From pore to process: ultra-efficient SF6/N2 continuous separation using inexpensive robust MOF composites

Abstract Physisorption presents a promising alternative to cryogenic distillation for capturing the most potent greenhouse gas, SF₆, but existing adsorbents face challenges in meeting diverse chemical and engineering concerns. Herein, with insights into in-pore chemistry and industrial process design, we report a systematic investigation that constructed two novel low-cost composites pellets (Al(fum)@2%HPC and Al(fum)@5%Kaolin) coupled with an innovative two-stage Vacuum Temperature Swing Adsorption (VTSA) process for the ultra-efficient recovery of low-concentration SF₆ from N₂. Record-high selectivities (> 2×10⁴) and SF₆ dynamic capacities (~2.7 mmol/g) were achieved, while exceptional SF₆ productivities (~58.7 L/kg), yields (~96.8%), and recyclability (~1000 cycles) were demonstrated in fixed-bed adsorption-desorption experiments under mild regeneration conditions. 2D solid-state NMR/in-situ FTIR, DFT-D binding/diffusion simulation analyses revealed the multi-site binding mode and the ultra-fast diffusion of SF₆ within the channels. The proposed VTSA processes successfully met the dual stringent requirements of both environmental protection and electricity equipment operation: the SF₆ recovery of 99.91% accompanied with a SF₆ purity/working capacity of 99.91%/2.1 mmol/g, which significantly outperformed the industrial employed adsorbent zeolite 13X and showed only 19% the energy consumption of the cryogenic distillation.