Journal Home > Online First
Nano Research https://doi.org/10.1007/s12274-024-6456-1
Research Article | Online first | Published: 30 January 2024

Rational design multi-color-emissive chemiluminescent carbon nanodots in a single solvothermal reaction

Show Author's Information Guang-Song Zheng,  Cheng-Long Shen( ),  Yuan Deng,  Kai-Kai Liu,  Jin-Hao Zang,  Lin Dong,  Qing Lou( ),  Chong-Xin Shan( )
Henan Key Laboratory of Diamond Optoelectronic Materials and Devices, Key Laboratory of Materials Physics, Ministry of Education, and School of Physics and Microelectronics, Zhengzhou University, Zhengzhou 450052, China
Keywords:
carbon nanodots, mechanism, chemiluminescence, regulation, energy level alignment
Topics:
Graphene quantum dots
Cite this article:
Zheng G-S, Shen C-L, Deng Y, et al. Rational design multi-color-emissive chemiluminescent carbon nanodots in a single solvothermal reaction. Nano Research, 2024, https://doi.org/10.1007/s12274-024-6456-1
Download citation
EndNote(RIS)
BibTeX

332

Views

56

Downloads

Citations

0

Crossref

0

WoS

0

Scopus

0

CSCD

Abstract Full text Electronic supplementary material About this article

Recently, the chemiluminescence (CL) induced by carbon nanodots (CDs) has intrigued researchers’ extensive interests in various applications due to its special light emission principle. However, the difficulty of synthesizing chemiluminescent CDs with full-spectrum emission severely hinders the further regulation of the CL emission mechanism. Herein, the multi-color-emissive chemiluminescent CDs are rational designed and further synthesized by regulating the sp2-hybrid core and sp3-hybrid surface from the citrate-ammonia molecular in a single solvothermal reaction. More experimental characterizations and density functional theory calculations reveal that the higher temperature can promote the crosslinking polymerization/carbonization of carbon core and the higher protonation of solvent can determine the core size of final CDs, resulting in the variant CL emission from molecular-, crosslinking- and core-states. Thus, the CL emission of the CDs can be further synthesized by tuning the luminescence chromophores in the formation process via regulating the temperature and solvent, enabling the applications of the CL CDs in illumination and information encryption. This study paves a new technology to understand the luminescence of CDs and affords an industry translational potential over traditional chemiluminescent molecular.


menu
Abstract
Full text
Outline
Electronic supplementary material
About this article

Rational design multi-color-emissive chemiluminescent carbon nanodots in a single solvothermal reaction

Show Author's information Guang-Song Zheng, Cheng-Long Shen( ), Yuan Deng, Kai-Kai Liu, Jin-Hao Zang, Lin Dong, Qing Lou( ), Chong-Xin Shan( )
Henan Key Laboratory of Diamond Optoelectronic Materials and Devices, Key Laboratory of Materials Physics, Ministry of Education, and School of Physics and Microelectronics, Zhengzhou University, Zhengzhou 450052, China

Abstract

Recently, the chemiluminescence (CL) induced by carbon nanodots (CDs) has intrigued researchers’ extensive interests in various applications due to its special light emission principle. However, the difficulty of synthesizing chemiluminescent CDs with full-spectrum emission severely hinders the further regulation of the CL emission mechanism. Herein, the multi-color-emissive chemiluminescent CDs are rational designed and further synthesized by regulating the sp2-hybrid core and sp3-hybrid surface from the citrate-ammonia molecular in a single solvothermal reaction. More experimental characterizations and density functional theory calculations reveal that the higher temperature can promote the crosslinking polymerization/carbonization of carbon core and the higher protonation of solvent can determine the core size of final CDs, resulting in the variant CL emission from molecular-, crosslinking- and core-states. Thus, the CL emission of the CDs can be further synthesized by tuning the luminescence chromophores in the formation process via regulating the temperature and solvent, enabling the applications of the CL CDs in illumination and information encryption. This study paves a new technology to understand the luminescence of CDs and affords an industry translational potential over traditional chemiluminescent molecular.

Keywords: carbon nanodots, mechanism, chemiluminescence, regulation, energy level alignment

References(42)

[1]

Lou, Q.; Ni, Q. C.; Niu, C. Y.; Wei, J. Y.; Zhang, Z. F.; Shen, W. X.; Shen, C. L.; Qin, C. C.; Zheng, G. S.; Liu, K. K. et al. Carbon nanodots with nearly unity fluorescent efficiency realized via localized excitons. Adv. Sci. 2022, 9, 2203622.
DOI Google Scholar
[2]

Wang, B. Y.; Lu, S. Y. The light of carbon dots: From mechanism to applications. Matter 2022, 5, 110–149.
DOI Google Scholar
[3]

