems with ultrathin film thickness <100nm. Herein the formation of ultrathin ionic diodes from hybrid nanoassemblies of nanoporous (NP) SiO2 nanofilms and polyelectrolyte layer-by-layer (LbL) multilayers is described. Ultrathin ionic diodes are prepared by integrating polyelectrolyte multilayers onto photo-oxidized NP SiO2 nanofilms obtained from silsesquioxane-containing block copolymer thin films as a template. The obtained ultrathin ionic diodes exhibit ion current rectification (ICR) properties with high ICR factor = ≈20 under low ionic strength and asymmetric pH conditions. It is concluded that this ICR behavior arises from effective ion accumulation and depletion at the interface of NP SiO2 nanofilms and LbL multilayers attributed to high ion selectivity by combining the experimental data and theoretical calculations using finite element methods. These results demonstrate that the hybrid nano assemblies of NP SiO2 nanofilms and polyelectrolyte LbL multilayers have potential applications for (bio)sensing materials and integrated ionic circuits for seamless connection of human-machine interfaces.

Modeling Ionized Gas in the Small Magellanic Cloud: The Wolf–Rayet Nebula N76

We present Cloudy modeling of infrared emission lines in the Wolf–Rayet (WR) nebula N76 caused by one of the most luminous and hottest WR stars in the low metallicity Small Magellanic Cloud. We use spatially resolved mid-infrared Spitzer/InfRared Spectrograph and far-infrared Herschel/PACS spectroscopy to establish the physical conditions of the ionized gas. The spatially resolved distribution of the emission allows us to constrain properties much more accurately than using spatially integrated quantities. We construct models with a range of constant hydrogen densities between nH = 4–10 cm−3 and a stellar wind-blown cavity of 10 pc, which reproduces the intensity and shape of most ionized gas emission lines, including the high ionization lines [O iv] and [Ne v], as well as [S iii], [S iv], [O iii], and [Ne iii]. Our models suggest that the majority of [Si ii] emission (91%) is produced at the edge of the H ii region around the transition between ionized and atomic gas while very little of the [C ii] (<5%) is associated with the ionized gas. The physical conditions of N76 are characterized by a hot HII region with a maximum electron temperature of T e ∼ 24,000 K, electron densities that range from n e ∼ 4 to 12 cm−3, and high ionization parameters of log(U)∼−1.15to−1.77. By analyzing a low-metallicity WR nebula with a single ionization source, this work gives valuable insights into the impact WR stars have on the galaxy-integrated ionized gas properties in nearby dwarf galaxies.

All solid-state lithium-ion batteries based on designed polyrotaxane-containing networks

Selecting the appropriate polymer structure for use as both a solid electrolyte and catholyte is essential for enhancing the electrochemical performance of all-solid-state lithium metal batteries. In this study, we are pioneering the customization of solid electrolyte and catholyte synthesis based on novel polyrotaxane (PRX)-containing polymer networks by altering the length of the polyether crosslinkers to tune the properties to meet specific needs of different components. On one hand, the modified PRX polymer networks based on the shorter crosslinker show good mechanical strength, high ionic conductivity (7.25 × 10−4 S cm−1) and high lithium ions transference number (0.54) at 60 °C, allowing their use as solid polymer electrolyte (SPE) self-supporting membranes. On the other hand, all-solid-state lithium-ion batteries with this SPE demonstrate a much higher initial capacity (above 160 mAh/g using LiFePO4 as active material at the cathode and lithium metal as anode), and better cycling performance when paired with longer cross-linked PRX as catholytes than the other non-customized combinations all solid lithium-ion batteries. Moreover, the cycling performance of the full cell can be further improved by incorporating different lithium salts in the electrolyte (LiTFSI) and cathode (LiClO4). This work highlights that the customized design of solid electrolytes and catholytes based on polymer networks is an efficient strategy to obtain high-performance all-solid-state lithium metal batteries

Tuning the microstructure of biomass-derived hard carbons by controlling the impurity removal process for enhanced Na ion storage performance

