Metal-Organic Framework Based Hydrogen-Bonding Nanotrap for Efficient Acetylene Storage and Separation

The removal of carbon dioxide (CO2) from acetylene (C2H2) is a critical industrial process for manufacturing high-purity C2H2. However, it remains challenging to address the tradeoff between adsorption capacity and selectivity, on account of their similar physical properties and molecular sizes. To overcome this difficulty, here we report a novel strategy involving the regulation of a hydrogen-bonding nanotrap on the pore surface to promote the separation of C2H2/CO2 mixtures in three isostructural metal-organic frameworks (MOFs, named MIL-160, CAU-10H, and CAU-23, respectively). Among them, MIL-160, which has abundant hydrogen-bonding acceptors as nanotraps, can selectively capture acetylene molecules and demonstrates an ultrahigh C2H2 storage capacity (191 cm(3) g(-1), or 213 cm(3) cm(-3)) but much less CO2 uptake (90 cm(3) g(-1)) under ambient conditions. The C(2)H(2 )adsorption amount of MIL-160 is remarkably higher than those for the other two isostructural MOFs (86 and 119 cm(3) g(-1) for CAU-10H and CAU-23, respectively) under the same conditions. More importantly, both simulation and experimental breakthrough results show that MIL-160 sets a new benchmark for equimolar C2H2/CO2 separation in terms of the separation potential (Delta(qbreak) = 5.02 mol/kg) and C(2)H(2 )productivity (6.8 mol/kg). In addition, in situ FT-IR experiments and computational modeling further reveal that the unique host-guest multiple hydrogen-bonding interaction between the nanotrap and C(2)H(2 )is the key factor for achieving the extraordinary acetylene storage capacity and superior C2 H-2/CO2 selectivity. This work provides a novel and powerful approach to address the tradeoff of this extremely challenging gas separation.

Automated summary

This study introduces a novel strategy to promote the separation of C2H2/CO2 mixtures by regulating a hydrogen-bonding nanotrap on the pore surface of three isostructural metal-organic frameworks. Among them, MIL-160 demonstrates an ultrahigh C2H2 storage capacity and superior C2H2/CO2 selectivity due to its multiple hydrogen-bonding interaction with C2H2.