Fabrication of Ultrathin Membranes Using 2D-MOF Nanosheets for Tunable Gas Separation

Two-dimensional (2D) metal-organic frameworks (MOF) nanosheets have emerged as novel membrane materials for gas separation. However, the development of ultrathin MOF membranes with tunable separation performances is still a challenge. Herein, we developed a facile GO-assisted restacking method to fabricate defect-free membranes with monolayer Zr-BTB nanosheets. Obtained ultrathin membranes ranging from 130 nm to 320 nm show tunable separation performances and exceed the 2008 Robeson upper bound by changing the amount of nanolayers in vertical stacking direction. Furthermore, a heating filtration method was used to change the restacking process of nanosheets in the horizontal direction. As a result, H₂/CO₂ selectivity can be enhanced by two times with the same membrane thickness (130 nm) and H₂ permeance is almost maintained to be 7.0×10⁻⁷ mol m⁻² s⁻¹ pa⁻¹. This method may provide a possible way to efficiently tune the gas separation performances of MOF membranes.     

Sequential Chemistry Toward Core–Shell Structured Metal Sulfides as Stable and Highly Efficient Visible-Light Photocatalysts

A universal sequential synthesis strategy in aqueous solution is presented for highly uniform core–shell structured photocatalysts, which consist of a metal sulfide light absorber core and a metal sulfide co-catalyst shell. We show that the sequential chemistry can drive the formation of unique core–shell structures controlled by the constant of solubility product of metal sulfides. A variety of metal sulfide core–shell structures have been demonstrated, including CdS@CoS_x, CdS@MnS_x, CdS@NiS_x, CdS@ZnS_x, CuS@CdS, and more complexed CdS@ZnS_x@CoS_x. The obtained strawberry-like CdS@CoS_x core–shell structures exhibit a high photocatalytic H₂ production activity of 3.92 mmol h⁻¹ and an impressive apparent quantum efficiency of 67.3 % at 420 nm, which is much better than that of pure CdS nanoballs (0.28 mmol h⁻¹), CdS/CoS_x composites (0.57 mmol h⁻¹), and 5 %wt Pt-loaded CdS photocatalysts (1.84 mmol h⁻¹).     

Two-Dimensional LDH Film Templating for Controlled Preparation and Performance Enhancement of Polyamide Nanofiltration Membranes

Tailored design of high-performance nanofiltration membranes that can be used in a variety of applications such as water desalination, resource recovery, and sewage treatment is desirable. Herein, we describe the use of layered double hydroxides (LDH) intermediate layer to control the interfacial polymerization between trimesoyl chloride (TMC) and piperazine (PIP) for the preparation of polyamide (PA) membrane. The dense surface of LDH layer and its unique mass transfer behavior influence the diffusion of PIP, and the supporting role of the LDH layer allows the formation of ultrathin PA membranes. By only changing the concentration of PIP, a series of membranes with controllable thickness from 10 to 50 nm and tunable crosslinking-degree can be prepared. The membrane prepared with a higher concentration of PIP shows excellent performance for divalent salt retention with water permeance of 28 Lm⁻² h⁻¹ bar⁻¹, high rejection of 95.1 % for MgCl₂ and 97.1 % for Na₂SO₄. While the membrane obtained with a lower concentration of PIP can sieve dye molecules of different sizes with a flux of up to 70 Lm⁻² h⁻¹ bar⁻¹. This work demonstrates a novel strategy for the controllable preparation of high-performance nanofiltration membranes and provides new insights into how the intermediate layer affects the IP reaction and the final separation performance.     

Growth of High‐Quality,Thickness‐Reduced Zeolite Membranes towards N2/CH4 Separation Using High‐Aspect‐Ratio Seeds

Greatly improved zeolite membranes were prepared by using high‐aspect‐ratio zeolite seeds. Slice‐shaped seeds with a high aspect ratio (AR) facilitated growth of thinner continuous SAPO‐34 membranes of much higher quality. These membranes showed N₂ permeances as high as (2.87±0.15)×10⁻⁷ mol m⁻² s⁻¹ Pa⁻¹ at 22 °C while maintaining a decent N₂/CH₄ selectivity (9–11.2 for equimolar mixture). On the basis of these thinner high‐quality SAPO‐34 membranes, fine‐tuning the local crystal structure by incorporating more silicon further increased the N₂ permeance by 1.4 times without sacrificing the N₂/CH₄ selectivity. We expect that application of large AR zeolite seeds might be a viable strategy to grow thin high‐quality zeolite membranes. In addition, fine‐tuning of the crystal structure by changing the crystal composition might be a feasible way for further improving the separating performance of high‐quality zeolite membranes.     

