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Solvent-controlled synthesis strategy of multicolor emission carbon dots and its applications in sensing and light-emitting devices

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Abstract

Carbon dots (CDs), as a new kind of carbon-based luminescent nanomaterials, have drawn widespread attention in the fields of fluorescence sensing, optoelectronic devices, and biological imaging. This work uses citric acid (CA) and Nile Blue A (NBA) as precursors. By simply changing the solvent in the reaction, their bandgaps were systematically controlled, thereby successfully obtaining bright blue, yellow and red fluorescence emission CDs (B-, Y- and RCDs). The higher quantum yield (QY) of B-, Y- and RCDs are 64%, 57% and 51%, respectively. The selected precursors and different solvents are the key to the formation of three emission CDs. Detailed characterization and density functional theory (DFT) calculations further indicate that the difference in emission color of CDs is due to the size of the sp2 conjugate domain. In addition, we used multicolor CDs as fluorescent probes to investigate their performance in detection. Among them, BCDs and YCDs can detect Sudan Red I with high selectivity and sensitivity. In the concentration range of 0 to 80 µM, the detection limits are 56 and 41 nM, respectively. Multicolor emitting phosphors and fluorescent films are also obtained by mixing CDs with other matrices. Using Ultraviolet (UV) chip as the excitation source and combining with multicolor fluorescent film and a certain proportion of B-, Y-, and RCDs/epoxy resin composites, bright monochromatic light-emitting diodes (LEDs) and white LED (WLED) with high color rendering index (CRI) were prepared. The above results indicate that the multicolor CDs prepared by us have great application potential in the fields of food safety control and optical devices.

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References

  1. Li, S. H.; Su, W.; Wu, H.; Yuan, T.; Yuan, C.; Liu, J.; Deng, G.; Gao, X. C.; Chen, Z. M.; Bao, Y. M. et al. Targeted tumour theranostics in mice via carbon quantum dots structurally mimicking large amino acids. Nat. Biomed. Eng. 2020, 4, 704–716.

    Article  CAS  Google Scholar 

  2. Zhu, Z. J.; Zhai, Y. L.; Li, Z. H.; Zhu, P. Y.; Mao, S.; Zhu, C. Z.; Du, D.; Belfiore, L. A.; Tang, J. G.; Lin, Y. H. Red carbon dots: Optical property regulations and applications. Mater. Today 2019, 30, 52–79.

    Article  CAS  Google Scholar 

  3. Huo, F.; Karmaker, P. G.; Liu, Y. H.; Zhao, B.; Yang, X. P. Preparation and biomedical applications of multicolor carbon dots: Recent advances and future challenges. Part. Part. Syst. Char. 2020, 37, 1900489.

    Article  Google Scholar 

  4. Liu, J. J.; Li, R.; Yang, B. Carbon dots: A new type of carbon-based nanomaterial with wide applications. ACS Cent. Sci. 2020, 6, 2179–2195.

    Article  CAS  Google Scholar 

  5. Shamsipur, M.; Barati, A.; Karami, S. Long-wavelength, multicolor, and white-light emitting carbon-based dots: Achievements made, challenges remaining, and applications. Carbon 2017, 124, 429–472.

    Article  CAS  Google Scholar 

  6. Rosso, C.; Filippini, G.; Prato, M. Carbon dots as nano-organocatalysts for synthetic applications. ACS Catal. 2020, 10, 8090–8105.

    Article  CAS  Google Scholar 

  7. Rani, U. A.; Ng, L. Y.; Ng, C. Y.; Mahmoudi, E. A review of carbon quantum dots and their applications in wastewater treatment. Adv. Colloid Interface Sci. 2020, 278, 102124.

    Article  Google Scholar 

  8. Chung, Y. J.; Kim, J.; Park, C. B. Photonic carbon dots as an emerging nanoagent for biomedical and healthcare applications. ACS Nano 2020, 14, 6470–6497.