Biomass-derived hard carbons are promising anode materials of sodium-ion batteries (SIBs) due to their low cost, renewability and high specific capacity. However, there are inevitably some impurities in biomasses that may not only affect the purity, but microstructure and electrochemical performance of hard carbons. Although the impurities can be removed by appropriate treatments after carbonization, the microstructure of hard carbons can hardly be changed. In this work, taking ficus macrophylla leaves (FMLs) as the model biomass, the effects of impurities and their removing process on the microstructure and Na ion storage performance of hard carbons are investigated. It is found that the presence of Ca and Si-bearing impurities in FMLs results in more graphite-like structure in hard carbons because of their catalytic graphitization effect. The acid and base washing processes after carbonization can mostly get rid of the inorganic impurities is unable to increase the plateau region capacities associating to Na ion insertion in the interlayer of graphitic microcrystals and Na metal filling in micropores. By contrast, by stepwisely removing the Ca and Si-bearing impurities from raw materials before carbonization, hard carbons with high purity, larger interlayer space and more micropores are produced, which exhibit a high reversible specific capacity of 336 mAh g−1 at 20 mA g−1, a high initial Coulombic efficiency of 93 %, excellent rate capability (245 mAh g−1 at 2 A g−1) and robust cycle stability. This study implies that controlling the impurity removal process can simultaneously tune the microstructure of hard carbon anodes derived from biomasses towards high performance Na ion storage.

High performance rechargeable aluminium ion batteries enabled by full utilization and understanding of polyaniline cathodes

As a renowned conductive polymer, polyaniline (PANI) shows remarkable potential in organic cathode materials for rechargeable aluminium ion batteries (RAIBs). However, existing research has not given sufficient understanding and explanation of the structure and states of PANI but failed to achieve ideal electrochemical performance. In this study, we differentiate and investigate for the first time its primary-doped (PANI-1), re-doped (PANI-Re), secondary-doped (PANI-2), and emeraldine based (PANI-EB) forms, meanwhile attempt to enhance the conductivity of PANI-EB using multi-walled carbon nanotubes (PANI-EB@C). Among them, the high-doped PANI-2 and non-doped PANI-EB exhibit theoretical capacity utilization far superior to lower doped PANI-1 and PANI-Re, with both specific capacities reaching approximately 225 mAh/g (full capacity utilization rate of 76.53 %) at a current density of 1 A/g, while maintaining capacity retention rates of 92.89 % after 2000 cycles and 92.44 % after 5000 cycles, respectively. Furthermore, the high-conductivity PANI-EB@C displays a discharge specific capacity of 284 mAh/g (full capacity utilization rate of 96.59 %), with a capacity retention rate of 91.19 % after 5000 cycles. Electrochemical analysis, Gaussian theoretical calculations, ex-situ characterization collectively indicate that the electrochemical performance of doped PANI is positively correlated with the degree of doping-induced conductivity changes, while the unique internal redox process of PANI-EB enhances the release of performance and could be further optimized by the assistant of conductivity medium. This work advances the classification of the electrochemical performance and structural understanding of PANI cathode materials to an extremely high stage, towards the practical application of a low-cost, high-performance, sustainable, and green cathode material in large-scale energy storage devices.

Zwitterionic channels within covalent organic frameworks facilitate proton-selective transport for flow battery membrane

Flow batteries demand for ion conductive membranes (ICMs) with high ion selectivity to achieve efficient energy conversion. Herein, we engineered a cysteine-modified covalent organic framework (Cys-COF) by a Thiol-ene click reaction. As a promising proton carrier, the incorporation of the Cys-COF with sulfonated poly(ether ketone) (SPEEK) yields advanced ICMs for vanadium flow batteries (VFBs). The zwitterionic cysteine groups anchored on the nanochannel walls simultaneously narrowed the pore size and ameliorated the protophilicity of Cys-COF, resulting in improved vanadium permeating resistance and proton conductivity. As a result, the optimal membrane demonstrated synchronized improvements in coulombic efficiency (95.01 %-98.84 %), voltage efficiency (95.15 %–77.84 %) and energy efficiency (90.41 %–76.94 %) with the current densities ranging from 40 to 200 mA cm−2. Regarding stability test, it achieved exceptional energy efficiency (∼84.3 %) over 1100 cycles and 550 h at the constant current density of 120 mA cm−2, outperforming pure polymer membrane and Nafion 212.

