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Semiconducting single-walled carbon nanotubes (s-SWCNTs) are the foundation of CNT-based electronics and optoelectronics. For practical applications, s-SWCNTs should be produced with high purity, high structural quality, low cost, and high yield. Currently conjugated polymer wrapping method shows great potential to fulfill these requirements due to its advantages of simple operation process, high purity separation, and easy scaling-up. However, only a small portion of both CNTs and polymers go into the final solution, and most of them are discarded after a single use, resulting in high cost and low yield. In this paper, we introduce a closed-loop recycling strategy, in which raw materials (CNTs and polymers) and solvents were all recycled and reused for multiple separation cycles. In each cycle, high-purity (> 99.9%) s-SWCNTs were obtained with no significant change of structural quality. After 7 times of recycling and separation, the material cost was reduced to ~ 1% in comparison with commercially available products, and total yield was increased to 36% in comparison with 2%–5% for single cycle separation. Our proposed closed-loop recycling strategy paves the way for low-cost and high-yield mass production of high-quality s-SWCNTs.


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High-yield and low-cost separation of high-purity semiconducting single-walled carbon nanotubes with closed-loop recycling of raw materials and solvents

Show Author's information Fang Liu1,2Xingxing Chen1,2Haoming Liu1,3Jie Zhao1,2Meiqi Xi1,2Hongshan Xiao1,2Tongkang Lu1,2Yu Cao1,2,4,5( )Yan Li1,3,4,5Lianmao Peng1,2,4,5Xuelei Liang1,2,4,5( )
Center for Carbon-Based Electronics Peking University Beijing 100871 China
Key Laboratory for the Physics and Chemistry of Nanodevices Department of Electronics Peking University Beijing 100871 China
College of Chemistry and Molecular Engineering Peking University Beijing 100871 China
Shanxi Institute for Carbon-Based Thin Film Electronics Peking University (SICTFE-PKU) Taiyuan 030012 China
Taiyuan Laboratory for Carbon-Based Thin Film Electronics Taiyuan 030012 China

Abstract

Semiconducting single-walled carbon nanotubes (s-SWCNTs) are the foundation of CNT-based electronics and optoelectronics. For practical applications, s-SWCNTs should be produced with high purity, high structural quality, low cost, and high yield. Currently conjugated polymer wrapping method shows great potential to fulfill these requirements due to its advantages of simple operation process, high purity separation, and easy scaling-up. However, only a small portion of both CNTs and polymers go into the final solution, and most of them are discarded after a single use, resulting in high cost and low yield. In this paper, we introduce a closed-loop recycling strategy, in which raw materials (CNTs and polymers) and solvents were all recycled and reused for multiple separation cycles. In each cycle, high-purity (> 99.9%) s-SWCNTs were obtained with no significant change of structural quality. After 7 times of recycling and separation, the material cost was reduced to ~ 1% in comparison with commercially available products, and total yield was increased to 36% in comparison with 2%–5% for single cycle separation. Our proposed closed-loop recycling strategy paves the way for low-cost and high-yield mass production of high-quality s-SWCNTs.

Keywords: carbon nanotubes, low-cost, closed-loop recycling, high-yield, high purity

References(41)

1
Saito, R.; Dresselhaus, G.; Dresselhaus, M. S. Physical Properties of Carbon Nanotubes; Imperial College Press: London, 1998.https://doi.org/10.1142/p080
DOI
2
International Technology Roadmap for Semiconductors [Online]. https://www.semiconductors.org/resources/2015-international-technology-roadmap-for-semiconductors-itrs/ (accessed Apr 17, 2021).
3

Franklin, A. D. Nanomaterials in transistors: From high-performance to thin-film applications. Science 2015, 349, aab2750.

4

Arnold, M. S.; Green, A. A.; Hulvat, J. F.; Stupp, S. I.; Hersam, M. C. Sorting carbon nanotubes by electronic structure using density differentiation. Nat. Nanotechnol. 2006, 1, 60–65.

5

Liu, H. P.; Nishide, D.; Tanaka, T.; Kataura, H. Large-scale single- chirality separation of single-wall carbon nanotubes by simple gel chromatography. Nat. Commun. 2011, 2, 309.

6

Zheng, M.; Jagota, A.; Semke, E. D.; Diner, B. A.; Mclean, R. S.; Lustig, S. R.; Richardson, R. E.; Tassi, N. G. DNA-assisted dispersion and separation of carbon nanotubes. Nat. Mater. 2003, 2, 338–342.

7

Khripin, C. Y.; Fagan, J. A.; Zheng, M. Spontaneous partition of carbon nanotubes in polymer-modified aqueous phases. J. Am. Chem. Soc. 2013, 135, 6822–6825.

