Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 11, Issue 11, Pages 10680-10688Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b01423
Keywords
desulfurization; SO2 capture; polar sites; IAST selectivity; reversible
Funding
- National Natural Science Foundation of China [51672186]
- Nanchang University
- Arizona State University
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It is very challenging to achieve efficient and deep desulfurization, especially in flue gases with an extremely low SO2 concentration. Herein, we report a microporous metal organic framework (ELM-12) with specific polar sites and proper pore size for the highly efficient SO2 removal from flue gas and other SO2-containing gases. A high SO2 capacity of 61.2 cm(3).g(-1) combined with exceptionally outstanding selectivity of SO2/CO2 (30), SO2/CH4 (871), and SO2/N-2 (4064) under ambient conditions (i.e., 10:90 mixture at 298 K and 1 bar) was achieved. Notably, the SO2/N-2 selectivity is unprecedented among ever reported values of porous materials. Moreover, the dispersion-corrected density functional theory calculations illustrated the superior SO2 capture ability and selectivity arise from the high-density SO2 binding sites of the CF3SL3- group in the pore cavity (S delta+... O delta(-) interactions) and aromatic linkers in the pore walls (H delta+center dot center dot center dot O delta- interactions). Dynamic breakthrough experiments confirm the regeneration stability and excellent separation performance. Furthermore, ELM-12 is also stable after exposure to SO2, water vapor, and organic solvents.
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