Hybrid Transition-Metal Oxide and Nitride@N-Doped Reduced Graphene Oxide Electrodes for High-Performance,Flexible, and All-Solid-State Supercapacitors

Nanoscale composites for high-performance electrodes employed in flexible, all-solid-state supercapacitors are being developed. A series of binder-free composites, each consisting of a transition bimetal oxide, a metal oxide, and a metal nitride grown on N-doped reduced graphene oxide (rGO)-wrapped nickel foam are obtained by using a universal strategy. Three different transition metals, Co, Mo, and Fe, are separately compounded with nickel ions, which originate from the nickel foam, to form three composites, NiCoO₂@Co₃O₄@Co₂N, NiMoO₄@MoO₃@Mo₂N, and NiFe₂O₄@Fe₃O₄@Fe₂N, respectively. These as-prepared active materials have similar regular variation patterns in their properties, including better conductivity and battery-mimicking pseudocapacitance, which result in their high whole-electrode capacitance performance [2598.3 F g⁻¹ (39.85 F cm⁻²), 3472.6 F g⁻¹ (41.43 F cm⁻²) and 1907.5 F g⁻¹ (3.41 F cm⁻²) for the composites incorporating Co, Mo, and Fe, respectively]. The as-assembled flexible, all-solid-state NiCoO₂@Co₃O₄@Co₂N//KOH/PVA//NiCoO₂@Co₃O₄@Co₂N device can be easily bent and exhibits high energy density and power density of 92.8 Wh kg⁻¹ and 1670.4 W kg⁻¹, respectively. The universality of this design strategy could allow it to be employed in producing hybrid materials for high-performance energy-storage devices.     

Enhancement of Visible-Light-Driven Hydrogen Evolution Activity of 2D π-Conjugated Bipyridine-Based Covalent Organic Frameworks via Post-Protonation

Photocatalytic hydrogen (H₂) evolution represents a promising and sustainable technology. Covalent organic frameworks (COFs)-based photocatalysts have received growing attention. A 2D fully conjugated ethylene-linked COF (BTT-BPy-COF) was fabricated with a dedicated designed active site. The introduced bipyridine sites enable a facile post-protonation strategy to fine-tune the actives sites, which results in a largely improved charge-separation efficiency and increased hydrophilicity in the pore channels synergically. After modulating the degree of protonation, the optimal BTT-BPy-PCOF exhibits a remarkable H₂ evolution rate of 15.8 mmol g⁻¹ h⁻¹ under visible light, which surpasses the biphenyl-based COF 6 times. By using different types of acids, the post-protonation is proved to be a potential universal strategy for promoting photocatalytic H₂ evolution. This strategy would provide important guidance for the design of highly efficient organic semiconductor photocatalysts.     

Molecular Engineering of a Metal-Organic Polymer for Enhanced Electrochemical Nitrate-to-Ammonia Conversion and Zinc Nitrate Batteries

Metal–organic framework-based materials are promising single-site catalysts for electrocatalytic nitrate (NO₃⁻) reduction to value-added ammonia (NH₃) on account of well-defined structures and functional tunability but still lack a molecular-level understanding for designing the high-efficient catalysts. Here, we proposed a molecular engineering strategy to enhance electrochemical NO₃⁻-to-NH₃ conversion by introducing the carbonyl groups into 1,2,4,5-tetraaminobenzene (BTA) based metal-organic polymer to precisely modulate the electronic state of metal centers. Due to the electron-withdrawing properties of the carbonyl group, metal centers can be converted to an electron-deficient state, fascinating the NO₃⁻ adsorption and promoting continuous hydrogenation reactions to produce NH₃. Compared to CuBTA with a low NO₃⁻-to-NH₃ conversion efficiency of 85.1 %, quinone group functionalization endows the resulting copper tetraminobenzoquinone (CuTABQ) distinguished performance with a much higher NH₃ FE of 97.7 %. This molecular engineering strategy is also universal, as verified by the improved NO₃⁻-to-NH₃ conversion performance on different metal centers, including Co and Ni. Furthermore, the assembled rechargeable Zn−NO₃⁻ battery based on CuTABQ cathode can deliver a high power density of 12.3 mW cm⁻². This work provides advanced insights into the rational design of metal complex catalysts through the molecular-level regulation for NO₃⁻ electroreduction to value-added NH₃.     

