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

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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.

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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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Authors and Affiliations

  1. State Key Laboratory of Separation Membranes and Membrane Processes, Tiangong University, Tianjin, 300387, China

    Hejin Zhu, Wenjuan Xue, Hongliang Huang, Lvyun Chen, Haoyu Liu & Chongli Zhong

  2. Country School of Chemistry and Chemical Engineering, Tiangong University, Tianjin, 300387, China

    Wenjuan Xue, Hongliang Huang, Haoyu Liu & Chongli Zhong

  3. School of Material Science and Engineering, Tiangong University, Tianjin, 300387, China

    Hejin Zhu, Lvyun Chen & Chongli Zhong

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  1. Hejin Zhu
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  2. Wenjuan Xue
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  3. Hongliang Huang
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  5. Haoyu Liu
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Correspondence to Hongliang Huang or Chongli Zhong.

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Zhu, H., Xue, W., Huang, H. et al. Water boosted CO2/C2H2 separation in L-arginine functionalized metal—organic framework. Nano Res. 16, 6113–6119 (2023). https://doi.org/10.1007/s12274-022-5028-5

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  • DOI: https://doi.org/10.1007/s12274-022-5028-5

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