Ðorđević, L.; Arcudi, F.; Cacioppo, M.; Prato, M. A multifunctional chemical toolbox to engineer carbon dots for biomedical and energy applications. Nat. Nanotechnol. 2022, 17, 112–130.
DOI Google Scholar
[4]

Shi, Y. X.; Su, W.; Yuan, F. L.; Yuan, T.; Song, X. Z.; Han, Y. Y.; Wei, S. Y.; Zhang, Y.; Li, Y. C.; Li, X. H. et al. Carbon dots for electroluminescent light-emitting diodes: Recent progress and future prospects. Adv. Mater. 2023, 35, 2210699.
DOI Google Scholar
[5]

Yuan, F. L.; Li, S. H.; Fan, Z. T.; Meng, X. Y.; Fan, L. Z.; Yang, S. H. Shining carbon dots: Synthesis and biomedical and optoelectronic applications. Nano Today 2016, 11, 565–586.
DOI Google Scholar
[6]

Shen, C. L.; Lou, Q.; Zang, J. H.; Liu, K. K.; Qu, S. N.; Dong, L.; Shan, C. X. Near-infrared chemiluminescent carbon nanodots and their application in reactive oxygen species bioimaging. Adv. Sci. 2020, 7, 1903525.
DOI Google Scholar
[7]

Lou, Q.; Chen, N.; Zhu, J. Y.; Liu, K. K.; Li, C.; Zhu, Y. S.; Xu, W.; Chen, X.; Song, Z. J.; Liang, C. H. et al. Thermally enhanced and long lifetime red TADF carbon dots via multi-confinement and phosphorescence assisted energy transfer. Adv. Mater. 2023, 35, 2211858.
DOI Google Scholar
[8]

Vallan, L.; Urriolabeitia, E. P.; Ruipérez, F.; Matxain, J. M.; Canton-Vitoria, R.; Tagmatarchis, N.; Benito, A. M.; Maser, W. K. Supramolecular-enhanced charge transfer within entangled polyamide chains as the origin of the universal blue fluorescence of polymer carbon dots. J. Am. Chem. Soc. 2018, 140, 12862–12869.
DOI Google Scholar
[9]

Yuan, F. L.; Yuan, T.; Sui, L.; Wang, Z. B.; Xi, Z. F.; Li, Y. C.; Li, X. H.; Fan, L. Z.; Tan, Z.; Chen, A. M. et al. Engineering triangular carbon quantum dots with unprecedented narrow bandwidth emission for multicolored LEDs. Nat. Commun. 2018, 9, 2249.
DOI Google Scholar
[10]

Xue, S. S.; Li, P. F.; Sun, L.; An, L.; Qu, D.; Wang, X. Y.; Sun, Z. C. The formation process and mechanism of carbon dots prepared from aromatic compounds as precursors: A review. Small 2023, 19, 2206180.
DOI Google Scholar
[11]

Bartolomei, B.; Bogo, A.; Amato, F.; Ragazzon, G.; Prato, M. Nuclear magnetic resonance reveals molecular species in carbon nanodot samples disclosing flaws. Angew. Chem., Int. Ed. 2022, 61, e202200038.
DOI Google Scholar
[12]

Huang, C. S.; Feng, M. R.; Zhu, X. E.; Zhou, Q. Y.; Zeng, S. S.; Huang, Y. F.; Zhang, H. F. Polymer precursor strategy toward the precise synthesis of uniform hairy carbon dots with tunable sizes and size effects over their fluorescence. Macromolecules 2021, 54, 11497–11507.
DOI Google Scholar
[13]

Chen, Y. L.; Spiering, A. J. H.; Karthikeyan, S.; Peters, G. W. M.; Meijer, E. W.; Sijbesma, R. P. Mechanically induced chemiluminescence from polymers incorporating a 1,2-dioxetane unit in the main chain. Nat. Chem. 2012, 4, 559–562.
DOI Google Scholar
[14]

Yang, M. W.; Huang, J. G.; Fan, J. L.; Du, J. J.; Pu, K. Y.; Peng, X. J. Chemiluminescence for bioimaging and therapeutics: Recent advances and challenges. Chem. Soc. Rev. 2020, 49, 6800–6815.
DOI Google Scholar
[15]

Kagalwala, H. N.; Gerberich, J.; Smith, C. J.; Mason, R. P.; Lippert, A. R. Chemiluminescent 1,2-dioxetane iridium complexes for near-infrared oxygen sensing. Angew. Chem., Int. Ed. 2022, 61, e202115704.
DOI Google Scholar
[16]

Shen, C. L.; Jiang, T. C.; Lou, Q.; Zhao, W. B.; Lv, C. F.; Zheng, G. S.; Liu, H. R.; Li, P. F.; Dai, L. L.; Liu, K. K. et al. Near-infrared chemiluminescent carbon nanogels for oncology imaging and therapy. SmartMat 2022, 3, 269–285.
DOI Google Scholar
[17]