Robust S4⋅⋅⋅O Supramolecular Synthons: Structures of Radical-Radical Cocrystals [p-XC6F4CNSSN]2[TEMPO] (X=F,Cl, Br,I, CN)

Cocrystallization of the dithiadiazolyl (DTDA) radicals p-XC₆F₄CNSSN (X=F, Cl, Br, I, CN) with TEMPO afforded the 2 : 1 cocrystals [p-XC₆F₄CNSSN]₂[TEMPO] ( 1 – 5 ) whose structures all reflect a common S₄⋅⋅⋅O supramolecular motif. The nature of this interaction was probed by DFT calculations (M06/aug-cc-pVDZ) on 1 which revealed that the enthalpy of formation of the [C₆F₅CNSSN]₂[TEMPO] supramolecular motif from [C₆F₅CNSSN]₂ and TEMPO is substantial (−54.0 kJ mol⁻¹). Electronic structure calculations revealed a TEMPO-based doublet S= configuration as the ground state with limited spin density on the DTDA rings (2.4 %). The corresponding spin quartet state is +78.9 kJ mol⁻¹ higher in energy. An atoms-in-molecules analysis reveals four bond critical points (BCPs) between the TEMPO O and the DTDA S atoms as well as additional BCPs between selected DTDA S atoms and methyl H atoms of the TEMPO molecule. Herein, the structures of 2 – 5 are considered within the context of a hierarchical view of competing and complementary intermolecular interactions; in particular, the established supramolecular CN⋅⋅⋅S−S synthon is sacrificed in order to form the new S₄⋅⋅⋅O interaction.     

Advanced Lithium Extraction Membranes Derived from Tagged-Modification of Polyamide Networks

Efficient Mg²⁺/Li⁺ separation is crucial to combating the lithium shortage worldwide, yet current nanofiltration membranes suffer from low efficacy and/or poor scalability, because desirable properties of membranes are entangled and there is a trade-off. This work reports a “tagged-modification” approach to tackle the challenge. A mixture of 3-bromo-trimethylpropan-1-aminium bromide (E₁) and 3-aminopropyltrimethylazanium (E₂) was designed to modify polyethylenimine – trimesoyl chloride (PEI-TMC) membranes. E₁ and E₂ reacted with the PEI and TMC, respectively, and thus, the membrane properties (hydrophilicity, pore sizes, charge) were untangled and intensified simultaneously. The permeance (34.3 L m⁻² h⁻¹ bar⁻¹) and Mg²⁺/Li⁺ selectivity (23.2) of the modified membranes are about 4 times and 2 times higher than the pristine membrane, and they remain stable in a 30-days test. The permeance is the highest among all analogous nanofiltration membranes. The tagged-modification method enables the preparation of large-area membranes and modules that produce high-purity lithium carbonate (Li₂CO₃) from simulated brine.     

Anisotropic Gas Separation in Oriented ZIF-95 Membranes Prepared by Vapor-Assisted In-Plane Epitaxial Growth

Control of the microstructure grain orientation, grain boundaries and thickness are crucial for MOF membranes. We report a novel synthesis strategy to prepare highly c-oriented ZIF-95 membranes through vapor-assisted in-plane epitaxial growth. In a mixed DMF/water vapor atmosphere, in-plane epitaxial growth of a ZIF-95 seeds layer was achieved to obtain an oriented and well-intergrown ZIF-95 membrane with a thickness of only 600 nm. Demonstrated by both experimental and simulation studies, the c-oriented ZIF-95 membrane displayed superior separation performance because a perfectly oriented structure resulted in a notable reduction of intercrystalline defects and transport pathways. For the separation of equimolar binary mixtures at 100 °C and 1 bar, the mixture separation factors of H₂/CO₂ and H₂/CH₄ were 32.2 and 53.7, respectively, with an H₂ permeance of over 7.9×10⁻⁷ mol m⁻² s⁻¹ Pa⁻¹, which was 4.6 times higher than that of a randomly oriented ZIF-95 membrane.     

