Fully inverse adsorption enables one-step high-purity C<sub>2</sub>H<sub>2</sub> separation from ternary C2 mixtures in a robust porous crystal.

Zhang, Mingxing; Duan, Jingui; Feng, Yanfei; Bai, Junfeng · Nat Commun · 2025

basic_science · Level V

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Abstract

Direct harvesting of electronic-grade acetylene (C<sub>2</sub>H<sub>2</sub>) from ternary C2 mixtures is a great challenge due to the ubiquitous adsorption preference of conventional porous materials (C<sub>2</sub>H<sub>2</sub> > ethylene (C<sub>2</sub>H<sub>4</sub>) > ethane (C<sub>2</sub>H<sub>6</sub>)). Here, we report a strategy to reverse this selectivity by leveraging ligand functionalization in porous crystals. Through the incorporation of trifluoromethyl/methyl groups into a pyrazole-carboxylate linker, we engineer a series of MOF-5 analogs. The optimal material, NTU-98, fully reverses the adsorption trend of C2 hydrocarbons (C<sub>2</sub>H<sub>6</sub> > C<sub>2</sub>H<sub>4</sub> > C<sub>2</sub>H<sub>2</sub>), enabling direct production of C<sub>2</sub>H<sub>2</sub> with >99.99% purity from ternary feeds at room temperature in one-step. Combined density functional theory calculations and gas-loaded crystallographic analyses unveil the molecular mechanism: methyl groups precisely positioned within the cages enhance host-guest interactions with C<sub>2</sub>H<sub>4</sub> and C<sub>2</sub>H<sub>6</sub>, while suppressing the binding affinity for C<sub>2</sub>H<sub>2</sub>. This work presents a porous crystal for direct C<sub>2</sub>H<sub>2</sub> purification from ternary feeds and a blueprint for designing microporous environments targeting challenging separations.