Programmed fluorine binding engineering in anion-pillared metal-organic framework for record trace acetylene capture from ethylene.
basic_science · Level V
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- Record sourced from PubMed, PMID 37540740.
- Also identified by DOI 10.1126/sciadv.adh0135 and PMC identifier 10403210.
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Abstract
Porous physisorbents are attractive candidates for selective capture of trace gas or volatile compounds due to their low energy footprints. However, many physisorbents suffer from insufficient sorbate-sorbent interactions, resulting in low uptake or inadequate selectivity when gases are present at trace levels. Here, we report a strategy of programmed fluorine binding engineering in anion-pillared metal-organic frameworks to maximize C<sub>2</sub>H<sub>2</sub> binding affinity for benchmark trace C<sub>2</sub>H<sub>2</sub> capture from C<sub>2</sub>H<sub>4</sub>. A robust material (ZJU-300a) was elaborately designed to provide multiple-site fluorine binding model, resulting in an ultrastrong C<sub>2</sub>H<sub>2</sub> binding affinity. ZJU-300a exhibits a record-high C<sub>2</sub>H<sub>2</sub> uptake of 3.23 millimoles per gram (at 0.01 bar and 296 kelvin) and one of the highest C<sub>2</sub>H<sub>2</sub>/C<sub>2</sub>H<sub>4</sub> selectivity (1672). The adsorption binding of C<sub>2</sub>H<sub>2</sub> and C<sub>2</sub>H<sub>4</sub> was visualized by gas-loaded ZJU-300a structures. The separation capacity was confirmed by breakthrough experiments for 1/99 C<sub>2</sub>H<sub>2</sub>/C<sub>2</sub>H<sub>4</sub> mixtures, affording the maximal dynamic selectivity (264) and C<sub>2</sub>H<sub>4</sub> productivity of 436.7 millimoles per gram.