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Generating triplet states in carbon quantum dots confined in mesoporous MgO for phosphorescence and photocatalysis applications

介孔氧化镁中碳量子点三重态的产生及其磷光和光催化特性

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Abstract

In this study, room-temperature phosphorescence (RTP) was observed from carbon quantum dots (CQDs), which were embedded in porous magnesium oxide (MgO) via the high-temperature pyrolysis of citric acid (CA) and Mg2(OH)2CO3. The mesoporous MgO confined the CQDs via oxygen-containing groups and through changes in the angular momentum of surface atoms. Then, triplet states were created and the MgO-CQDs hybridization showed a typical excitation-dependent phenomenon, wherein fluorescence and RTP were red shifted when the excitation wavelength shifted to a longer wavelength, rendering an anticounterfeiting application. Moreover, the pyrolysis of CA in MgO resulted in a high specific surface area and extended the absorption wavelength range. Accompanied with the enhanced charge separation induced by delayed recombination of electrons and holes in the surface triplet state of CQDs, hybridization revealed an improved photocatalytic capability to degrade organic pollutants compared with pure MgO and its hybridization of CQDs without the Mg2(OH)2CO3 precursor.

摘要

本文通过高温热解柠檬酸(CA)和Mg2(OH)2CO3的混合物将碳量子点嵌入到介孔MgO中, 并观察到室温磷光. 碳量子点通过含氧官能团与MgO连接并被限制于MgO介孔中. 由于碳量子点表面原子自动受限, 其电子自旋角动量将改变, 产生自旋三重态并可获得磷光. 碳量子点与MgO的杂化复合物表现出典型的激发依赖现象, 当激发波长增加时, 荧光和室温磷光产生明显的红移, 因此具有良好的防伪应用价值. CA在MgO中热解, 使碳量子点与MgO的杂化复合物具有较高的比表面积和较宽的吸收波长. 碳量子点的三重态电子延迟复合提高了载流子分离效率. 因此与对照组样品对比, 该复合物对有机污染物的光催化降解能力有显著提高.

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References

  1. Wang R, Lu KQ, Tang ZR, et al. Recent progress in carbon quantum dots: Synthesis, properties and applications in photocatalysis. J Mater Chem A, 2017, 5: 3717–3734

    Article  CAS  Google Scholar 

  2. Choppadandi M, Guduru AT, Gondaliya P, et al. Structural features regulated photoluminescence intensity and cell internalization of carbon and graphene quantum dots for bioimaging. Mater Sci Eng-C, 2021, 129: 112366

    Article  CAS  Google Scholar 

  3. Cui L, Ren X, Wang J, et al. Synthesis of homogeneous carbon quantum dots by ultrafast dual-beam pulsed laser ablation for bioimaging. Mater Today Nano, 2020, 12: 100091

    Article  Google Scholar 

  4. Yao Q, Wu H, Jin Y, et al. One-pot synthesis of fluorescent nitrogen-doped graphene quantum dots for portable detection of iron ion. Curr Appl Phys, 2022, 41: 191–199

    Article  Google Scholar 

  5. Li WD, Zeng XY, Lv GY, et al. Fluorescent graphene oxide derived from carbonized citric acid for copper(II) ions detection. Rare Met, 2021, 40: 1443–1450

    Article  CAS  Google Scholar 

  6. Yao Q, Wu H, Jin Y, et al. Construction of NaYF4:Yb, Ho/B, N-GQDs nanocomposites for double anti-counterfeiting fluorescence ink. J Lumin, 2022, 251: 119186

    Article  CAS  Google Scholar 

  7. Zhang Y, Song H, Wang L, et al. Solid-state red laser with a single longitudinal mode from carbon dots. Angew Chem Int Ed, 2021, 60: 25514–25521

    Article  CAS  Google Scholar 

  8. Li J, Yun X, Hu Z, et al. Three-dimensional nitrogen and phosphorus co-doped carbon quantum dots/reduced graphene oxide composite aerogels with a hierarchical porous structure as superior electrode materials for supercapacitors. J Mater Chem A, 2019, 7: 26311–26325

    Article  CAS  Google Scholar 

  9. Wei G, Zhao X, Du K, et al. A general approach to 3D porous CQDs/MxOy (M = Co, Ni) for remarkable performance hybrid super-capacitors. Chem Eng J, 2017, 326: 58–67

    Article  CAS  Google Scholar 

  10. Nagaraj A, Munusamy MA, Al-Arfaj AA, et al. Functional ionic liquid-capped graphene quantum dots for chromium removal from chromium contaminated water. J Chem Eng Data, 2019, 64: 651–667

