The release of textile dyeing wastewater results in significant environmental pollution and endangers human health. Membrane separation technology offers distinct advantages in textile wastewater treatment due to its energy efficiency, high performance, and excellent separation capabilities. This study demonstrates a facile MOF-polymer hybrid membrane fabrication strategy through amine-enhanced interfacial coordination. The introduced –NH2 groups via Noria and polyethyleneimine (PEI) co-deposition would chelate metal ions, which enhances the heterogeneous nucleation and the compatibility of metal–organic framework (MOF) and polymer. The optimized membrane exhibits superior dye sieving performance, achieving Congo red rejection of 98.9% and water permeance of 23.2 L m-2h−1 bar−1. Microstructural analysis reveals dense intergrown zeolitic imidazolate framework-8 (ZIF-8) architectures, validating the co-deposition approach as an effective surface engineering protocol for constructing continuous MOF-polymer hybrid membranes with defect-free interfaces. The membrane also shows superior operational stability at different pH levels and during long-term operation, which shows great potential for practical application.
Dimethyl carbonate (DMC), recognized as an environmentally benign green chemical, holds significant industrial value. In the realm of MeOH/DMC mixture separation, pervaporation technology aligns closely with China's dual-carbon strategic objectives due to its inherent low-energy consumption characteristics. This study employs doping modification to optimize the performance of polyethyleneimine (PEI)-based pervaporation membrane. Specifically, ZIF-8 was etched with tannic acid (TA) and the etched product (TA@ZIF-8) was incorporated into the PEI matrix to fabricate the c-TA@ZIF-8/PEI composite membrane. The TA-etched ZIF-8 plays a dual role: it creates additional mass transfer pathways to enhance separation efficiency, while simultaneously enabling chemical interactions with PEI that improve the anti-swelling properties of the resulting pervaporation membrane. This method effectively breaks the trade-off between membrane's separation performance and anti-swelling properties. The optimized membrane demonstrated exceptional separation performance, achieving a total permeation flux of 0.7 kg center dot m-2 center dot h-1 and a separation factor of 51.91 when treating a 10 wt% MeOH/DMC mixture at 50 degrees C. Through this composite modification approach, the research successfully balanced separation efficiency with anti-swelling properties, presenting a novel technological framework for industrial-scale organic solvent separation membranes.
As a critical component in alkaline water electrolyzers, the separator plays a vital role in overall performance. To overcome the limitations of traditional separators (e.g., low ionic conductivity and insufficient alkaline stability), this study proposes an innovative "pre-embedded monomer-interfacial polymerization" strategy and develops a novel dual-structure, dual-function polymer electrolyte membrane. This membrane achieves simultaneous optimization of stability and conductivity by in situ constructing a uniform QA crosslinked network within the ISM matrix via the Menshutkin reaction. synergistically integrating the alkali stability of ISM with the efficient ion transport properties of AEM. The optimized membrane (POBP-PMDETA-4) exhibited high ionic conductivity (92.3 mS/cm at 70 degrees C), high electrolyte uptake (101.83%), good hydrophilicity (42.2 degrees), and excellent performance in AWE,achieving 2.01 V at a current density of 0.4 A/cm2 with stable operation for 346 h. This study offers a promising strategy for designing high-performance, durable separators for advanced alkaline water electrolysis.
Metal-organic frameworks (MOFs)-based mixed matrix membranes (MMMs) have demonstrated significant potential in CO2 separation applications. However, challenges including inadequate CO2 affinity of MOFs and insufficient compatibility at MOF-polymer interface have hindered further advancement of MMMs. Hence, this work proposes a synergistic optimization strategy involving mixed-ligand and metal modification to overcome mentioned limitations. Initially, various defect-functionalized NH2-MIL-125 (DXNMIL-125) fillers were synthesized by adding 5-hydroxy-o-aminobenzoic acid ligands and integrated into carboxyl-modified cPIM-1 to formulate MMMs. The resulting MMMs were then Zn (II)-modified to further strengthen gas separation capabilities. The plentiful unsaturated Ti sites in DXNMIL-125 and the introduction of Zn (II) impart exceptional CO2 affinity to MMMs. Furthermore, they form multiple cross-linked structures with cPIM-1 via coordination, thereby improving interfacial compatibility and separation stability of MMMs. The binding energy derived from molecular simulation and CO2 adsorption results verify that defect sites enhance CO2 adsorption capacity of MOF. The optimal Zn@D33NMIL/cPIM-10 MMMs achieve a CO2 permeability of 4312.2 Barrer and a CO2/N2 selectivity of 34.8, reaching 2019 McKeown upper bound. This study presents a viable pathway for developing new-generation CO2 selective separation MMMs.
