Multiscale Co-Assembly to Meso-Macroporous Foamed Single-Crystal Metal–Organic Frameworks for the Supported Capture of Sulfur Dioxide

Xun Kan; Guanqing Zhang; Jun Ma; Fengqing Liu; Yu Tang; Fujian Liu; Xianfeng Yi; Yuefeng Liu; Anmin Zheng; Lilong Jiang; Feng Shou Xiao; Sheng Dai

doi:10.1002/adfm.202312044

Multiscale Co-Assembly to Meso-Macroporous Foamed Single-Crystal Metal–Organic Frameworks for the Supported Capture of Sulfur Dioxide

Xun Kan, Guanqing Zhang, Jun Ma, Fengqing Liu, Yu Tang, Fujian Liu, Xianfeng Yi, Yuefeng Liu, Anmin Zheng, Lilong Jiang, Feng Shou Xiao, Sheng Dai

Chemical Sciences Division

Research output: Contribution to journal › Article › peer-review

19 Scopus citations

Abstract

The introduction of enlarged and interconnected nanochannels into metal–organic frameworks (MOFs) overcome their micropore size restriction, enhances mass transportation, and improves the accessibility of anchored metal clusters. Herein, foamed Ce-MOF single crystals (F-Ce-MOF-SC-x) designed from a multiscale co-assembly is reported in the presence of a copolymer template and 1,3,5-trimethylbenzene as a structural regulator. The resultant F-Ce-MOF-SC-x possessed well-defined microporous tandem-ordered meso-macroporous foams with superior connectivity and versatile Ce-defective unsaturated sites (Ce-DUS). F-Ce-MOF-SC-x is applied as a stable carrier for anchoring polytertiary amines (PA) via coordination interactions with Ce-DUS. Owing to the superior ability of PA to recognize SO₂, the resultant F-Ce-MOF-SC-x@yPA delivers exceptional performance in terms of the high-temperature reversible adsorption and separation of SO₂, including a remarkable capacity for SO₂, spectacular selectivity for SO₂/CO₂/N₂, an ultrafast adsorption equilibrium rate, and stability for 50 cycles. These characteristics are outstanding among those of MOFs and superior to those of many reported SO₂ adsorbents.

Original language	English
Article number	2312044
Journal	Advanced Functional Materials
Volume	34
Issue number	19
DOIs	https://doi.org/10.1002/adfm.202312044
State	Published - May 10 2024

Funding

X.K., G.Z., and J.M. contributed equally to this work. This work was supported by the National Science Foundation of China (22221005, 22378064, 22022804, and 21978052), the Natural Science Foundation for Distinguished Young Scholars of Fujian Province (2020J06037), and the Major Program of Qingyuan Innovation Laboratory (00121003). The authors thank the staff at the BL14W1 beamline of the Shanghai Synchrotron Radiation Facility for the measurements of EXAFS and XANES.

Keywords

SO adsorption
foam nanostructure
macromolecule immobilization
metal–organic framework
multiscale assembly
separation

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title = "Multiscale Co-Assembly to Meso-Macroporous Foamed Single-Crystal Metal–Organic Frameworks for the Supported Capture of Sulfur Dioxide",

abstract = "The introduction of enlarged and interconnected nanochannels into metal–organic frameworks (MOFs) overcome their micropore size restriction, enhances mass transportation, and improves the accessibility of anchored metal clusters. Herein, foamed Ce-MOF single crystals (F-Ce-MOF-SC-x) designed from a multiscale co-assembly is reported in the presence of a copolymer template and 1,3,5-trimethylbenzene as a structural regulator. The resultant F-Ce-MOF-SC-x possessed well-defined microporous tandem-ordered meso-macroporous foams with superior connectivity and versatile Ce-defective unsaturated sites (Ce-DUS). F-Ce-MOF-SC-x is applied as a stable carrier for anchoring polytertiary amines (PA) via coordination interactions with Ce-DUS. Owing to the superior ability of PA to recognize SO2, the resultant F-Ce-MOF-SC-x@yPA delivers exceptional performance in terms of the high-temperature reversible adsorption and separation of SO2, including a remarkable capacity for SO2, spectacular selectivity for SO2/CO2/N2, an ultrafast adsorption equilibrium rate, and stability for 50 cycles. These characteristics are outstanding among those of MOFs and superior to those of many reported SO2 adsorbents.",

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author = "Xun Kan and Guanqing Zhang and Jun Ma and Fengqing Liu and Yu Tang and Fujian Liu and Xianfeng Yi and Yuefeng Liu and Anmin Zheng and Lilong Jiang and Xiao, {Feng Shou} and Sheng Dai",

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AU - Tang, Yu

AU - Liu, Fujian

AU - Yi, Xianfeng

AU - Liu, Yuefeng

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AB - The introduction of enlarged and interconnected nanochannels into metal–organic frameworks (MOFs) overcome their micropore size restriction, enhances mass transportation, and improves the accessibility of anchored metal clusters. Herein, foamed Ce-MOF single crystals (F-Ce-MOF-SC-x) designed from a multiscale co-assembly is reported in the presence of a copolymer template and 1,3,5-trimethylbenzene as a structural regulator. The resultant F-Ce-MOF-SC-x possessed well-defined microporous tandem-ordered meso-macroporous foams with superior connectivity and versatile Ce-defective unsaturated sites (Ce-DUS). F-Ce-MOF-SC-x is applied as a stable carrier for anchoring polytertiary amines (PA) via coordination interactions with Ce-DUS. Owing to the superior ability of PA to recognize SO2, the resultant F-Ce-MOF-SC-x@yPA delivers exceptional performance in terms of the high-temperature reversible adsorption and separation of SO2, including a remarkable capacity for SO2, spectacular selectivity for SO2/CO2/N2, an ultrafast adsorption equilibrium rate, and stability for 50 cycles. These characteristics are outstanding among those of MOFs and superior to those of many reported SO2 adsorbents.

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Multiscale Co-Assembly to Meso-Macroporous Foamed Single-Crystal Metal–Organic Frameworks for the Supported Capture of Sulfur Dioxide

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