Yang, J.; Yin, W.; Van, R.; Yin, K. Y.; Wang, P.; Zheng, C.; Zhu, B. Y.; Ran, K.; Zhang, C.; Kumar, M. et al. Turn-on chemiluminescence probes and dual-amplification of signal for detection of amyloid beta species in vivo. Nat. Commun. 2020, 11, 4052.
DOI Google Scholar
[18]

Lyu, Y.; Pu, K. Y. Recent advances of activatable molecular probes based on semiconducting polymer nanoparticles in sensing and imaging. Adv. Sci. 2017, 4, 1600481.
DOI Google Scholar
[19]

Ouyang, Y.; Zhang, P.; Manis-Levy, H.; Paltiel, Y.; Willner, I. Transient dissipative optical properties of aggregated Au nanoparticles, CdSe/ZnS quantum dots, and supramolecular nucleic acid-stabilized Ag nanoclusters. J. Am. Chem. Soc. 2021, 143, 17622–17632.
DOI Google Scholar
[20]

Dong, S. Q.; Yuan, Z. Q.; Zhang, L. J.; Lin, Y. J.; Lu, C. Rapid screening of oxygen states in carbon quantum dots by chemiluminescence probe. Anal. Chem. 2017, 89, 12520–12526.
DOI Google Scholar
[21]

Zhen, X.; Zhang, C. W.; Xie, C.; Miao, Q. Q.; Lim, K. L.; Pu, K. Y. Intraparticle energy level alignment of semiconducting polymer nanoparticles to amplify chemiluminescence for ultrasensitive in vivo imaging of reactive oxygen species. ACS Nano 2016, 10, 6400–6409.
DOI Google Scholar
[22]

Augusto, F. A.; de Souza, G. A.; de Souza Júnior, S. P.; Khalid, M.; Baader, W. J. Efficiency of electron transfer initiated chemiluminescence. Photochem. Photobiol. 2013, 89, 1299–1317.
DOI Google Scholar
[23]

Shen, C. L.; Lou, Q.; Lv, C. F.; Zang, J. H.; Qu, S. N.; Dong, L.; Shan, C. X. Bright and multicolor chemiluminescent carbon nanodots for advanced information encryption. Adv. Sci. 2019, 6, 1802331.
DOI Google Scholar
[24]

Zheng, G. S.; Shen, C. L.; Lou, Q.; Han, J. F.; Ding, Z. Z.; Deng, Y.; Wu, M. Y.; Liu, K. K.; Zang, J. H.; Dong, L. et al. Meter-scale chemiluminescent carbon nanodot films for temperature imaging. Mater. Horiz. 2022, 9, 2533–2541.
DOI Google Scholar
[25]

Shen, C. L.; Zheng, G. S.; Wu, M. Y.; Wei, J. Y.; Lou, Q.; Ye, Y. L.; Liu, Z. Y.; Zang, J. H.; Dong, L.; Shan, C. X. Chemiluminescent carbon nanodots as sensors for hydrogen peroxide and glucose. Nanophotonics 2020, 9, 3597–3604.
DOI Google Scholar
[26]

Shen, C. L.; Lou, Q.; Lv, C. F.; Zheng, G. S.; Zang, J. H.; Jiang, T. C.; Cheng, Z.; Liu, K. K.; Niu, C. Y.; Dong, L. et al. Trigonal nitrogen activates high-brightness chemiluminescent carbon nanodots. ACS Mater. Lett. 2021, 3, 826–837.
DOI Google Scholar
[27]

Xia, C. L.; Zhu, S. J.; Feng, T. L.; Yang, M. X.; Yang, B. Evolution and synthesis of carbon dots: From carbon dots to carbonized polymer dots. Adv. Sci. 2019, 6, 1901316.
DOI Google Scholar
[28]

Rigodanza, F.; Burian, M.; Arcudi, F.; Đorđević, L.; Amenitsch, H.; Prato, M. Snapshots into carbon dots formation through a combined spectroscopic approach. Nat. Commun. 2021, 12, 2640.
DOI Google Scholar
[29]

Song, Y. B.; Zhu, S. J.; Zhang, S. T.; Fu, Y.; Wang, L.; Zhao, X. H.; Yang, B. Investigation from chemical structure to photoluminescent mechanism: A type of carbon dots from the pyrolysis of citric acid and an amine. J. Mater. Chem. C 2015, 3, 5976–5984.
DOI Google Scholar
[30]

Wang, B. Y.; Song, H. Q.; Tang, Z. Y.; Yang, B.; Lu, S. Y. Ethanol-derived white emissive carbon dots: The formation process investigation and multi-color/white LEDs preparation. Nano Res. 2022, 15, 942–949.
DOI Google Scholar
[31]