Water scarcity has intensified the reliance on reverse osmosis (RO) for water treatment. However, the persistent challenge of membrane fouling limits the long-term efficacy of RO in addressing water scarcity. Conventional hydrophilic modification strategy is difficult to overcome the electrostatic adsorption toward charged foulants owing to the negatively charged membrane surface. In this study, a dual-strategy approach combining amination and photoinitiated radical polymerization (PRP) is developed to construct an advanced highly hydrophilic and near-electroneutral RO membrane. Following the IP reaction, photoinitiators and small-molecule amines are anchored via a one-step amination reaction, and amphiphilic brushes are subsequently grafted under UV irradiation via a PRP reaction. Unlike conventional stepwise modifications that compromise the polyamide separation layer, this approach integrates charge neutralization and hydrophilic brush grafting in a non-destructive manner. The near-electroneutral surface remarkably weakens the electrostatic interaction and the exceptional hydration capacity (30.7 degrees) of highly hydrophilic surface provides a robust hydration shield, boosting the RO membrane with sustainable fouling resistance. The resulting RO membrane achieves a high water permeance of 3.3 L m- 2 h- 1 bar- 1 with a water/NaCl selectivity of 15.8 bar- 1. The membrane demonstrates an desirable antifouling performance against various charged foulants (such as exceptionally high flux recovery ratios of 98.4%, 97.7% and 99.3% for negatively charged sodium dodecyl sulfate, positively charged cetyl-trimethyl ammonium bromide, and gypsum scaling, respectively), outperforming most current advanced anti-fouling RO membranes. The dual barrier of hydration repulsion and electrostatic shielding eliminates electrostatic and hydrophobic fouling simultaneously, overcoming the limitations of single-foulant studies. In contrast to complex multi-step methods, our structurally coherent two-step process enables uniform, controllable grafting and can be extended to nanofiltration. Interfacial thermodynamics and molecular simulations elucidate the underlying synergy, while practical secondary effluent treatment, superior chemical stability, and strategy universality confirm its engineering potential. This work offers a scalable surface-engineering platform that synergistically tunes charge and hydrophilicity for sustainable water treatment.
Superhydrophobic coatings hold broad application prospects across numerous fields. However, the super-hydrophobicity is often compromised by poor mechanical robustness of micro-nano structures, which severely hinders their practical application. Herein, a novel fluorine-free Pickering emulsion-based microsphere cell (PMC) with inherent micro-nano composite structures via in-situ droplet solidification. Combined with PMC and polymer binder, the composite coating achieves a water contact angle greater than 165 degrees and a water sliding angle of 2.7 degrees owing to the abundant well-defined micro-nano structures. Importantly, this coating exhibits unique self-similar structure and self-repair ability, which endow the coating with superior mechanical robustness, enabling the maintenance of a above contact angle 160 degrees until complete wear. When subjected to mechanical stress, the self-similar structure effectively preserves the micro-structures while the fractured PMC exposes the encapsulated hydrophobic-SiO2 seeds to repair the damaged nano-structures, which jointly maintains the coating's super-hydrophobicity. Furthermore, the coating demonstrates the excellent self-cleaning and freezing delay performance (1600 s,-15 degrees C), which is 11 times of bare substrate. Scalable preparation of the PMC is achieved, readily yielding kilogram-scale products and demonstrating practical applicability. This study develops a durable superhydrophobic coating with self-similar structure and self-repair ability, showing promising potential for large-scale production and practical application.