Formation of Ultrathin,Continuous Metal–Organic Framework Membranes on Flexible Polymer Substrates

Metal–organic framework (MOF) materials have an enormous potential in separation applications, but to realize their potential as semipermeable membranes they need to be assembled into thin continuous macroscopic films for fabrication into devices. By using a facile immersion technique, we prepared ultrathin, continuous zeolitic imidazolate framework (ZIF‐8) membranes on titania‐functionalized porous polymeric supports. The coherent ZIF‐8 layer was surprisingly flexible and adhered well to the support, and the composite membrane could sustain bending and elongation. The membranes exhibited molecular sieving behavior, close to the theoretical permeability of ZIF‐8, with hydrogen permeance up to 201×10⁻⁷ mol m⁻² s⁻¹ Pa⁻¹ and an ideal H₂/CO₂ selectivity of 7:1. This approach offers significant opportunities to exploit the unique properties of MOFs in the fabrication of separation and sensing devices.     

Boosting Na+ Storage Ability of Bimetallic MoxW1−xSe2 with Expanded Interlayers

In spite of the valuable advancements in the fabrication of transition-metal selenides (TMSs)-based hybrid structures, only single-metal selenides have been obtained through most of the present methods. Herein, a facile room-temperature self-polymerization and subsequent selenization strategy is proposed for the synthesis of bimetallic Mo_xW_1−xSe₂ nanosheets with expanded interlayers decorated with N-doped carbon-matrix assembled flowerlike hierarchical microspheres (Mo_xW_1−xSe₂/NC). Depending on the excellent coordination ability of dopamine with metal ions, self-formed flowerlike single precursors are harvested. The unique hybrid architecture benefits the penetration of the electrolyte, accelerates Na⁺ insertion/extraction kinetics, enhances electron-transfer ability, and alleviates the volume expansion and aggregation during cycling processes. Therefore, the bimetallic Mo_xW_1−xSe₂/NC electrode delivers high reversible capacities of 264 mA h g⁻¹ at 1 A g⁻¹ for 700 cycles, 204.4 mA h g⁻¹ at 4 A g⁻¹ for 1400 cycles, and 153.3 mA h g⁻¹ at 8 A g⁻¹ for 2000 cycles, as well as an excellent rate capability up to 10 A g⁻¹ with a capacity of 188.9 mA h g⁻¹. Our study offers an effective strategy to boost sodium storage performance through elaborate structural engineering.     

Palladium Complexes Based on Ylide-Functionalized Phosphines (YPhos): Broadly Applicable High-Performance Precatalysts for the Amination of Aryl Halides at Room Temperature

Palladium allyl, cinnamyl, and indenyl complexes with the ylide-substituted phosphines Cy₃P⁺−C⁻(R)PCy₂ (with R=Me ( L1 ) or Ph ( L2 )) and Cy₃P⁺−C⁻(Me)PtBu₂ ( L3 ) were prepared and applied as defined precatalysts in C−N coupling reactions. The complexes are highly active in the amination of 4-chlorotoluene with a series of different amines. Higher yields were observed with the precatalysts in comparison to the in situ generated catalysts. Changes in the ligand structures allowed for improved selectivities by shutting down β-hydride elimination or diarylation reactions. Particularly, the complexes based on L2 (joYPhos) revealed to be universal precatalysts for various amines and aryl halides. Full conversions to the desired products are reached mostly within 1 h reaction time at room temperature, thus making L2 to one of the most efficient ligands in C−N coupling reactions. The applicability of the catalysts was demonstrated for aryl chlorides, bromides and iodides together with primary and secondary aryl and alkyl amines, including gram-scale applications also with low catalyst loadings of down to 0.05 mol %. Kinetic studies further demonstrated the outstanding activity of the precatalysts with TOF over 10.000 h⁻¹.     

