Layered double hydroxide (LDH) is considered a highly promising electrode material for supercapacitors (SCs) due to its high theoretical specific capacitance. However, LDH powders often suffer from poor electrical conductivity, structure pulverization, slow charge transport, and insufficient active sites. Herein, a self‐supporting electrode with a Mott–Schottky heterostructure has been designed for high‐performance SCs. The electrode consists of low crystallinity NiCo‐LDH nanosheets and vertical graphene (VG) directly grown on carbon cloth. The LDH was converted from a metal–organic framework (MOF) by the sol–gel method. This self‐supporting electrode provides fast charge transfer, reducing the pulverization effect and energy barrier. The Mott–Schottky heterostructure of LDH@VG regulates electron density and enhances electron transfer, as confirmed by density functional theory calculation. The optimized LDH@VG heterostructure electrode exhibits an excellent areal capacitance of 5513.8 mF cm⁻² and rate capability of 82.1%. Furthermore, the fabricated hybrid SC demonstrates excellent energy density of 404.8 μWh cm⁻² at 1.6 mW cm⁻² and a remarkable cycling life, with a capacitance of 92.0% after 10 000 cycles. This work not only provides a simple dip‐coating and MOF conversion method to synthesize heterojunction‐based electrodes, but also broadens the horizon for designing advanced electrode materials for SCs.

Fillers play a critical role in the performance of mixed matrix membranes (MMMs). Microporous metal azolate frameworks (MAFs) are a subclass material of metal–organic frameworks (MOFs). Due to the uncoordinated nitrogen of the organic ligands, MAF-7 (SOD-[Zn(mtz)₂], Hmtz = 3-methyl-1,2,4-triazole, window: d = 0.34 nm) shows excellent CO₂ adsorption performance. In this work, Pebax 1657/MAF-7 MMMs were prepared by a sample solution casting method with MAF-7 particles as fillers for the first time. By means of X-ray diffraction (XRD), scanning electron microscope (SEM), infrared radiation (IR), and thermogravimetry (TG), the compositional and structural properties of the mixed matrix membrane with different filler content were analyzed. The results show that the compatibility of MAF-7 and Pebax is good with a filler content of 5 wt.%. The pure gas testing showed that mixed matrix membrane has a high ideal CO₂/N₂ selectivity of 124.84 together with a better CO₂ permeability of 76.15 Barrer with the optimized filler content of 5 wt.%. The obtained membrane showed 323.04% enhancement in selectivity of CO₂/N₂ and 27.74% increase in the permeability of CO₂ compared to the pristine membrane at 25 °C and 3 bar. The excellent separation performance may be due to the ligands that can afford a Lewis base active site for CO₂ binding with the uniform dispersion of MAF-7 particles in Pebax and the favorable interface compatibility. The obtained membrane overcomes the Robeson’s upper bound in 2008 for CO₂/N₂ separation. This work provides a new strategy by utilizing MAFs as fillers with triazole ligand to enhance the gas separation performance of mixed matrix membranes.

The development of efficient and metal-free heterogeneous catalysts for the chemical fixation of CO₂ into value-added products is still a challenge. Herein, we reported two kinds of polar group (−COOH, −OH)-functionalized porous ionic polymers (PIPs) that were constructed from the corresponding phosphonium salt monomers (v-PBC and v-PBH) using a solvothermal radical polymerization method. The resulting PIPs (POP-PBC and POP-PBH) can be used as efficient bifunctional heterogeneous catalysts in the cycloaddition reaction of CO₂ with epoxides under relatively low temperature, ambient pressure, and metal-free conditions without any additives. It was found that the catalytic activities of the POP-PBC and POP-PBH were comparable with the homogeneous catalysts of Me-PBC and PBH and were higher than that of the POP-PPh₃-COOH that was synthesized through a post-modification method, indicating the importance of the high concentration catalytic active sites in the heterogeneous catalysts. Reaction under low CO₂ concentration conditions showed that the activity of the POP-PBC (with a conversion of 53.8% and a selectivity of 99.0%) was higher than that of the POP-PBH (with a conversion of 32.3% and a selectivity of 99.0%), verifying the promoting effect of the polar group (−COOH group) in the porous framework. The POP-PBC can also be recycled at least five times without a significant loss of catalytic activity, indicating the high stability and robustness of the PIPs-based heterogeneous catalysts.