Membrane separation technology exhibits significant advantages for helium extraction from low‑helium natural gas. Nevertheless, its performance is still constrained by the inherent trade‑off between permeability and selectivity, posing a significant challenge for the selective separation of a target gas. Here, we propose a targeted microphase engineering strategy that precisely optimizes the nanophase separation structure of copolyimide membranes by adjusting the ratio of 9,9-bis(4-amino-3-Chlorophenyl)fluorene (CFDA) and 9,9-bis(4-amino-3-fluorophenyl)fluorene (FFDA), thereby enabling specific separation of He/CH4 and He/N2. Experiments and molecular simulations jointly demonstrate that at a CFDA/FFDA ratio of 1:3, the membrane forms a dense chain-stacking structure that effectively suppresses CH4 diffusion, achieving a He/CH4 selectivity of 78.0 and a permeability of 185.3 Barrer. When the ratio is adjusted to 1:5, fluorine atoms induce the formation of a space-filling structure with sieving properties, enabling size-selective suppression of N2 diffusion, achieving a He/N2 selectivity of 37.7 and a permeability of 159.2 Barrer. Furthermore, both membranes exhibit excellent long-term stability over 210 days and maintain high He/CH4(324.5,6FDA-C/F(1:3)FDA) and He/N2(44.2, 6FDA-C/F(1:5)FDA) separation selectivity in ternary gas mixtures (He/CH4/N2 = 0.5/98/1.5 vol%). This study elucidates the structure-function relationship between chemical composition, nanostructure, and separation performance at the molecular level, providing a design strategy for developing high-performance targeted gas separation membranes tailored to practical demands.
Organic solvent nanofiltration (OSN) holds great potential for replacing energy-intensive separation processes but suffers from low permeance. This study enhanced membrane permeance without compromising rejection via two strategies: (1) HKUST-1 was added to optimize the polyimide (P84) membrane substrate; (2) MIL-53(Fe) was added to polyamide (PA) layer to achieve a trade-off between permeance and rejection. The results showed that HKUST-1 increased the porosity of the support layer, thereby facilitating the transport of solvents. Density functional theory (DFT) calculations revealed that the hydrolysis of HKUST-1 was thermodynamically favorable, which was further confirmed by FTIR. The resulting structural optimization was validated by SEM. In the PA selective layer, MIL-53(Fe) exhibited intense coordination bonding with amide groups. Similarly, the addition of MIL-53(Fe) significantly enhanced the DMAc permeance from 2.41 L & centerdot;m(-2)& centerdot;h(-1)& centerdot;bar(-1) to 10.70 L & centerdot;m(-2)& centerdot;h(-1)& centerdot;bar(-1), approximately increasing by 4.4 times, while the CR rejection also improved concurrently from 91.91% to 92.69%. Regression models (R-2 > 0.95) base on correlation analysis confirmed the reliability of the permeance and selective. This study provided a systematic design framework for high-performance OSN membranes.
Hydrate-based CO2 sequestration demonstrates promising potential for long-term carbon storage. However, considering that the hydrate stable zone is located in the shallow seabed, the adaptability and leakage risk of the formed CO2 hydrate-liquid CO2-seawater system need to be investigated. Therefore, we explore the CO2 leakage behavior from the CO2 hydrate-liquid CO2-seawater coexistence system in submarine sediments caused by external p-T changes. The processes of system expansion and phase change corresponding to different p-T evolutionary paths are analyzed, thereby revealing their impact mechanisms on CO2 leakage. The form of CO2 leakage depends on the phase equilibrium boundary crossed by its state evolution trajectory, and there are three types of phase transition processes: liquid CO2 gasification followed by hydrate decomposition into CO2 gas; hydrate decomposition into liquid CO2 followed by liquid CO2 gasification; hydrate decomposes directly into liquid CO2. The results show that severe CO2 leakage occurs after liquid CO2 vaporization, with an escape rate approaching 90%. When the reservoir pressure is sufficient to maintain liquid CO2, the escape rate resulting from hydrate decomposition induced by temperature increase is approximately 14%. Meanwhile, due to larger volume changes, higher hydrate saturation can actually lead to an increase in the CO2 leakage rate to 20%. Even so, CO2 sequestration density in the hydrate state is higher than in the liquid state, and hydrated CO2 sequestration can spontaneously mitigate changes in environmental temperature, representing a more stable sequestration form. This study provides new insights into the control of CO2 leakage for geologic CO2 sequestration.