8

Nish, A.; Hwang, J. Y.; Doig, J.; Nicholas, R. J. Highly selective dispersion of single-walled carbon nanotubes using aromatic polymers. Nat. Nanotechnol. 2007, 2, 640–646.

9

Qiu, S.; Wu, K. J.; Gao, B.; Li, L. Q.; Jin, H. H.; Li, Q. W. Solution- processing of high-purity semiconducting single-walled carbon nanotubes for electronics devices. Adv. Mater. 2019, 31, 1800750.

10

Wang, H. L.; Bao, Z. N. Conjugated polymer sorting of semiconducting carbon nanotubes and their electronic applications. Nano Today 2015, 10, 737–758.

11

Fong, D.; Adronov, A. Recent developments in the selective dispersion of single-walled carbon nanotubes using conjugated polymers. Chem. Sci. 2017, 8, 7292–7305.

12

Lei, T.; Pochorovski, I.; Bao, Z. N. Separation of semiconducting carbon nanotubes for flexible and stretchable electronics using polymer removable method. Acc. Chem. Res. 2017, 50, 1096–1104.

13

Yang, F.; Wang, M.; Zhang, D. Q.; Yang, J.; Zheng, M.; Li, Y. Chirality pure carbon nanotubes: Growth, sorting, and characterization. Chem. Rev. 2020, 120, 2693–2758.

14

Lee, H. W.; Yoon, Y.; Park, S.; Oh, J. H.; Hong, S.; Liyanage, L. S.; Wang, H. L.; Morishita, S.; Patil, N.; Park, Y. J. et al. Selective dispersion of high purity semiconducting single-walled carbon nanotubes with regioregular poly(3-alkylthiophene)s. Nat. Commun. 2011, 2, 541.

15

Ding, J. F.; Li, Z.; Lefebvre, J.; Cheng, F. Y.; Dubey, G.; Zou, S.; Finnie, P.; Hrdina, A.; Scoles, L.; Lopinski, G. P. et al. Enrichment of large- diameter semiconducting SWCNTs by polyfluorene extraction for high network density thin film transistors. Nanoscale 2014, 6, 2328–2339.

16

Mistry, K. S.; Larsen, B. A.; Blackburn, J. L. High-yield dispersions of large-diameter semiconducting single-walled carbon nanotubes with tunable narrow chirality distributions. ACS Nano 2013, 7, 2231–2239.

17

Brady, G. J.; Joo, Y.; Wu, M. Y.; Shea, M. J.; Gopalan, P.; Arnold, M. S. Polyfluorene-sorted, carbon nanotube array field-effect transistors with increased current density and high on/off ratio. ACS Nano 2014, 8, 11614–11621.

18
http://www.carbonsolution.com/ (accessed Apr 17, 2021).
19
http://nanointegris.com/ (accessed Apr 17, 2021).
20
http://www.derthon.com/ (accessed Apr 17, 2021).
21
https://www.jkchemical.com (accessed Apr 17, 2021).
22

Graf, A.; Zakharko, Y.; Schießl, S. P.; Backes, C.; Pfohl, M.; Flavel, B. S.; Zaumseil, J. Large scale, selective dispersion of long single- walled carbon nanotubes with high photoluminescence quantum yield by shear force mixing. Carbon 2016, 105, 593–599.

23

Yu, X. Q.; Liu, D.; Kang, L. X.; Yang, Y.; Zhang, X. P.; Lv, Q. J.; Qiu, S.; Jin, H. H.; Song, Q. J.; Zhang, J. et al. Recycling strategy for fabricating low-cost and high-performance carbon nanotube TFT devices. ACS Appl. Mater. Interfaces 2017, 9, 15719–15726.

24

Gao, T. Z.; Lei, T.; Molina-Lopez, F.; Bao, Z. N. Enhanced process integration and device performance of carbon nanotubes via flocculation. Small Methods 2018, 2, 1800189.

25

Lei, T.; Chen, X. Y.; Pitner, G.; Wong, H. S. P.; Bao, Z. N. Removable and recyclable conjugated polymers for highly selective and high- yield dispersion and release of low-cost carbon nanotubes. J. Am. Chem. Soc. 2016, 138, 802–805.

26

Gu, J. T.; Han, J.; Liu, D.; Yu, X. Q.; Kang, L. X.; Qiu, S.; Jin, H. H.; Li, H. B.; Li, Q. W.; Zhang, J. Solution-processable high-purity semiconducting SWCNTs for large-area fabrication of high- performance thin-film transistors. Small 2016, 12, 4993–4999.

