Affiliation:
1. College of Chemistry and Chemical Engineering Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization Taiyuan University of Technology Taiyuan 030024 Shanxi Province China
2. Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Taiyuan 030024 Shanxi Province China
Abstract
AbstractPorous materials with d3 electronic configuration open metal sites have been proved to be effective adsorbents for N2 capture and N2/O2 separation. However, the reported materials remain challenging to address the trade‐off between adsorption capacity and selectivity. Herein, we report a robust MOF, MIL‐102Cr, that features two binding sites, can synergistically afford strong interactions for N2 capture. The synergistic adsorption site exhibits a benchmark Qst of 45.0 kJ mol−1 for N2 among the Cr‐based MOFs, a record‐high volumetric N2 uptake (31.38 cm3 cm−3), and highest N2/O2 selectivity (13.11) at 298 K and 1.0 bar. Breakthrough experiments reveal that MIL‐102Cr can efficiently capture N2 from a 79/21 N2/O2 mixture, providing a record 99.99 % pure O2 productivity of 0.75 mmol g−1. In situ infrared spectroscopy and computational modelling studies revealed that a synergistic adsorption effect by open Cr(III) and fluorine sites was accountable for the strong interactions between the MOF and N2.
Funder
National Natural Science Foundation of China
Natural Science Foundation of Shanxi Province
Subject
General Chemistry,Catalysis
Cited by
2 articles.
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