    Article  CAS  Google Scholar 

  9. Li, W. D.; Liu, Y.; Wang, B. Y.; Song, H. Q.; Liu, Z. Y.; Lu, S. Y.; Yang, B. Kilogram-scale synthesis of carbon quantum dots for hydrogen evolution, sensing and bioimaging. Chin. Chem. Lett. 2019, 30, 2323–2327.

    Article  CAS  Google Scholar 

  10. He, P.; Shi, Y. X.; Meng, T.; Yuan, T.; Li, Y. C.; Li, X. H.; Zhang, Y.; Fan, L. Z.; Yang, S. H. Recent advances in white light-emitting diodes of carbon quantum dots. Nanoscale 2020, 12, 4826–4832.

    Article  CAS  Google Scholar 

  11. Huang, Y. Y.; Lin, H.; Qiu, J.; Luo, Z. T.; Yao, Z. Q.; Liu, L. B.; Liu, H. B.; Tang, X. S.; Fu, X. X. High color rendering indices of white light-emitting diodes based on environmentally friendly carbon and AIZS nanoparticles. J. Mater. Chem. C 2020, 8, 7734–7740.

    Article  CAS  Google Scholar 

  12. Walther, B. K.; Dinu, C. Z.; Guldi, D. M.; Sergeyev, V. G.; Creager, S. E.; Cooke, J. P.; Guiseppi-Elie, A. Nanobiosensing with graphene and carbon quantum dots: Recent advances. Mater. Today 2020, 39, 23–46.

    Article  CAS  Google Scholar 

  13. Song, H. Q.; Liu, X. J.; Wang, B. Y.; Tang, Z. Y.; Lu, S. Y. High production-yield solid-state carbon dots with tunable photoluminescence for white/multi-color light-emitting diodes. Sci. Bull. 2019, 64, 1788–1794.

    Article  CAS  Google Scholar 

  14. Yuan, F. L.; He, P.; Xi, Z. F.; Li, X. H.; Li, Y. C.; Zhong, H. Z.; Fan, L. Z.; Yang, S. H. Highly efficient and stable white LEDs based on pure red narrow bandwidth emission triangular carbon quantum dots for wide-color gamut backlight displays. Nano Res. 2019, 12, 1669–1674.

    Article  CAS  Google Scholar 

  15. Zheng, K.; Li, X.; Chen, M. J.; Gong, Y.; Tang, A. W.; Wang, Z. G.; Wei, Z. R.; Guan, L.; Teng, F. Controllable synthesis highly efficient red, yellow and blue carbon nanodots for photo-luminescent light-emitting devices. Chem. Eng. J. 2020, 380, 122503.

    Article  CAS  Google Scholar 

  16. Wang, B. Y.; Li, J.; Tang, Z. Y.; Yang, B.; Lu, S. Y. Near-infrared emissive carbon dots with 33.96% emission in aqueous solution for cellular sensing and light-emitting diodes. Sci. Bull. 2019, 64, 1285–1292.

    Article  CAS  Google Scholar 

  17. Jiao, Y.; Liu, Y.; Meng, Y. T.; Gao, Y. F.; Lu, W. J.; Liu, Y.; Gong, X. J.; Shuang, S. M.; Dong, C. Novel processing for color-tunable luminescence carbon dots and their advantages in biological systems. ACS Sustainable Chem. Eng. 2020, 8, 8585–8592.

    Article  CAS  Google Scholar 

  18. Ding, Y. F.; Zheng, J. X.; Wang, J. L.; Yang, Y. Z.; Liu, X. G. Direct blending of multicolor carbon quantum dots into fluorescent films for white light emitting diodes with an adjustable correlated color temperature. J. Mater. Chem. C 2019, 7, 1502–1509.

    Article  CAS  Google Scholar 

  19. Shen, C. L.; Lou, Q.; Liu, K. K.; Dong, L.; Shan, C. X. Chemiluminescent carbon dots: Synthesis, properties, and applications. Nano Today 2020, 35, 100954.