Tao, S. Y.; Zhou, C. J.; Kang, C. Y.; Zhu, S. J.; Feng, T. L.; Zhang, S. T.; Ding, Z. Y.; Zheng, C. Y.; Xia, C. L.; Yang, B. Confined-domain crosslink-enhanced emission effect in carbonized polymer dots. Light: Sci. Appl. 2022, 11, 56.
DOI Google Scholar
[32]

Vacher, M.; Galván, I. F.; Ding, B. W.; Schramm, S.; Berraud-Pache, R.; Naumov, P.; Ferré, N.; Liu, Y. J.; Navizet, I.; Roca-Sanjuán, D. et al. Chemi- and bioluminescence of cyclic peroxides. Chem. Rev. 2018, 118, 6927–6974.
DOI Google Scholar
[33]

Dou, X. N.; Lin, Z.; Chen, H.; Zheng, Y. Z.; Lu, C.; Lin, J. M. Production of superoxide anion radicals as evidence for carbon nanodots acting as electron donors by the chemiluminescence method. Chem. Commun. 2013, 49, 5871–5873.
DOI Google Scholar
[34]

Mao, D.; Wu, W. B.; Ji, S. L.; Chen, C.; Hu, F.; Kong, D. L.; Ding, D.; Liu, B. Chemiluminescence-guided cancer therapy using a chemiexcited photosensitizer. Chem 2017, 3, 991–1007.
DOI Google Scholar
[35]

Wang, Z. F.; Yuan, F. L.; Li, X. H.; Li, Y. C.; Zhong, H. Z.; Fan, L. Z.; Yang, S. H. 53% efficient red emissive carbon quantum dots for high color rendering and stable warm white-light-emitting diodes. Adv. Mater. 2017, 29, 1702910
DOI Google Scholar
[36]

Yang, H. Y.; Liu, Y. L.; Guo, Z. Y.; Lei, B. F.; Zhuang, J. L.; Zhang, X. J.; Liu, Z. M.; Hu, C. F. Hydrophobic carbon dots with blue dispersed emission and red aggregation-induced emission. Nat. Commun. 2019, 10, 1789.
DOI Google Scholar
[37]

Li, D.; Jing, P. T.; Sun, L. H.; An, Y.; Shan, X. Y.; Lu, X. H.; Zhou, D.; Han, D.; Shen, D. Z.; Zhai, Y. C. et al. Near-infrared excitation/emission and multiphoton-induced fluorescence of carbon dots. Adv. Mater. 2018, 30, 1705913.
DOI Google Scholar
[38]

Li, D.; Liang, C.; Ushakova, E. V.; Sun, M. H.; Huang, X. D.; Zhang, X. Y.; Jing, P. T.; Yoo, S. J.; Kim, J. et al. Thermally activated upconversion near-infrared photoluminescence from carbon dots synthesized via microwave assisted exfoliation. Small 2019, 15, 1905050.
DOI Google Scholar
[39]

Zhang, Q.; Wang, F. Q.; Wang, R. Y.; Liu, J. L.; Ma, Y. P. X.; Qin, X. R.; Zhong, X. X. Activating one/two-photon excited red fluorescence on carbon dots: Emerging n→ π photon transition induced by amino protonation. Adv. Sci. 2023, 10, 2207566.
DOI Google Scholar
[40]

Cao, M. Y.; Zhao, X. J.; Gong, X. Ionic liquid-assisted fast synthesis of carbon dots with strong fluorescence and their tunable multicolor emission. Small 2022, 18, 2106683.
DOI Google Scholar
[41]

Zeng, Q. S.; Feng, T. L.; Tao, S. Y.; Zhu, S. J.; Yang, B. Precursor-dependent structural diversity in luminescent carbonized polymer dots (CPDs): The nomenclature. Light: Sci. Appl. 2021, 10, 142.
DOI Google Scholar
[42]

Ma, Z. Z.; Shi, Z. F.; Qin, C. C.; Cui, M. H.; Yang, D. W.; Wang, X. J.; Wang, L. T.; Ji, X. Z.; Chen, X.; Sun, J. L. et al. Stable yellow light-emitting devices based on ternary copper halides with broadband emissive self-trapped excitons. ACS Nano 2020, 14, 4475–4486.
DOI Google Scholar
File
6456_ESM.pdf (2.2 MB)
Publication history
Copyright
Acknowledgements

Publication history

Received: 14 October 2023
Revised: 27 December 2023
Accepted: 28 December 2023
Published: 30 January 2024

Copyright

© Tsinghua University Press 2024

Acknowledgements

Acknowledgements

We gratefully acknowledge the support of the National Natural Science Foundation of China (Nos. U2004168, 12074348, 11974317, 12261141661, and 62204223), the China Postdoctoral Science Foundation (No. 2022TQ0307), and the Natural Science Foundation of Henan Province (Nos. 212300410078 and 222102310664)

Return