Electrolyte and interphase engineering through solvation structure regulation for stable lithium metal batteries

Lithium metal batteries (LMBs) are considered to be one of the most promising high-energy-density battery systems. However, their practical application in carbonate electrolytes is hampered by lithium dendrite growth, resulting in short cycle life. Herein, an electrolyte regulation strategy is developed to improve the cyclability of LMBs in carbonate electrolytes by introducing LiNO₃ using trimethyl phosphate with a slightly higher donor number compared to NO₃⁻ as a solubilizer. This not only allows the formaion of Li⁺-coordinated NO₃⁻ but also achieves the regulation of electrolyte solvation structures, leading to the formation of robust and ion-conductive solid-electrolyte interphase films with inorganic-rich inner and organic-rich outer layers on the Li metal anodes. As a result, high Coulombic efficiency of 99.1% and stable plating/stripping cycling of Li metal anode in Li||Cu cells were realized. Furthermore, excellent performance was also demonstrated in Li||LiNi_0.83Co_0.11Mn_0.06O₂ (NCM83) full cells and Cu||NCM83 anode-free cells using high mass-loading cathodes. This work provides a simple interphase engineering strategy through regulating the electrolyte solvation structures for high-energy-density LMBs.     

Substituent Effect to Fine-Tune Energy Levels of Atom-Precise [MoOS3]2− Modified Copper(I) Thiolate Clusters Boosting Recyclable Photocatalysis

The propulsion of photocatalytic hydrogen (H₂) production is limited by the rational design and regulation of catalysts with precise structures and excellent activities. In this work, the [MoOS₃]²⁻ unit is introduced into the Cu^I clusters to form a series of atomically-precise Mo^VI−Cu^I bimetallic clusters of [Cu₆(MoOS₃)₂(C₆H₅(CH₂)S)₂(P(C₆H₄−R)₃)₄] ⋅ xCH₃CN (R=H, CH₃, or F), which show high photocatalytic H₂ evolution activities and excellent stability. By electron push-pull effects of the surface ligand, highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) levels of these Mo^VI−Cu^I clusters can be finely tuned, promoting the resultant visible-light-driven H₂ evolution performance. Furthermore, Mo^VI−Cu^I clusters loaded onto the surface of magnetic Fe₃O₄ carriers significantly reduced the loss of catalysts in the collection process, efficiently addressing the recycling issues of such small cluster-based catalyst. This work not only highlights a competitively universal approach on the design of high-efficiency cluster photocatalysts for energy conversion, but also makes it feasible to manipulate the catalytic performance of clusters through a rational substituent strategy.     

High‐performance thin film composite membranes with well‐defined poly(dimethylsiloxane)‐b‐poly(ethylene glycol) copolymer additives for CO2 separation

A series of well‐defined diblock copolymers (BCPs) consisting of poly(ethylene glycol) (PEG) and poly(dimethylsiloxane) (PDMS) were synthesized and blended with commercially available PEBAX® 2533 to form the active layer of thin‐film composite (TFC) membranes, via spin‐coating. BCPs with a PEG component ranging from 1 to 10 kDa and a PDMS component ranging from 1 to 10 kDa were synthesized by a facile condensation reaction of hydroxyl terminated PEG and carboxylic acid functionalized PDMS. The BCP/PEBAX® 2533 blends up to 50 wt % on cross‐linked PDMS gutter layers were tested at 35 °C and 350 kPa. TFC membranes containing BCPs of 1 kDa PEG and 1–5 kDa PDMS produced optimal results with CO₂ permeances of approximately 1000 GPU which is an increase up to 250% of the permeance of pure PEBAX® 2533 composite membranes, while maintaining a CO₂/N₂ selectivity of 21. © 2015 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2015 , 53, 1500–1511     

Two‐Dimensional Metal–Organic Framework Nanosheets for Membrane‐Based Gas Separation

Metal–organic framework (MOF) nanosheets could serve as ideal building blocks of molecular sieve membranes owing to their structural diversity and minimized mass‐transfer barrier. To date, discovery of appropriate MOF nanosheets and facile fabrication of high performance MOF nanosheet‐based membranes remain as great challenges. A modified soft‐physical exfoliation method was used to disintegrate a lamellar amphiprotic MOF into nanosheets with a high aspect ratio. Consequently sub‐10 nm‐thick ultrathin membranes were successfully prepared, and these demonstrated a remarkable H₂/CO₂ separation performance, with a separation factor of up to 166 and H₂ permeance of up to 8×10⁻⁷ mol m⁻² s⁻¹ Pa⁻¹ at elevated testing temperatures owing to a well‐defined size‐exclusion effect. This nanosheet‐based membrane holds great promise as the next generation of ultrapermeable gas separation membrane.     