Self‐Supporting Solid Electrolyte Based on Supramolecular Interaction for Stable Li Metal Batteries

AbstractLi metal batteries based on solid polymer electrolytes offer the benefits of high energy density and safety, as well as extended cycling life, making them an excellent candidate for the next‐generation battery system. However, current solid polymer electrolytes still suffer from low ion conductivity and Li+ transfer number, which seriously restricts its practical application. Herein, a self‐supporting composite solid polymer electrolyte was prepared, where phenolic resin rich in hydroxyl groups (BR) and polyethylene oxide (PEO) are mixed evenly and poured onto a cellulose membrane in one step. In such an electrolyte, PEO and BR combine to form intermolecular hydrogen bonds, lowering the crystallinity of PEO and increasing the Li+ transfer number. Lastly, the obtained solid electrolytes exhibited a high ion conductivity (1.1×10−4 S cm−1) and Li+ transfer number (0.53), as well as improved electrochemical window. Consequently, Li || Li symmetrical cells can run stably for more than 700 h at 0.1 mA cm−2/0.25 mAh cm−2. And full cells with LiFePO4 cathode can also demonstrate high discharge capacity of 152.12 mAh g−1 and rate performance. We believe that such a design based on supramolecular interaction offer a new avenue to advanced solid polymer electrolytes.

Optimizing Nanofluidic Energy Harvesting in Synthetic Clay-based Membranes by Annealing Treatment.

Nanofluidic energy harvesting from salinity gradients is studied in 2D nanomaterials-based membranes with promising performance as high ion selectivity and fast ion transport. In addition, moving forward to scalable, feasible systems requires environmentally friendly materials to make the application sustainable. Clay-based membranes are attractive for being environmentally friendly, non-hazardous, and easy to manipulate materials. However, achieving underwater stability for clay-based membranes remains challenging. In this work, the synthetic clay Laponite is used to prepare clay-based membranes with high stability and excellent performance for osmotic energy harvesting. The Laponite membranes (Lap-membranes) are stabilized by low-temperature annealing treatment to effectively reduce the interlayer space, achieving a continuous operation under salinity gradients. Furthermore, the Lap-membranes conserve integrity while soaking in water for more than one month. The output power density improves from ≈4.97W m-2 on the pristine membrane to ≈9.89W m-2 in the membrane treated 12 h at 300°C from a 30-fold concentration gradient. Especially, It is found that the presence of interlayer water to be favorable for ion transport. Different mechanisms are proposed in the Lap-membranes involved for efficient ion selectivity and the states found with varying annealing temperatures. This work demonstrates the potential application of Laponite based nanomaterials for nanofluidic energy harvesting.

Synthesis and electrochemical properties of activated lignite carbons-reduced graphene oxide nanocomposites symmetric supercapacitors

Ultra-fast chargeable or rechargeable symmetric carbon-based supercapacitors (SCSs) with high capacity, inexpensive, and non-flammability have attracted much attention for electronics and energy storage devices. However, improving both high redox reaction and ion transport/diffusion processes by enhancing high energy storage performance and rapid ion/electron transport SCSs electrode materials remains challenging. Herein, we presented a successful preparation of activated lignite carbons-reduced graphene oxide (ALC-rGO) nanocomposite (NCp) with the ALC:rGO ratio of 80:20 wt% by a one-pot hydrothermal for high electrochemical performance. Importantly, the matrix of ALC-rGO NCp was primary amorphous carbon with hexagonal graphitic layers and pore structures of plentiful micropores and mesopores. Remarkably, the ALC-rGO NCp electrode exhibited a maximum specific capacitance (Csc) of 152.12 F/g at 0.5 A/g. Interestingly, the SCSs-ACL-rGO device could illustrate a good performance at a potential voltage of 1.8 V with Csc of 50.90 F/g at 1 A/g and capacity retention of 96.0 % at 5 A/g after 2,000 cycles GCD test.

Stretchable interconnected modular electrochromic devices enabled by self-healing, self-adhesive, and ion-conducting polymer electrolyte

Here, we propose a versatile terpolymer electrolyte material, UPy-PEGMA-VBMI, comprised of three monomers: ureidopyrimidinone methacrylate (UPyMA), poly(ethylene glycol) methacrylate (PEGMA), and vinyl benzyl-methylimidazolium (VBMI). The UPy-PEGMA-VBMI, supported by a combination of soft ethylene glycol chains, an ion-conducting imidazole unit, and self-complementary quadruple hydrogen bonds of UPy, exhibits exceptional properties such as high stretchability, rapid self-repair, solution processability, self-adhesion, and ion conduction. The UPy-PEGMA-VBMI was then applied to make ion gel composite films, demonstrating a notable ionic conductivity of 3.84 × 10−3 S cm−1 while maintaining robust stretching and adhesive characteristics. The electrochromic devices (ECDs) fabricated by this ion gel demonstrate outstanding performance, with fast switching times, long-term kinetic stability, and extraordinarily high coloration efficiency of 443.83 cm2 C−1. The stretchable ECDs are fabricated by utilizing the stretchable nature of UPy-PEGMA-VBMI, exhibiting a transmittance contrast of 42.7 % at an extension of 53 % and operational stability during stretching cycles. Moreover, self-healing and self-adhesive features enable the fabrication of interconnected modular ECDs, implementing area-scalable devices. These modular ECDs, each powered independently, provide arbitrary positioning and shifting of individual device patches, overcoming the performance limitations of conventional large-area devices. The unprecedented material and resulting devices open new possibilities for electrochromic applications, particularly in stretchable ECDs, pattern-switching devices, and scalable flexible ECDs.

