Highly Selective and Reversible Sulfur Dioxide Adsorption on a Microporous Metal-Organic Framework via Polar Sites

Yan Zhang, Peixin Zhang, Weikang Yu, Jinghan Zhang, Jiejing Huang, Jun Wang, Mai Xu, Qiang Deng, Zheling Zeng, Shuguang Deng

Research output: Contribution to journalArticle

14 Scopus citations

Abstract

It is very challenging to achieve efficient and deep desulfurization, especially in flue gases with an extremely low SO 2 concentration. Herein, we report a microporous metal-organic framework (ELM-12) with specific polar sites and proper pore size for the highly efficient SO 2 removal from flue gas and other SO 2 -containing gases. A high SO 2 capacity of 61.2 cm 3 ·g -1 combined with exceptionally outstanding selectivity of SO 2 /CO 2 (30), SO 2 /CH 4 (871), and SO 2 /N 2 (4064) under ambient conditions (i.e., 10:90 mixture at 298 K and 1 bar) was achieved. Notably, the SO 2 /N 2 selectivity is unprecedented among ever reported values of porous materials. Moreover, the dispersion-corrected density functional theory calculations illustrated the superior SO 2 capture ability and selectivity arise from the high-density SO 2 binding sites of the CF 3 SO 3 - group in the pore cavity (S δ+ ···O δ- interactions) and aromatic linkers in the pore walls (H δ+ ···O δ- interactions). Dynamic breakthrough experiments confirm the regeneration stability and excellent separation performance. Furthermore, ELM-12 is also stable after exposure to SO 2 , water vapor, and organic solvents.

Original languageEnglish (US)
Pages (from-to)10680-10688
Number of pages9
JournalACS Applied Materials and Interfaces
Volume11
Issue number11
DOIs
StatePublished - Mar 20 2019

Keywords

  • desulfurization
  • IAST selectivity
  • polar sites
  • reversible
  • SO capture

ASJC Scopus subject areas

  • Materials Science(all)

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