    Article  CAS  Google Scholar 

  11. Wang C, Bi L, Liu J, et al. Microalgae-derived carbon quantum dots mediated formation of metal sulfide nano-adsorbents with exceptional cadmium removal performance. J Colloid Interface Sci, 2023, 629: 994–1002

    Article  CAS  Google Scholar 

  12. Zhu S, Zhang J, Tang S, et al. Surface chemistry routes to modulate the photoluminescence of graphene quantum dots: From fluorescence mechanism to up-conversion bioimaging applications. Adv Funct Mater, 2012, 22: 4732–4740

    Article  CAS  Google Scholar 

  13. Lai S, Jin Y, Shi L, et al. Mechanisms behind excitation- and concentration-dependent multicolor photoluminescence in graphene quantum dots. Nanoscale, 2020, 12: 591–601

    Article  CAS  Google Scholar 

  14. Yang X, Ai L, Yu J, et al. Photoluminescence mechanisms of redemissive carbon dots derived from non-conjugated molecules. Sci Bull, 2022, 67: 1450–1457

    Article  CAS  Google Scholar 

  15. Wang B, Wei Z, Sui L, et al. Electron-phonon coupling-assisted universal red luminescence of o-phenylenediamine-based carbon dots. Light Sci Appl, 2022, 11: 172

    Article  CAS  Google Scholar 

  16. Wu Y, Fang X, Shi J, et al. Blue-to-green manipulation of carbon dots from fluorescence to ultralong room-temperature phosphorescence for high-level anti-counterfeiting. Chin Chem Lett, 2021, 32: 3907–3910

    Article  CAS  Google Scholar 

  17. Yang L, Zhang Q, Huang Y, et al. A sequential dual-lock strategy for generation of room-temperature phosphorescence of boron doped carbon dots for dynamic anti-counterfeiting. J Colloid Interface Sci, 2023, 632: 129–139

    Article  CAS  Google Scholar 

  18. Feng Q, Xie Z, Zheng M. Colour-tunable ultralong-lifetime room temperature phosphorescence with external heavy-atom effect in boron-doped carbon dots. Chem Eng J, 2021, 420: 127647

    Article  CAS  Google Scholar 

  19. Fang X, Tang Y, Ma YJ, et al. Ultralong-lived triplet excitons of room-temperature phosphorescent carbon dots located on g-C3N4 to boost photocatalysis. Sci China Mater, 2023, 66: 664–671

    Article  CAS  Google Scholar 

  20. Wang Q, Cai J, Biesold-McGee GV, et al. Silk fibroin-derived nitrogen-doped carbon quantum dots anchored on TiO2 nanotube arrays for heterogeneous photocatalytic degradation and water splitting. Nano Energy, 2020, 78: 105313

    Article  CAS  Google Scholar 

  21. Xie Z, Feng Y, Wang F, et al. Construction of carbon dots modified MoO3/g-C3N4 Z-scheme photocatalyst with enhanced visible-light photocatalytic activity for the degradation of tetracycline. Appl Catal B-Environ, 2018, 229: 96–104

    Article  CAS  Google Scholar 

  22. Qian X, Yue D, Tian Z, et al. Carbon quantum dots decorated Bi2WO6 nanocomposite with enhanced photocatalytic oxidation activity for VOCs. Appl Catal B-Environ, 2016, 193: 16–21

    Article  CAS  Google Scholar 

  23. Kuramochi Y, Fujisawa Y, Satake A. Photocatalytic CO2 reduction mediated by electron transfer via the excited triplet state of Zn(II) porphyrin. J Am Chem Soc, 2020, 142: 705–709

    Article  CAS  Google Scholar 

  24. Strieth-Kalthoff F, Glorius F. Triplet energy transfer photocatalysis: Unlocking the next level. Chem, 2020, 6: 1888–1903

    Article  CAS  Google Scholar 

  25. Zhao X, Hou Y, Liu L, et al. Triplet photosensitizers showing strong absorption of visible light and long-lived triplet excited states and application in photocatalysis: A mini review. Energy Fuels, 2021, 35: 18942–18956

    Article  CAS  Google Scholar 

  26. Bobrowski A, Nowak K, Zarebski J. Application of a bismuth film electrode to the voltammetric determination of trace iron using a Fe(III)-TEA-BrO3− catalytic system. Anal Bioanal Chem, 2005, 382: 1691–1697

    Article  CAS  Google Scholar 

  27. Wang T, Wang A, Wang R, et al. Carbon dots with molecular fluorescence and their application as a “turn-off” fluorescent probe for ferricyanide detection. Sci Rep, 2019, 9: 10723

    Article  Google Scholar 

  28. Tang G, Zhang K, Feng T, et al. One-step preparation of silica microspheres with super-stable ultralong room temperature phosphorescence. J Mater Chem C, 2019, 7: 8680–8687

