Liquefied natural gas coupled with adsorbed natural gas charging (LNG-ANG) offers an efficient solution for recycling boil-off gas, providing a promising strategy for the competent storage and transportation of natural gas. The key challenge in LNG-ANG coupling systems is identifying adsorbents that exhibit superior methane adsorption performance and excellent stability under cryogenic conditions (∼159 K). In this work, we systematically investigated the methane adsorption performance of a stable metal–organic framework, PCN-250-Fe2Ni, under LNG-ANG related conditions. The results demonstrated that PCN-250-Fe2Ni exhibited a high methane capacity of 286 cm3 (standard temperature and pressure, STP) cm−3 (0.227 g g−1) at 6 bar/159 K. Furthermore, the pellet composite of PCN-250-Fe2Ni and polyvinyl butyral also displayed a high methane adsorption capacity with excellent cycling stability. Combined with grand canonical Monte Carlo simulations, our findings revealed that the cage-type pores serve as initial methane adsorption sites, followed by the channel-type pores, both of which contribute to the framework’s high low-temperature methane storage performance at saturation.
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