Mixed Cu2Se Hexagonal Nanosheets@Co3Se4 Nanospheres for High-Performance Asymmetric Supercapacitors

Rational designing and constructing multiphase hybrid electrode materials is an effective method to compensate for the performance defects of the single component. Based on this strategy, Cu₂Se hexagonal nanosheets@Co₃Se₄ nanospheres mixed structures have been fabricated by a facile two-step hydrothermal method. Under the synergistic effect of the high ionic conductivity of Cu₂Se and the remarkable cycling stability of Co₃Se₄, Cu₂Se@Co₃Se₄ can exhibit outstanding electrochemical performance as a novel electrode material. The as-prepared Cu₂Se@Co₃Se₄ electrode displays high specific capacitance of 1005 F g⁻¹ at 1 A g⁻¹ with enhanced rate capability (56 % capacitance retention at 10 A g⁻¹), and ultralong lifespan (94.2 % after 10 000 cycles at 20 A g⁻¹). An asymmetric supercapacitor is assembled applying the Cu₂Se@Co₃Se₄ as anode and graphene as cathode, which delivers a wide work potential window of 1.6 V, high energy density (30.9 Wh kg⁻¹ at 0.74 kW kg⁻¹), high power density (21.0 Wh kg⁻¹ at 7.50 kW kg⁻¹), and excellent cycling stability (85.8 % after 10 000 cycles at 10 A g⁻¹).     

Dimensional and Optoelectronic Tuning of Lead-free Perovskite Cs3Bi2I9−nBrn Single Crystals for Enhanced Hard X-ray Detection

Inorganic Bi-based perovskites have shown great potential in X-ray detection for their large absorption to X-rays, diverse low-dimensional structures, and eco-friendliness without toxic metals. However, they suffer from poor carrier transport properties compared to Pb-based perovskites. Here, we propose a mixed-halogen strategy to tune the structural dimensions and optoelectronic properties of Cs₃Bi₂I_9−nBr_n (0≤n≤9). Ten centimeter-sized single crystals are successfully grown by the Bridgman technique. Upon doping bromine to zero-dimensional Cs₃Bi₂I₉, the crystal transforms into a two-dimensional structure as the bromine content reaches Cs₃Bi₂I₈Br. Correspondingly, the optoelectronic properties are adjusted. Among these crystals, Cs₃Bi₂I₈Br exhibits negligible ion migration, moderate resistivity, and the best carrier transport capability. The sensitivities in 100 keV hard X-ray detection are 1.33×10⁴ and 1.74×10⁴ μC Gy_air⁻¹ cm⁻² at room temperature and 75 °C, respectively, which are the highest among all reported bismuth perovskites. Moreover, the lowest detection limit of 28.6 nGy_air s⁻¹ and ultralow dark current drift of 9.12×10⁻⁹ nA cm⁻¹ s⁻¹ V⁻¹ are obtained owing to the high ionic activation energy. Our work demonstrates that Br incorporation is an effective strategy to enhance the X-ray detection performance by tuning the dimensional and optoelectronic properties.     

Synthesis of crosslinked PEG/IL blend membrane via one-pot thiol–ene/epoxy chemistry

Poly(ethylene glycol) (PEG)-based membranes have obtained considerable attentions for CO₂ separation for their promising CO₂ separation performance and excellent thermal/chemical resistance. In this work, a one-pot thiol–ene/epoxy reaction was used to prepare crosslinked PEG-based and PEG/ionic liquids (ILs) blend membranes. Four ILs of the same cation [Bmim]⁺ with different anions ([BF₄]⁻, [PF₆]⁻, [NTf₂]⁻, and [TCM]⁻) were chosen as the additives. The chemical structure, thermal properties, hydrophilicity, and permeation performance of the resultant membranes were investigated to study the ILs' effects. An increment in CO₂ permeability (~34%) was obtained by optimizing monomer ratios and thus crosslinking network structures. Adding ILs into optimized PEG matrix shows distinct influences in CO₂ separation performance depending on the anions' types, due to the different CO₂ affinities and compatibilities with PEG matrix. Among these ILs, [Bmim][NTf₂] was found the most effective in enhancing CO₂ transport by simultaneously increasing the solubility and diffusivity of CO₂. © 2020 The Authors. Journal of Polymer Science published by Wiley Periodicals LLC. J. Polym. Sci. 2020 , 58, 2575-2585