To mitigate the efficiency degradation of photovoltaic (PV) modules caused by dust contamination and low-temperature icing, we report a fluorine-free, robust, and transparent superhydrophobic coating fabricated via a spray-curing process. A PDMS-based interpenetrating polyurea (U-PDMS) and epoxy (PDMS-E44) network serves as the polymer matrix, while trace 3-amino-propyltriethoxysilane (APTES) acts as an interfacial bridge and local crosslinking regulator, strengthening cohesion and adhesion while suppressing SiO2 aggregation, without compromising optical clarity. By optimizing the SiO2 content, the coating balances superhydrophobicity and high transmittance (90.8%), accompanied by an excellent contact angle of 167.5 degrees and an ultralow sliding angle of 0.9 degrees. More importantly, it retains superhydrophobicity after 50 tape-peeling cycles and delays droplet freezing by similar to 8-fold at -5 degrees C compared with pristine glass. As PV encapsulation glass, the coating causes only a 0.76% initial power conversion efficiency (PCE) loss, enables 99.3% recovery of short-circuit current density (J(sc)) after soiling-and-rinsing, and exhibits a 3.94% decrease in normalized PCE after 40 days of outdoor exposure, compared to 11.74% for pristine glass. Overall, this coating provides durable anti-soiling and anti-icing protection for PV modules, while maintaining high transmittance and practical processability.
Two-dimensional MXene materials exhibit significant promise in hydrogen separation membranes, especially for the effective separation of H2/CO2 mixtures, thanks to their structured interlayer channels and profusion of surface functional groups. However, in humid or watery conditions, MXene membranes are susceptible to interlayer swelling, which significantly impairs their ability to separate materials. In order to improve the hydrothermal stability of MXene membranes for effective H2/CO2 separation, we used polyvinyl alcohol (PVA) to intercalate between the MXene nanosheets and cross-link them via heat treatment. The method of heat crosslinking makes it easier for the functional groups of PVA and MXene nanosheets to connect, giving the membrane superior molecular sieving capabilities. Additionally, PVA improves MXene's interlayer spacing, resulting in quicker gas transport paths. MXene's size-selective characteristics and surface adsorption capability efficiently inhibit CO2 diffusion while facilitating H2 permeation. The resultant 20 % PMM composite membrane demonstrates a H2 permeance of 1453 GPU and a H2/CO2 selectivity of 45, sustaining steady separation performance during 72 h of operation, including 20 h in a humid environment.
Abstract Membrane separation technology exhibits significant advantages for helium extraction from low‐helium natural gas. Nevertheless, its performance remains constrained by the inherent trade‐off between permeability and selectivity. Here, we systematically tailor the nanoscale architecture of copolyimide membranes by adjusting the ratio of 9,9‐bis(4‐amino‐3‐chlorophenyl)fluorene (CFDA) to 9,9‐bis(4‐amino‐3‐fluorophenyl)fluorene (FFDA), enabling selective separation of He/CH 4 and He/N 2 . At a CFDA/FFDA ratio of 1:3, the membrane shows a moderate fractional free volume (FFV = 24.06%), which restricts the diffusion of CH 4 more effectively than that of He, leading to a He/CH 4 selectivity of 78.0. At a ratio of 1:5, the denser structure (FFV = 23.72%) with a lower FFV enhances size‐exclusion for N 2 , achieving a He/N 2 selectivity of 37.7. Both membranes exhibit excellent 210‐day stability and maintain high selectivity in a ternary mixture (He/CH 4 /N 2 = 0.5/98/1.5, vol%). This work elucidates the composition‐nanostructure‐performance relationship, offering a rational design strategy for targeted gas separation membranes.
Membranes with high selectivity and water permeance are required for improving product water quality and increasing process efficiency. Traditional surfactant-assisted interfacial polymerization (IP) could improve selectivity of polyamide (PA) nanofiltration (NF) membranes but usually decreased water permeance. Here, short hydrophobic chain surfactant, sodium p-styrene sulfonate (SSS) with styrene and sulfonic acid groups was utilized as a new aqueous surfactant during IP process to prepare the PA-NF membrane, improving water permeability and salt rejection simultaneously. SSS had higher critical micelle concentration and can be richly incorporated within PA layer. The membranes characterizations were conducted by atomic force microscopy, scanning electron microscopy, attenuated total reflectance-Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, goniometer, and zeta potential analyzer. The regulated membrane exhibited slightly enlarged and more uniform pore size, as well as smoother, more hydrophilic and negatively charged membrane surface. The water flux increased from 46.6 +/- 3.7 L center dot m- 2 center dot h- 1 to 61.9 +/- 2.6 L center dot m- 2 center dot h- 1 (increasing by 32.83%), while Na2SO4 rejection increased by 10.18%. The Cl-/SO42- selectivity increased from 15.2 to 45.1 when using mixed salts solution as feed. Furthermore, SSS-regulated membrane demonstrated increased tetracycline rejection. Enhanced resistance properties (pH stability and antifouling properties) were also observed for SSSregulated membrane. The study presents a novel surfactant for the fabrication of PA-NF membrane.