    Article  CAS  Google Scholar 

  29. Wang C, Chen Y, Xu Y, et al. Aggregation-induced room-temperature phosphorescence obtained from water-dispersible carbon dot-based composite materials. ACS Appl Mater Interfaces, 2020, 12: 10791–10800

    Article  CAS  Google Scholar 

  30. Wang C, Chen Y, Hu T, et al. Color tunable room temperature phosphorescent carbon dot based nanocomposites obtainable from multiple carbon sources via a molten salt method. Nanoscale, 2019, 11: 11967–11974

    Article  CAS  Google Scholar 

  31. Abdulrazzaq OA, Bourdo SE, Saini V, et al. Acid-free polyaniline:graphene-oxide hole transport layer in organic solar cells. J Mater Sci-Mater Electron, 2020, 31: 21640–21650

    Article  CAS  Google Scholar 

  32. Sharma G, Deshpande UP, Kumar D, et al. Study of ultrathin magnetic cobalt films on MgO(001). J Appl Phys, 2012, 112: 023910

    Article  Google Scholar 

  33. Li M, Zhao Z, Ma L, et al. The influence of an MgO nanolayer on the planar Hall effect in NiFe films. J Appl Phys, 2015, 117: 123908

    Article  Google Scholar 

  34. Tadesse A, RamaDevi D, Hagos M, et al. Synthesis of nitrogen doped carbon quantum dots/magnetite nanocomposites for efficient removal of methyl blue dye pollutant from contaminated water. RSC Adv, 2018, 8: 8528–8536

    Article  CAS  Google Scholar 

  35. Wu H, Chai Y, Yang C, et al. In-situ grown nano silver iodide-graphene oxide-cotton hybrid filter material for dynamic visible light response photocatalysis. Separation Purification Tech, 2022, 295: 121192

    Article  CAS  Google Scholar 

  36. Wu H, Peng J, Sun H, et al. Surface activation of calcium tungstate by europium doping for improving photocatalytic performance: Towards lanthanide site photocatalysis. Chem Eng J, 2022, 432: 134339

    Article  CAS  Google Scholar 

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (51972065) and Guangdong Natural Science Foundation (2021A1515010179).

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Authors and Affiliations

  1. School of Physics and Optoelectronic Engineering, Guangdong University of Technology, Guangdong, 510006, China

    Qing Yao  (姚清), Haoyi Wu  (吴浩怡), Jinji Liang  (梁锦基), Chuanlong Wang  (王传龙), Yahong Jin  (金亚洪) & Yihua Hu  (胡义华)

  2. Institute for NanoScale Science and Technology, College of Science and Engineering, Flinders University, South Australia, 5042, Australia

    Youhong Tang  (唐友宏)

Authors
  1. Qing Yao  (姚清)
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  2. Haoyi Wu  (吴浩怡)
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  6. Yihua Hu  (胡义华)
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Contributions

Author contributions Wu H, Hu Y, and Yao Q conceptualized this work and designed the experiments. Yao Q performed the experiments related to the synthesis, characterization, fluorescence, and phosphorescence performance. Liang J carried out the photocatalytic tests. Wang C, Jin Y, and Tang Y helped with the data analyses and mechanism discussion. Wu H, Yao Q, and Tang Y co-wrote and revised the manuscript.

Corresponding authors

Correspondence to Haoyi Wu  (吴浩怡) or Yihua Hu  (胡义华).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Supplementary information Supporting data are available in the online version of the paper.

Qing Yao is a Master’s student at the College of Physics and Optoelectronic Engineering, Guangdong University of Technology. He graduated from the Southwest Petroleum University with a Bachelor’s degree in 2020. He is dedicated to the design and synthesis of carbon quantum dots and their fluorescence and phosphorescence emission.

Haoyi Wu received his PhD degree from Guangdong University of Technology in 2011. After finishing the postdoctoral and Japan Society for the Promotion of Science fellows at Tsinghua University and the National Institute of Advanced Industrial Science and Technology, he was employed at Guangdong University of Technology. His research interest is focused on luminescence materials and photocatalysts.

Yihua Hu received his PhD degree from Anhui Institute of Optics and Fine Mechanics, Chinese Academy of Sciences. He is a professor at Guangdong University of Technology. His research interest is focused on optical spectroscopy and various kinds of luminescence materials.

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40843_2023_2679_MOESM1_ESM.pdf

Generating triplet states in carbon quantum dots confined in mesoporous MgO for phosphorescence and photocatalysis applications

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Yao, Q., Wu, H., Liang, J. et al. Generating triplet states in carbon quantum dots confined in mesoporous MgO for phosphorescence and photocatalysis applications. Sci. China Mater. 67, 170–178 (2024). https://doi.org/10.1007/s40843-023-2679-x

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