Ultrahigh Metal-Organic Framework Loading and Flexible Nanofibrous Membranes for Efficient CO2 Capture with Long-Term, Ultrastable Recyclability

In the global transition to a sustainable low carbon economy, CO2 capture and storage technology plays a key role in reducing emissions. Metal-organic frameworks (MOFs) are crystalline materials with ultrahigh porosity, tunable pore size, and rich functionalities, holding the promise for CO2 capture. However, the intrinsic fragility and depressed processability of MOF crystals make the fabrication of the flexible MOF nanofibrous membrane (NFM) rather challenging. Herein, we demonstrate an effective strategy for the versatile preparation of self-supported and flexible HKUST-1 NFM with ultrahigh HKUST-1 loading (up to 82 wt %) and stable and uniform HKUST-1 growth through the combination of electrospinning, multistep seeded growth, and activation process. The loading rate of MOF is the highest level among the reported analogues. Significantly, the HKUST-1 NFM exhibits a prominent CO2 adsorption capacity of 3.9 mmol g(-1), good CO2/N-2 selectivity, and remarkable recyclability. The CO2 capacity retains similar to 95% (3.7 mmol g(-1)) of the initial value after 100 adsorption-desorption cycles, indicating that the HKUST-1 NFM has long-term and ultrastable recyclability and a significant practical value. Thus, the low-cost and scalable production pathway is able to convert MOF particles into self-supported and flexible NFMs, and thereby, they are better applied to the efficient postcombustion CO2 capture.