Yaqiang Xie

Poly(ionic liquid)s (PILs) are versatile materials with wide-ranging applications, yet the use of porous PILs for adsorbing perfluoroalkyl and polyfluoroalkyl substances (PFASs) has been scarcely reported. Herein, we report a series of imidazolium-based mesoporous PILs for the removal of PFASs through multiple interaction mechanisms. Among them, PDB-F, synthesized via free-radical copolymerization of divinylbenzene (DVB) and 3-(4,4,4-trifluorobutyl)-1-vinyl-1H-3-imidazolium bromide (F-VBIm) at a 1:1 mol ratio, exhibited an exceptional adsorption capacity (2471.7 mg/g at 25 °C) for perfluorooctanoic acid (PFOA), ranking it among the most effective polymer-based adsorbents to date. Comprehensive structural characterization and performance studies revealed that the outstanding PFASs adsorption by PDB-F arises from the synergistic effects of electrostatic, hydrophobic, pore filling, and fluorophilic (F-F) interactions. Moreover, PDB-F demonstrated high efficacy in removing trace-level PFOA across different water matrices along with versatility for several common PFASs. Besides, PDB-F displayed good regeneration and remarkable reusability. This work offers valuable insights into the role of synergistic interactions in PFASs adsorption and lays the foundation for the rational design of high-performance adsorbents in the future.

CoP is considered as an efficient electrocatalyst for the hydrogen evolution reaction (HER) in acidic electrolytes but its performance in alkaline solutions is generally poor because of its slow reaction kinetics, which further limits its application in overall water splitting. Herein, we demonstrate a strategy to greatly accelerate its HER and OER kinetics in alkaline solutions through Mn incorporation. Ternary Mn_xCo_1−xP microcubes with a tunable Mn/Co ratio strongly anchored on rGO were synthesized using Prussian blue analogues as precursors. The synergy between the high activity of Mn_xCo_1−xP microcubes and the good conductivity of rGO leads to the superior performance of the hybrid toward water splitting in 1 M KOH. The optimized Mn_0.6Co_0.4P–rGO electrocatalyst shows high activity and stability towards both the HER and OER with low overpotentials of 54 and 250 mV at 10 mA cm⁻², respectively. Furthermore, the water electrolyzer using Mn_0.6Co_0.4P–rGO as both the cathode and anode only requires a cell voltage as low as 1.55 V to reach a current density of 10 mA cm⁻², making Mn_0.6Co_0.4P–rGO a competitive and cost-effective electrocatalyst for water splitting.

Hypercrosslinked MPILs with high ionic density and excellent textural properties were prepared for efficient simultaneous CO₂ adsorption and cycloaddition.

The design and synthesis of metal–organic frameworks (MOFs) enclosed with multiple catalytic active sites is favorable for cooperative catalysis, but is is still challenging. Herein, we developed a sequential postsynthetic ionization and metalation strategy to prepare bifunctional multivariate Zr-MOFs incorporating zinc porphyrin and imidazolium functionalities. Using this facile strategy, tetratopic [5,10,15,20-tetrakis(4-carboxyphenyl)porphyrinato]zinc(II) (ZnTCPP) ligands were successfully installed into the cationic Zr-MOF to obtain ZnTCPP⊂(Br^–)Etim-UiO-66. These MTV-MOFs, including TCPP⊂Im-UiO-66, TCPP⊂(Br^–)Etim-UiO-66, and ZnTCPP⊂(Br^–)Etim-UiO-66, were well characterized and used in CO₂ capture and conversion into cyclic carbonate from allyl glycidyl ether and CO₂ under cocatalyst-free and 1 bar CO₂ pressure conditions. It was found that the structural features and CO₂ affinity properties of these MTV-MOFs can be tuned by introducing imidazolium groups or doping zinc sites. Additionally, ZnTCPP⊂(Br^–)Etim-UiO-66 exhibited enhanced catalytic activities compared to other MTV-MOFs herein for obtaining the 3-allyloxy-1,2-proplyene carbonate product, which was attributed to the cooperative effect of Zn²⁺ sites and Br^– ions in this microporous ionic MTV-MOF. ZnTCPP⊂(Br^–)Etim-UiO-66 can be recycled easily and used at least three times.

A mesoporous cationic Cr-based metal–organic framework (MOF), FJI-C10, has been obtained and exhibited excellent performances in chemical fixation of CO₂ into cyclic carbonates under co-catalyst free and mild conditions.

Novel sponge-like ammonium-based PILs with rich exposed anion, excellent textural properties, and CO₂ adsorption were prepared for efficient CO₂ cycloaddition.