Lithium-ion batteries (LIBs) play a critical role in reducing carbon emissions in the automotive industry. However, they face challenges related to safety and performance failures. Smart technologies offer a promising solution to address these issues. Bioinspired microcapsules are a common approach to enhancing the performance and safety of smart LIBs. However, despite their potential, this area has not been thoroughly explored. This review provides an overview of the preparation methods for microcapsules, including physical, chemical, and physicochemical techniques. These microcapsules are categorized based on their mechanisms into electrode self-healing burst microcapsules, interphase-forming sustained-release microcapsules, live-lithium sustained-release microcapsules, and flame-retardant burst microcapsules. A comprehensive analysis of their bioinspired design concepts, mechanisms, and performance is presented, along with the design criteria for microcapsules suitable for LIBs. Finally, the review explores the potential applications of microcapsule technologies in LIBs and their future trends, such as enhancing existing technologies for novel applications like solid-state batteries and developing new types of microcapsules. This review aims to provide a foundation for the implementation of microcapsule technologies in LIBs and to highlight the latest advancements in smart batteries.
Excessive carbon emission leads to global warming, threatening human survival. Membrane-based carbon capture technology is an important component of carbon capture, utilization, and storage (CCUS) technology and one of the main upstream technologies for achieving carbon neutrality. PIM-1 materials exhibit high CO2 permeability but lower CO2/N2 selectivity, making it a significant focus to improve CO2/N2 selectivity without sacrificing CO2 permeability. In this work, Noria was introduced as a block through the bottom-up approach into the PIM-1 molecular chain, forming Noria-based porous organic polymer (NPOP) microregions with excellent CO2 affinity. Additionally, the presence of NPOP increases the interchain gaps, resulting in a higher free volume. Consequently, the separation membrane prepared under optimal conditions broke the 2008 upper bound, with a 43.6 % increase in CO2 permeability and a 41.7 % increase in CO2/N2 selectivity. Furthermore, NPOP could form colloidal networks and provide rigidity to the separation membrane, endowing it with excellent aging resistance. After 6 months of aging, the CO2 permeability of 0.5 %Noria decreased by only 33.4 % (67.4 % for pure PIM-1), indicating its strong potential for widespread applications.
Extraction of lithium resources from salt lake brines is an effective method to solve the shortage of lithium resources nowadays. However, magnesium-lithium separation has become a critical issue for lithium extraction from salt lakes with high Mg2+/Li+ 2+ /Li + ratio, due to the similar ionic characteristics of Li+ + (0.38 nm), and Mg2+ 2+ (0.43 nm). Herein, an amine monomer containing crown ether group (4 '-aminobenzo-15-crown-5-ether '-aminobenzo-15-crown-5-ether (NH2-B15C5)) 2 -B15C5)) was introduced into the interfacial polymerization (IP) process of piperazine (PIP) and homotrimethylene tricarbonyl chloride (TMC) to prepare polyamide (PA) nanofiltration (NF) membranes with Li+ + selective transport channels. NH2-B15C5 2 -B15C5 shows good compatibility and selective complexation to Li+, + , which acts as Li+ + selective transport channels effectively retaining Mg2+ 2+ and allowing Li+ + to cross the membrane smoothly, therefore solving the problem of poor lithium-magnesium separation performance of most of the NF membranes currently. Molecular dynamics simulations (MD) also confirmed that NH2-B15C5 2 -B15C5 has a stronger affinity for Li+ + than for Mg2+. 2+ . The NH2-B15C5/PIP-TMC 2 -B15C5/PIP-TMC membrane exhibited excellent separation performance and water permeance in simulated salt lake brine (2000 ppm, W Mg/Li = 100), where the S Li, Mg and water permeance were 32.2 and 8.22 L center dot m-2 center dot h-1 center dot bar-1 . Importantly, the crown ether is introduced into the PA separator layer in the form of covalent bonds, hence showing excellent stability. Overall, an NF membrane with high lithium- magnesium separation performance was designed for the extraction of lithium resources from high Mg2+/Li+ 2+ /Li + ratio salt lake brine.