Three neo-Clerodane Diterpenoids from Tinospora cordifolia Stems and Their Arginase Inhibitory Activities.

Three neo-clerodane diterpenoids, including two new tinocordifoliols A (1) and B (2) and one known tinopanoid R (3), were isolated from the ethyl acetate-soluble fraction of the 70% ethanol extract of Tinospora cordifolia stems. The structures were elucidated by various spectroscopic methods, including one dimensional (1D) and 2D-NMR, high resolution-electrospray ionization (HR-ESI)-MS, and electronic circular dichroism (ECD) data. The T. cordifolia extract and all isolated compounds 1-3 possessed arginase I inhibitory activities. Among them, 3 exhibited moderate competitive inhibition of human arginase I (IC50 = 61.9 µM). Furthermore, docking studies revealed that the presence of a β-substituted furan in 3 may play a key role in the arginase I inhibitory activities.

Multiple-functional LiTi2(PO4)3 modification improving long-term performances of Li-rich Mn-based cathode material for advanced lithium-ion batteries

Li-rich layered oxides with high energy densities have become one kind of promising cathode for advanced lithium-ion batteries, however some issues are severely hindering their practical applications. To address these challenges, fast ion conductive LiTi2(PO4)3 (LTPO) is employed to modify the typical Li-rich cathode Li1·2Mn0·56Ni0·17Co0·07O2 (LMNCO) via a sol-gel process combined with a two-step annealing treatment in this work. Serving as a physical separator, LTPO coating effectively depresses the side reactions at cathode-electrolyte interface and the transition-metal dissolution from LMNCO active material under harsh electrochemical environment. Meanwhile, LTPO layer with high ion conductivity could facilitate the interfacial Li+ diffusion during charge/discharge process. In addition, partial Ti4+ ions doped into LMNCO effectively elevate the oxygen electronegativity and restrain the excessive oxidization of lattice oxygen, thus stabilizing the crystal structure and alleviating the stress-strain propagation upon cycling. Electrochemical characterization results demonstrate that the LTPO-modified LMNCO cathode exhibits a superior capacity retention of 86.5 % after 400 cycles at room temperature and that of 73.7 % even under an elevated temperature of 45 °C after 250 cycles under 1C. This study provides a facile strategy for the surface modification of Li-rich layered-structure oxides, which also sheds light in enhancing electrochemical performances for various cathode materials.

Structure and crystallization behavior of Na2O–ZrO2–SiO2–P2O5 glass for solid-state electrolyte separation

Glass ceramics containing Na super-ionic conductor (NASICON) crystals are promising candidates for solid-state electrolyte separators in aqueous sodium ion batteries due to their high ion conductivity, water stability, and productivity. Our objective was to fabricate a glass-ceramic separator by crystallizing a NASICON phase within the glass via heat-treatment. We conducted a detailed investigation into the structural evolution of the glass and the crystallization morphology. Upon heat-treatment, Si units polymerized to form an island-like phase, while P contributed to increasing non-bridging O to form a sea-like phase during droplet phase separation; subsequently, the Na2Zr2SiP2O12 crystalline phase formed. The remaining glass comprised Q4 units of Si in the island-like phase, and Q1 and Q2 units of P in the sea-like phase. The ionic conductivity of the sample increased by crystallization up to 5.4 × 10–5 S⋅cm –1 at 300 K. Furthermore, the water leakage tests showed that both the glass and glass-ceramics exhibited low leakages.

Electrostatic Repulsion Facilitated Ion Transport in Covalent-Organic Framework Membranes.

