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Nano Research 2023, 16(5): 6113-6119 https://doi.org/10.1007/s12274-022-5028-5
Research Article | Issue | Published: 03 November 2022

Water boosted CO2/C2H2 separation in L-arginine functionalized metal–organic framework

Show Author's Information Hejin Zhu1,3,  Wenjuan Xue1,2,  Hongliang Huang1,2( ),  Lvyun Chen1,3,  Haoyu Liu1,2,  Chongli Zhong1,2,3( )
State Key Laboratory of Separation Membranes and Membrane Processes, Tiangong University, Tianjin 300387, China
Country School of Chemistry and Chemical Engineering, Tiangong University, Tianjin 300387, China
School of Material Science and Engineering, Tiangong University, Tianjin 300387, China
Keywords:
moisture, CO2 adsorption, metal–organic frameworks, L-arginine, acetylene (C2H2) purification
Topics:
Organic frameworks
Cite this article:
Zhu H, Xue W, Huang H, et al. Water boosted CO2/C2H2 separation in L-arginine functionalized metal–organic framework. Nano Research, 2023, 16(5): 6113-6119. https://doi.org/10.1007/s12274-022-5028-5
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Abstract Full text Electronic supplementary material About this article

The separation of CO2/C2H2 mixture by CO2-selective sorbents is an energy-efficient C2H2 purification technique, but is strategically challenging due to their similar molecular size and physicochemical properties. Meanwhile, water is inevitable in CO2/C2H2 mixture and it is usually a significant barrier because of its competitive adsorption with CO2. To address this challenge, herein, we report the first example of metal–organic framework (MOF) that exhibits water-boosted CO2 adsorption and CO2/C2H2 separation by anchoring L-arginine (ARG) on the Zr6 cluster of MOF-808. The CO2 affinity and capacity in the resulting MOF-808-ARG are markedly facilitated by the presence of water, while the C2H2 adsorption is significantly suppressed. Specifically, CO2 adsorption capacities in adsorption isotherm and breakthrough measurement are increased to 143% and 184%, respectively. In addition, the wet MOF-808-ARG exhibits the record CO2/C2H2 selectivity of 1,180 under zero coverage. Breakthrough experiments reveal that CO2/C2H2 mixture can be completely separated and the result of mass spectrometry indicates that the C2H2 purity in the outlet is up to 99.9%. In situ infrared (IR) results and density functional theory (DFT) calculations reveal the water-promoted CO2 adsorption mechanism that the formation of bicarbonate products in the presence of water is thermodynamically and kinetically more favorable than that without water. Moreover, MOF-808-ARG also possesses excellent water stability and excellent regeneration of CO2 adsorption. This work provides a new paradigm by transforming the negative effects of water into positive ones for CO2/C2H2 separation.


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Electronic supplementary material
About this article

Water boosted CO2/C2H2 separation in L-arginine functionalized metal–organic framework

Show Author's information Hejin Zhu1,3, Wenjuan Xue1,2, Hongliang Huang1,2( ), Lvyun Chen1,3, Haoyu Liu1,2, Chongli Zhong1,2,3( )
State Key Laboratory of Separation Membranes and Membrane Processes, Tiangong University, Tianjin 300387, China
Country School of Chemistry and Chemical Engineering, Tiangong University, Tianjin 300387, China
School of Material Science and Engineering, Tiangong University, Tianjin 300387, China

Abstract

The separation of CO2/C2H2 mixture by CO2-selective sorbents is an energy-efficient C2H2 purification technique, but is strategically challenging due to their similar molecular size and physicochemical properties. Meanwhile, water is inevitable in CO2/C2H2 mixture and it is usually a significant barrier because of its competitive adsorption with CO2. To address this challenge, herein, we report the first example of metal–organic framework (MOF) that exhibits water-boosted CO2 adsorption and CO2/C2H2 separation by anchoring L-arginine (ARG) on the Zr6 cluster of MOF-808. The CO2 affinity and capacity in the resulting MOF-808-ARG are markedly facilitated by the presence of water, while the C2H2 adsorption is significantly suppressed. Specifically, CO2 adsorption capacities in adsorption isotherm and breakthrough measurement are increased to 143% and 184%, respectively. In addition, the wet MOF-808-ARG exhibits the record CO2/C2H2 selectivity of 1,180 under zero coverage. Breakthrough experiments reveal that CO2/C2H2 mixture can be completely separated and the result of mass spectrometry indicates that the C2H2 purity in the outlet is up to 99.9%. In situ infrared (IR) results and density functional theory (DFT) calculations reveal the water-promoted CO2 adsorption mechanism that the formation of bicarbonate products in the presence of water is thermodynamically and kinetically more favorable than that without water. Moreover, MOF-808-ARG also possesses excellent water stability and excellent regeneration of CO2 adsorption. This work provides a new paradigm by transforming the negative effects of water into positive ones for CO2/C2H2 separation.

Keywords: moisture, CO2 adsorption, metal–organic frameworks, L-arginine, acetylene (C2H2) purification

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Publication history
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Acknowledgements

Publication history

Received: 22 June 2022
Revised: 26 August 2022
Accepted: 08 September 2022
Published: 03 November 2022
Issue date: May 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by National Natural Science Foundation of China (Nos. 22038010, 22141001, and 21978212) and the Science and Technology Plans of Tianjin (Nos. 21ZYJDJC00040 and 20ZYJDJC00110).

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