    Article  CAS  Google Scholar 

  20. Kumari, R.; Pal, K.; Karmakar, P.; Sahu, S. K. pH-responsive Mndoped carbon dots for white-light-emitting diodes, fingerprinting, and bioimaging. ACS Appl. Nano Mater. 2019, 2, 5900–5909.

    Article  CAS  Google Scholar 

  21. Madhu, M.; Chen, T. H.; Tseng, W. L. White-light emission of single carbon dots prepared by hydrothermal carbonization of poly(diallyldimethylammonium chloride): Applications to fabrication of white-light-emitting films. J. Colloid Interface Sci. 2019, 556, 120–127.

    Article  CAS  Google Scholar 

  22. Xu, A. L.; Wang, G.; Li, Y. Q.; Dong, H.; Yang, S. W.; He, P.; Ding, G. Q. Carbon-based quantum dots with solid-state photoluminescent: Mechanism, implementation, and application. Small 2020, 16, 2004621.

    Article  CAS  Google Scholar 

  23. Miao, S. H.; Liang, K.; Zhu, J. J.; Yang, B.; Zhao, D. Y.; Kong, B. Hetero-atom-doped carbon dots: Doping strategies, properties and applications. Nano Today 2020, 33, 100879.

    Article  CAS  Google Scholar 

  24. Zhi, B.; Yao, X. X.; Cui, Y.; Orr, G.; Haynes, C. L. Synthesis, applications and potential photoluminescence mechanism of spectrally tunable carbon dots. Nanoscale 2019, 11, 20411–20428.

    Article  CAS  Google Scholar 

  25. Nguyen, H. A.; Srivastava, I.; Pan, D.; Gruebele, M. Unraveling the fluorescence mechanism of carbon dots with sub-single-particle resolution. ACS Nano 2020, 14, 6127–6137.

    Article  CAS  Google Scholar 

  26. Karami, S.; Shamsipur, M.; Taherpour, A. A.; Jamshidi, M.; Barati, A. In situ chromophore doping: A new mechanism for the long-wavelength emission of carbon dots. J. Phys. Chem. C 2020, 124, 10638–10646.

    Article  CAS  Google Scholar 

  27. Li, L. B.; Dong, T. Photoluminescence tuning in carbon dots: Surface passivation or/and functionalization, heteroatom doping. J. Mater. Chem. C 2018, 6, 7944–7970.

    Article  CAS  Google Scholar 

  28. Lu, S. Y.; Sui, L. Z.; Liu, J. J.; Zhu, S. J.; Chen, A. M.; Jin, M. X.; Yang, B. Near-infrared photoluminescent polymer-carbon nanodots with two-photon fluorescence. Adv. Mater. 2017, 29, 1603443.

    Article  Google Scholar 

  29. He, T.; Wang, G. N.; Liu, J. X.; Zhao, W. L.; Huang, J. J.; Xu, M. X.; Wang, J. P.; Liu, J. Dummy molecularly imprinted polymer based microplate chemiluminescence sensor for one-step detection of Sudan dyes in egg. Food Chem. 2019, 288, 347–353.

    Article  CAS  Google Scholar 

  30. Zhao, D.; Zhang, Z. X.; Liu, X. M.; Zhang, R.; Xiao, X. C. Rapid and low-temperature synthesis of N, P co-doped yellow emitting carbon dots and their applications as antibacterial agent and detection probe to Sudan Red I. Mater. Sci. Eng. C 2021, 119, 111468.

    Article  CAS  Google Scholar 

  31. Wu, M.; Sun, L. J.; Miao, K. S.; Wu, Y. Z.; Fan, L. J. Detection of Sudan dyes based on inner-filter effect with reusable conjugated polymer fibrous membranes. ACS Appl. Mater. Interfaces 2018, 10, 8287–8295.

