Reversible coordinative binding and separation of sulfur dioxide in a robust metal-organic framework with open copper sites

被引：213

作者：

Smith, Gemma L. ^{[1
]}

Eyley, Jennifer E. ^{[1
]}

Han, Xue ^{[1
]}

Zhang, Xinran ^{[1
]}

Li, Jiangnan ^{[1
]}

Jacques, Nicholas M. ^{[1
]}

Godfrey, Harry G. W. ^{[1
]}

Argent, Stephen P. ^{[2
]}

McPherson, Laura J. McCormick ^{[3
]}

Teat, Simon J. ^{[3
]}

Cheng, Yongqiang ^{[4
]}

Frogley, Mark D. ^{[5
]}

Cinque, Gianfelice ^{[5
]}

Day, Sarah J. ^{[5
]}

Tang, Chiu C. ^{[5
]}

Easun, Timothy L. ^{[6
]}

Rudic, Svemir ^{[7
]}

Ramirez-Cuesta, Anibal J. ^{[4
]}

Yang, Sihai ^{[1
]}

Schroder, Martin ^{[1
]}

机构：

[1] Univ Manchester, Sch Chem, Manchester, Lancs, England

[2] Univ Nottingham, Sch Chem, Nottingham, England

[3] Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA USA

[4] Oak Ridge Natl Lab, Oak Ridge, TN USA

[5] Diamond Light Source, Harwell Sci Campus, Didcot, Oxon, England

[6] Cardiff Univ, Sch Chem, Cardiff, S Glam, Wales

[7] STFC Rutherford Appleton Lab, ISIS, Chilton, England

来源：

NATURE MATERIALS | 2019年 / 18卷 / 12期

基金：

英国工程与自然科学研究理事会;

关键词：

CARBON-DIOXIDE; CO2; CAPTURE; ADSORPTION; SO2; CAPACITY; CATALYST; REMOVAL; POLYMER; MOFS;

D O I：

10.1038/s41563-019-0495-0

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Emissions of SO2 from flue gas and marine transport have detrimental impacts on the environment and human health, but SO2 is also an important industrial feedstock if it can be recovered, stored and transported efficiently. Here we report the exceptional adsorption and separation of SO2 in a porous material, [Cu-2(L)] (H4L = 4',4'''-(pyridine-3,5-diyl)bis([1,1'-biphenyl]-3,5-dicarboxylic acid)), MFM-170. MFM-170 exhibits fully reversible SO2 uptake of 17.5 mmol g(-1) at 298 K and 1.0 bar, and the SO2 binding domains for trapped molecules within MFM-170 have been determined. We report the reversible coordination of SO2 to open Cu(ii ) sites, which contributes to excellent adsorption thermodynamics and selectivities for SO2 binding and facile regeneration of MFM-170 after desorption. MFM-170 is stable to water, acid and base and shows great promise for the dynamic separation of SO2 from simulated flue gas mixtures, as confirmed by breakthrough experiments.

引用

页码：1358 / +

页数：9

共 39 条

[1] ADSORPTION OF CARBON-DIOXIDE, SULFUR-DIOXIDE AND WATER-VAPOR BY MCM-41, A MODEL MESOPOROUS ADSORBENT [J].

BRANTON, PJ ;

HALL, PG ;

TREGUER, M ;

SING, KSW .

JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1995, 91 (13) :2041-2043

[2] Metal-organic frameworks with high capacity and selectivity for harmful gases [J].

Britt, David ;

Tranchemontagne, David ;

Yaghi, Omar M. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2008, 105 (33) :11623-11627

[3] Highly efficient separation of carbon dioxide by a metal-organic framework replete with open metal sites [J].

Britt, David ;

Furukawa, Hiroyasu ;

Wang, Bo ;

Glover, T. Grant ;

Yaghi, Omar M. .

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2009, 106 (49) :20637-20640

[4] Exceptional Adsorption and Binding of Sulfur Dioxide in a Robust Zirconium-Based Metal-Organic Framework [J].

Carter, Joseph H. ;

Han, Xue ;

Moreau, Florian Y. ;

da Silva, Ivan ;

Nevin, Adam ;

Godfrey, Harry G. W. ;

Tang, Chiu C. ;

Yang, Sihai ;

Schroder, Martin .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (46) :15564-15567

[5] Dramatic tuning of carbon dioxide uptake via metal substitution in a coordination polymer with cylindrical pores [J].

Caskey, Stephen R. ;

Wong-Foy, Antek G. ;

Matzger, Adam J. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (33) :10870-+

[6] Tunable Robust pats-MOFs: a Platform for Systematic Enhancement of the C2H2 Uptake and C2H2/C2H4 Separation Performance [J].

Chen, Di-Ming ;

Sun, Chun-Xiao ;

Zhang, Nan-Nan ;

Si, Huan-Huan ;

Liu, Chun-Sen ;

Du, Miao .

INORGANIC CHEMISTRY, 2018, 57 (05) :2883-2889

[7] Ultrahigh and Selective SO2 Uptake in Inorganic Anion-Pillared Hybrid Porous Materials [J].

Cui, Xili ;

Yang, Qiwei ;

Yang, Lifeng ;

Krishna, Rojamani ;

Zhang, Zhiguo ;

Bao, Zongbi ;

Wu, Hui ;

Ren, Qilong ;

Zhou, Wei ;

Chen, Banglin ;

Xing, Huabin .

ADVANCED MATERIALS, 2017, 29 (28)

[8] Significant Promotion Effect of Mo Additive on a Novel Ce-Zr Mixed Oxide Catalyst for the Selective Catalytic Reduction of NOx with NH3 [J].

Ding, Shipeng ;

Liu, Fudong ;

Shi, Xiaoyan ;

Liu, Kuo ;

Lian, Zhihua ;

Xie, Lijuan ;

He, Hong .

ACS APPLIED MATERIALS & INTERFACES, 2015, 7 (18) :9497-9506

[9] Gas-Induced Expansion and Contraction of a Fluorinated Metal-Organic Framework [J].

Fernandez, Carlos A. ;

Thallapally, Praveen K. ;

Motkuri, Radha Kishan ;

Nune, Satish K. ;

Sumrak, Joseph C. ;

Tian, Jian ;

Liu, Jun .

CRYSTAL GROWTH & DESIGN, 2010, 10 (03) :1037-1039

[10] Pilot-Scale Experimental Study on the CO2 Capture Process with Existing of SO2: Degradation, Reaction Rate, and Mass Transfer [J].

Gao, Jubao ;

Wang, Shujuan ;

Zhao, Bo ;

Qj, Guojie ;

Chen, Changhe .

ENERGY & FUELS, 2011, 25 (12) :5802-5809

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