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

doi:10.1021/acsami.9b01423

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 journal › Article › peer-review

60 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 language	English (US)
Pages (from-to)	10680-10688
Number of pages	9
Journal	ACS Applied Materials and Interfaces
Volume	11
Issue number	11
DOIs	https://doi.org/10.1021/acsami.9b01423
State	Published - Mar 20 2019

Keywords

IAST selectivity
SO capture
desulfurization
polar sites
reversible

ASJC Scopus subject areas

General Materials Science

Access to Document

10.1021/acsami.9b01423

Cite this

@article{164b41b449c546399b43be0440885fe8,

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

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.",

keywords = "IAST selectivity, SO capture, desulfurization, polar sites, reversible",

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

note = "Publisher Copyright: {\textcopyright} 2019 American Chemical Society.",

year = "2019",

month = mar,

day = "20",

doi = "10.1021/acsami.9b01423",

language = "English (US)",

volume = "11",

pages = "10680--10688",

journal = "ACS Applied Materials and Interfaces",

issn = "1944-8244",

publisher = "American Chemical Society",

number = "11",

}

TY - JOUR

T1 - Highly Selective and Reversible Sulfur Dioxide Adsorption on a Microporous Metal-Organic Framework via Polar Sites

AU - Zhang, Yan

AU - Zhang, Peixin

AU - Yu, Weikang

AU - Zhang, Jinghan

AU - Huang, Jiejing

AU - Wang, Jun

AU - Xu, Mai

AU - Deng, Qiang

AU - Zeng, Zheling

AU - Deng, Shuguang

PY - 2019/3/20

Y1 - 2019/3/20

N2 - 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.

AB - 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.

KW - IAST selectivity

KW - SO capture

KW - desulfurization

KW - polar sites

KW - reversible

UR - http://www.scopus.com/inward/record.url?scp=85062863411&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85062863411&partnerID=8YFLogxK

U2 - 10.1021/acsami.9b01423

DO - 10.1021/acsami.9b01423

M3 - Article

C2 - 30807083

AN - SCOPUS:85062863411

SN - 1944-8244

VL - 11

SP - 10680

EP - 10688

JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

IS - 11

ER -

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

Abstract

Keywords

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Cite this