    Article  CAS  Google Scholar 

  32. Wang, L.; Yang, R.; Li, J. J.; Qu, L. B.; Harrington, P. D. B. Highsensitive electrochemical sensor of Sudan I based on template-directed self-assembly of graphene-ZnSe quantum dots hybrid structure. Sens. Actuators B Chem. 2015, 215, 181–187.

    Article  CAS  Google Scholar 

  33. Su, A. M.; Zhong, Q. M.; Chen, Y. Y.; Wang, Y. L. Preparation of carbon quantum dots from cigarette filters and its application for fluorescence detection of Sudan I. Anal. Chim. Acta 2018, 1023, 115–120.

    Article  CAS  Google Scholar 

  34. Long, C. C.; Jiang, Z. X.; Shangguan, J. F.; Qing, T. P.; Zhang, P.; Feng, B. Applications of carbon dots in environmental pollution control: A review. Chem. Eng. J. 2021, 406, 126848.

    Article  CAS  Google Scholar 

  35. Jia, R. N.; Jin, K. F.; Zhang, J. M.; Zheng, X. J.; Wang, S.; Zhang, J. Colorimetric and fluorescent detection of glutathione over cysteine and homocysteine with red-emitting N-doped carbon dots. Sens. Actuators B Chem. 2020, 321, 128506.

    Article  CAS  Google Scholar 

  36. Cui, F. C.; Sun, J. D.; de Dieu Habimana, J.; Yang, X. X.; Ji, J.; Zhang, Y. Z.; Lei, H. T.; Li, Z. J.; Zheng, J. Y.; Fan, M. H. et al. Ultrasensitive fluorometric angling determination of staphylococcus aureus in vitro and fluorescence imaging in vivo using carbon dots with full-color emission. Anal. Chem. 2019, 91, 14681–14690.

    Article  CAS  Google Scholar 

  37. Jiao, Y.; Meng, Y. T.; Lu, W. J.; Gao, Y. F.; Liu, Y.; Gong, X. J.; Liu, Y.; Shuang, S. M.; Dong, C. Design of long-wavelength emission carbon dots for hypochlorous detection and cellular imaging. Talanta 2020, 219, 121170.

    Article  CAS  Google Scholar 

  38. Ding, H.; Zhou, X. X.; Wei, J. S.; Li, X. B.; Qin, B. T.; Chen, X. B.; Xiong, H. M. Carbon dots with red/near-infrared emissions and their intrinsic merits for biomedical applications. Carbon 2020, 167, 322–344

    Article  CAS  Google Scholar 

  39. Wang, H.; Haydel, P.; Sui, N.; Wang, L. N.; Liang, Y.; Yu, W. W. Wide emission shifts and high quantum yields of solvatochromic carbon dots with rich pyrrolic nitrogen. Nano Res. 2020, 13, 2492–2499.

    Article  CAS  Google Scholar 

  40. Li, X. X.; Wang, Z. F.; Liu, Y.; Zhang, W. G.; Zhu, C. F.; Meng, X. G. Bright tricolor ultrabroad-band emission carbon dots for white light-emitting diodes with a 96.5 high color rendering index. J. Mater. Chem. C 2020, 8, 1286–1291.

    Article  CAS  Google Scholar 

  41. Zhou, Z. J.; Ushakova, E. V.; Liu, E. S.; Bao, X.; Li, D.; Zhou, D.; Tan, Z. N.; Qu, S. N.; Rogach, A. L. A co-crystallization induced surface modification strategy with cyanuric acid modulates the bandgap emission of carbon dots. Nanoscale 2020, 12, 10987–10993.

    Article  CAS  Google Scholar 

  42. Shah, H.; Xie, W. J.; Wang, Y. Y.; Jia, X. R.; Nawaz, A.; Xin, Q.; Song, M. Y.; Gong, J. R. Preparation of blue- and green-emissive nitrogen-doped graphene quantum dots from graphite and their application in bioimaging. Mater. Sci. Eng. C 2021, 119, 111642.

