Citation: Chunyan Wang, Chen Wei, Hongyang Niu, Ligang Xu, Xue Liu. Graded nitro-engineering strategy: Tuning surface states and sp² conjugated domains of carbon quantum dots for full-color emission[J]. Chinese Chemical Letters, ;2025, 36(10): 111296. doi: 10.1016/j.cclet.2025.111296 shu

Graded nitro-engineering strategy: Tuning surface states and sp² conjugated domains of carbon quantum dots for full-color emission

Chunyan Wang ^{a, 1} ,
Chen Wei ^{a, 1} ,
Hongyang Niu ^a ,
Ligang Xu ^b ,
Xue Liu ^{a, c, *,}

a.
Institute of Clean Energy Chemistry, Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials, College of Chemistry, Liaoning University, Shenyang 110036, China
b.
Key Laboratory for Organic Electronics and Information Displays (KLOEID) & Jiangsu Key Laboratory for Biosensors, Institute of Advanced Materials (IAM), Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), Nanjing University of Posts & Telecommunications, Nanjing 210023, China
c.
School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 637371, Singapore

liuxue@lnu.edu.cn

Received Date: 10 December 2024
Revised Date: 2 May 2025
Accepted Date: 9 May 2025
Available Online: 9 May 2025

Figures(5)

Precise control of luminescence in carbon quantum dots (CQDs), from single-color to full-color emission, is crucial for advancing their applications in biomedical imaging and display technologies. While CQDs luminescence is primarily influenced by conjugated domains and surface states, the underlying interaction mechanisms remain poorly understood. This study explores a graded nitro-engineering approach to simultaneously regulate surface states and sp² conjugated domains through nitro (-NO₂) modulation, enabling comprehensive color tuning. Using o-phenylenediamine (o-PD) as the carbon source and adjusting nitric acid (HNO₃) concentrations, we synthesized tricolor-emitting nitro-functionalized CQDs (NO₂-CQDs). At lower -NO₂ concentrations, luminescence is mainly influenced by surface states, where the electron-withdrawing effect of -NO₂ enhances π-electron delocalization and stabilizes sp² conjugation. With increasing -NO₂ content, the lowest unoccupied molecular orbital (LUMO) energy level decreases (-2.12 eV to -3.39 eV), resulting in a red-shift in fluorescence. At higher -NO₂ concentrations, luminescence is primarily affected by the sp² conjugated domain, where steric hindrance reduces molecular planarity and conjugation, leading to a blue-shift in fluorescence as the sp² domain size decreases (4.03 nm to 2.83 nm). Combining experimental results with density functional theory (DFT) calculations, we reveal the dual role of -NO₂ in modulating CQDs luminescence, an approach rarely achieved through surface functionalization. This work presents a novel strategy for precise tuning of CQDs luminescence across the visible spectrum.
- Carbon quantum dots,
- Nitro groups,
- Full-color fluorescence,
- Surface engineering,
- Conjugated structure
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

Graded nitro-engineering strategy: Tuning surface states and sp2 conjugated domains of carbon quantum dots for full-color emission

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通讯作者: 陈斌, bchen63@163.com

Graded nitro-engineering strategy: Tuning surface states and sp² conjugated domains of carbon quantum dots for full-color emission