27

Dong, G. D.; Zhao, J.; Shen, L. J.; Xia, J. Y.; Meng, H.; Yu, W. H.; Huang, Q.; Han, H.; Liang, X. L.; Peng, L. M. Large-area and highly uniform carbon nanotube film for high-performance thin film transistors. Nano Res. 2018, 11, 4356–4367.

28

Zhao, J.; Shen, L. J.; Liu, F.; Zhao, P.; Huang, Q.; Han, H.; Peng, L. M.; Liang, X. L. Quality metrology of carbon nanotube thin films and its application for carbon nanotube-based electronics. Nano Res. 2020, 13, 1749–1755.

29
User's guide of cole parmer 750 watt ultrasonicator.
30

Barman, S. N.; LeMieux, M. C.; Baek, J.; Rivera, R.; Bao, Z. N. Effects of dispersion conditions of single-walled carbon nanotubes on the electrical characteristics of thin film network transistors. ACS Appl. Mater. Interfaces 2010, 2, 2672–2678.

31

O'Connell, M. J.; Bachilo, S. M.; Huffman, C. B.; Moore, V. C.; Strano, M. S.; Haroz, E. H.; Rialon, K. L.; Boul, P. J.; Noon, W. H.; Kittrell, C. et al. Band gap fluorescence from individual single-walled carbon nanotubes. Science 2002, 297, 593–596.

32

Tian, Y.; Jiang, H.; Laiho, P.; Kauppinen, E. I. Validity of measuring metallic and semiconducting single-walled carbon nanotube fractions by quantitative Raman spectroscopy. Anal. Chem. 2018, 90, 2517–2525.

33

Dresselhaus, M. S.; Dresselhaus, G.; Jorio, A.; Souza Filho, A. G.; Saito, R. Raman spectroscopy on isolated single wall carbon nanotubes. Carbon 2002, 40, 2043–2061.

34

Alam, M. A.; Pimparkar, N.; Kumar, S.; Murthy, J. Theory of nano­composite network transistors for macroelectronics applications. MRS Bull. 2006, 31, 466–470.

35

Ding, J.; Li, Z.; Lefebvre, J.; Cheng, F.; Dubey, G.; Zou, S.; Finnie, P.; Hrdina, A.; Scoles, L.; Lopinski, G. P.; Kingston, C. T.; Simard, B.; Malenfant, P. R. L. Enrichment of large-diameter semiconducting SWCNTs by polyfluorene extraction for high network density thin film transistors. Nanoscale 2014, 6, 2328–2339.

36

Wang, H.; Bao, Z. Conjugated polymer sorting of semiconducting carbon nanotubes and their electronic applications. Nano Today 2015, 10, 737–758.

37

Barman, S. N.; LeMieux, M. C.; Baek, J.; Rivera, R.; Bao, Z. Effects of dispersion conditions of single-walled carbon nanotubes on the electrical characteristics of thin film network transistors. Acs Appl Mater Inter 2010, 2, 2672–2678.

38

Lei, T.; Chen, X.; Pitner, G.; Wong, H. S. P.; Bao, Z. Removable and recyclable conjugated polymers for highly selective and high-yield dispersion and release of low-cost carbon nanotubes. J Am Chem Soc 2016, 138, 802–805.

39

Graf, A.; Zakharko, Y.; Schiessl, S. P.; Backes, C.; Pfohl, M.; Flavel, B. S.; Zaumseil, J. Large scale, selective dispersion of long single-walled carbon nanotubes with high photoluminescence quantum yield by shear force mixing. Carbon 2016, 105, 593–599.

40

Tian, Y.; Jiang, H.; Laiho, P.; Kauppinen, E. I. Validity of measuring metallic and semiconducting single-walled carbon nanotube fractions by quantitative raman spectroscopy. Anal Chem 2018, 90, 2517–2525.

41

Xia, J.; Zhao, J.; Meng, H.; Huang, Q.; Dong, G.; Zhang, H.; Liu, F.; Mao, D.; Liang, X.; Peng, L. Performance enhancement of carbon nanotube thin film transistor by yttrium oxide capping. Nanoscale 2018, 10, 4202–4208.

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Publication history
Copyright
Acknowledgements

Publication history

Received: 17 April 2021
Revised: 02 June 2021
Accepted: 08 June 2021
Published: 04 July 2021
Issue date: November 2021

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

This work was supported by the National Key Research and Development Program (Nos. 2016YFA0201902 and 2016YFA0201904), the National Natural Science Foundation of China (No. 51991341), Young Talents Program of Beijing (No. 2018000020028G349), and the Open Research Fund of Key Laboratory of Space Utilization, Chinese Academy of Sciences (No. LSU-KFJJ-2020-06).

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