    Article  Google Scholar 

  43. Ma, P. P.; Sun, X. B.; Pan, W.; Yu, G. F.; Wang, J. P. Green and orange emissive carbon dots with high quantum yields dispersed in matrices for phosphor-based white LEDs. ACS Sustainable Chem. Eng. 2020, 8, 3151–3161.

    Article  CAS  Google Scholar 

  44. Cai, W.; Zhang, T.; Xu, M.; Zhang, M. R.; Guo, Y. J.; Zhang, L. P.; Street, J.; Ong, W. J.; Xu, Q. Full color carbon dots through surface engineering for constructing white light-emitting diodes. J. Mater. Chem. C 2019, 7, 2212–2218.

    Article  CAS  Google Scholar 

  45. Zhang, M.; Xue, J.; Zhu, Y.; Yao, C.; Yang, D. Y. Multiresponsive white-light emitting aerogel prepared with codoped lanthanide/thymidine/carbon dots. ACS Appl. Mater. Interfaces 2020, 12, 22191–22199.

    Article  CAS  Google Scholar 

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

    Article  Google Scholar 

  47. Wang, B. Y.; Yu, J. K.; Sui, L. Z.; Zhu, S. J.; Tang, Z. Y.; Yang, B.; Lu, S. Y. Rational design of multi-color-emissive carbon dots in a single reaction system by hydrothermal. Adv. Sci. 2021, 8, 2001453.

    Article  CAS  Google Scholar 

  48. Arcudi, F.; Đorđević, L.; Prato, M. Rationally designed carbon nanodots towards pure white-light emission. Angew. Chem., Int. Ed. 2017, 56, 4170–4173.

    Article  CAS  Google Scholar 

  49. Zu, F. L.; Yan, F. Y.; Bai, Z. J.; Xu, J. X.; Wang, Y. Y.; Huang, Y. C.; Zhou, X. G. The quenching of the fluorescence of carbon dots: A review on mechanisms and applications. Microchim. Acta 2017, 184, 1899–1914.

    Article  CAS  Google Scholar 

  50. Yan, F. Y.; Jiang, Y. X.; Sun, X. D.; Wei, J. F.; Chen, L.; Zhang, Y. Y. Multicolor carbon dots with concentration-tunable fluorescence and solvent-affected aggregation states for white light-emitting diodes. Nano Res. 2020, 13, 52–60.

    Article  CAS  Google Scholar 

  51. Zhang, X. Q.; Yang, H. Y.; Wan, Z. J.; Su, T.; Zhang, X. J.; Zhuang, J. L.; Lei, B. F.; Liu, Y. L.; Hu, C. F. Self-quenching-resistant red emissive carbon dots with high stability for warm white light-emitting diodes with a high color rendering index. Adv. Opt. Mater. 2020, 8, 2000251.

    Article  CAS  Google Scholar 

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Acknowledgements

The work was supported by the National Natural Science Foundation of China (Nos. 51678409, 51638011, and 51578375), Tianjin Research Program of Application Foundation and Advanced Technology (Nos. 19JCYBJC19800, 18JCYBJC87500, and 15ZCZDSF00880), State Key Laboratory of Separation Membranes and Membrane Processes (Z1-201507), and the Program for Innovative Research Team in University of Tianjin (TD13-5042).

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

    Zhonghui Sun, Fanyong Yan, Jing Xu, Hao Zhang & Li Chen

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  1. Zhonghui Sun
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  3. Jing Xu
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Correspondence to Fanyong Yan.

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Solvent-controlled synthesis strategy of multicolor emission carbon dots and its applications in sensing and light-emitting devices

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Sun, Z., Yan, F., Xu, J. et al. Solvent-controlled synthesis strategy of multicolor emission carbon dots and its applications in sensing and light-emitting devices. Nano Res. 15, 414–422 (2022). https://doi.org/10.1007/s12274-021-3495-8

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