Covalent-organic framework (COF) membranes are increasingly used for many potential applications including ion separation, fuel cells, and ion batteries. It is of central importance to fundamentally and quantitatively understand ion transport in COF membranes. In this study, a series of COF membranes is designed with different densities and arrangements of functional groups and subsequently utilize molecular simulation to provide microscopic insights into ion transport in these membranes. The membrane with a single-sided layer exhibits the highest chloride ion (Cl-) conductivity of 77.2 mScm-1 at 30°C. Replacing the single-sided layer with a double-sided layer or changing layer arrangement leads to a decrease in Cl- conductivity up to 33% or 53%, respectively. It is revealed that the electrostatic repulsion between ions serves as a driving force to facilitate ion transport and the positions of functional groups determine the direction of electrostatic repulsion. Furthermore, the ordered pores generate concentrated ions and allow rapid ion transport. This study offers bottom-up inspiration on the design of new COF membranes with moderate density and proper arrangement of functional groups to achieve high ion conductivity.

Regulating the Solvation Structure in Polymer Electrolytes for High‐Voltage Lithium Metal Batteries

Solid polymer electrolytes are promising electrolytes for safe and high‐energy‐density lithium metal batteries. However, traditional ether‐based polymer electrolytes are limited by their low lithium‐ion conductivity and narrow electrochemical window because of the well‐defined and intimated Li+‐oxygen binding topologies in the solvation structure. Herein, we proposed a new strategy to reduce the Li+‐polymer interaction and strengthen the anion‐polymer interaction by combining strong Li+‐O (ether) interactions, weak Li+‐O (ester) interactions with steric hindrance in polymer electrolytes. In this way, a polymer electrolyte with a high lithium ion transference number (0.80) and anion‐rich solvation structure is obtained. This polymer electrolyte possesses a wide electrochemical window (5.5 V versus Li/Li+) and compatibility with both Li metal anode and high‐voltage NCM cathode. Li||LiNi0.5Co0.2Mn0.3O2 full cells with middle‐high active material areal loading (~7.5 mg cm‐2) can stably cycle at 4.5 V. This work provides new insight into the design of polymer electrolytes for high‐energy‐density lithium metal batteries through the regulation of ion‐dipole interactions.

Regulating the Solvation Structure in Polymer Electrolytes for High-Voltage Lithium Metal Batteries.

Solid polymer electrolytes are promising electrolytes for safe and high-energy-density lithium metal batteries. However, traditional ether-based polymer electrolytes are limited by their low lithium-ion conductivity and narrow electrochemical window because of the well-defined and intimated Li+-oxygen binding topologies in the solvation structure. Herein, we proposed a new strategy to reduce the Li+-polymer interaction and strengthen the anion-polymer interaction by combining strong Li+-O (ether) interactions, weak Li+-O (ester) interactions with steric hindrance in polymer electrolytes. In this way, a polymer electrolyte with a high lithium ion transference number (0.80) and anion-rich solvation structure is obtained. This polymer electrolyte possesses a wide electrochemical window (5.5 V versus Li/Li+) and compatibility with both Li metal anode and high-voltage NCM cathode. Li||LiNi0.5Co0.2Mn0.3O2 full cells with middle-high active material areal loading (~7.5 mg cm-2) can stably cycle at 4.5 V. This work provides new insight into the design of polymer electrolytes for high-energy-density lithium metal batteries through the regulation of ion-dipole interactions.

La0.8Sr0.2Ga0.8Mg0.2O3−δ − molten carbonate membrane for high − temperature CO2 separation

A perovskite structure La0.8Sr0.2Ga0.8Mg0.2O3−δ (LSGM), is a promising support material for dual − phase membrane for high − temperature CO2 separation owing to its high oxygen ion conductivity. The microstructure plays an important role in CO2 separation performance of the membrane. The result shows that effective particle − to − particle contact is a crucial guarantee for improving CO2 permeability. The uniformly distributed small pores of the support can greatly reduce the leakage. The Al2O3 coating on the porous support can improve the wettability between LSGM and molten carbonate, simultaneously increasing CO2 permeation flux while reducing leakage. The Al2O3 coated LSGM − based dual − phase membrane achieves a CO2 permeation flux of 0.34 mL min−1 cm−2 at 750 °C, with no detectable leakage. Above 750 °C, a reaction occurs between LSGM and molten carbonate, leading to a decline in membrane performance. For LSGM − carbonate dual − phase membranes, it is recommended to operate at temperatures not exceeding 750 °C.