Efficient membrane-based carbon capture is a key front-end technology for achieving carbon neutrality. Crystalline carbon materials offer advantages such as high mechanical strength and a high degree of structural regularity, and are often used as fillers in the fabrication of mixed matrix membranes (MMMs). However, they tend to undergo pi-pi stacking and aggregation, leading to the formation of non-selective defects within the membrane. In this work, amorphous carbon material Ketjen black (KB) was deeply aminated via a diazoniuminduced anchoring process (DIAP) and employed as a nanofiller to fabricate CO2-philic and aging-resistant PIM-based MMMs. TEM characterization confirmed that amino groups were successfully grafted onto both the surface and the internal pores of KB. Experimental results and molecular dynamics simulations revealed that the introduced amino groups enhanced the interaction energy between the filler and the polymer chains, thereby improving the compatibility between the inorganic and organic phases and significantly boosting the membrane's aging resistance. Additionally, the amino groups served as CO2-affinitive sites, effectively increasing the CO2/N2 selectivity. The incorporation of uniformly sized amorphous carbon nanoparticles increased the fractional free volume of the membrane without introducing non-selective defects, thus improving the CO2 permeability. Under optimized conditions, the resulting MMM exhibited a CO2 permeability of 9024 Barrer and a CO2/N2 selectivity of 23.7, exceeding the Robeson upper bound. After 180 days of aging, the CO2 permeability decreased by only 16.9 %, demonstrating excellent long-term performance and offering a new paradigm for the application of amorphous carbon materials in PIM-based membranes for carbon capture.
CO2 hydrate-based sequestration in submarine sediments shows great potential for carbon emission reduction. Considering the proportional relationship of CO2 and water for hydrates formation, their existing ratio largely determines the CO2 sequestration density and phase state. Here, this work focuses on determining the optimal ratio of CO2 to seawater in sediments simulated with 20-40 mesh (0.42-0.85 mm) quartz sand, in order to maximize CO2 hydrate conversion in sediments. The results show that the conversion rate of CO2 hydrate increases with the initial water saturation, reaching 15.3% at 80% initial water saturation. The optimal CO2 hydrate formation occurs at 30% initial water saturation, with the corresponding CO2 storage density in hydrate form of 33.09 kgm(-3) and the hydrate saturation of 22.3%. However, CO2 hydrate conversion rate is <10%, which implies that most CO2 still exists in liquid state, despite the presence of free water. The total CO2 sequestration density is negatively correlated with the initial water saturation, and at 10% initial water saturation, 398.73 kgm(-3) of CO2 is sequestered, of which only 18.02 kgm(-3) is hydrated. Additionally, the lower initial water saturation corresponds to the shorter time to achieve t(90) of CO2 consumption, and the water conversion rate to hydrate reaches 90% at 10% initial water saturation. In summary, adjusting the volume ratio of liquid CO2 to seawater can effectively increase the sequestration amount of CO2 hydrates, but methods to increase CO2 conversion to hydrate still need to be established. (c) 2025 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
Hydrate-based CO2 storage is a highly promising technology for long-term stable CO2 storage in sediments. However, the unclear displacement and hydration mechanisms, along with the low conversion rate of CO2 hydrates, have hindered the field application. Here, we report a method of the injection of CO2/water emulsion to replace liquid CO2 to regulate the ratio of CO2 to water in the sediment pores and to enhance their contact ability, which can significantly improve the CO2 hydrate conversion rate. Compared to liquid CO2 injection, emulsion injection can flow through more sediment pores with an increase in displacement efficiency by 45 %-62 %, which leaves a CO2-to-water ratio within the pores that is more suitable for hydrate formation, ultimately tripling the hydrate conversion rate. We have outlined the hydrate growth mechanisms for both injection forms, where the micron-sized CO2 droplets within the emulsion can greatly reduce the barrier effect of hydrate film. Under the combined influences, the CO2 storage density in hydrates up to 91.2 kg/m3 for CO2/water emulsion injection is 47.8 % higher than that of 61.7 kg/m3 for liquid CO2 injection. Our work provides a new approach to high conversion CO2 hydrate sequestration in submarine sediments.