Preparation of Solvent-Dependent Carbon Dots for Water Content Detection and Anti-Counterfeiting

doi:10.19894/j.issn.1000-0518.230372

Chinese Journal of Applied Chemistry ›› 2024, Vol. 41 ›› Issue (7): 937-947.DOI: 10.19894/j.issn.1000-0518.230372

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Preparation of Solvent-Dependent Carbon Dots for Water Content Detection and Anti-Counterfeiting

Sai CUI¹, Ya-Ting MENG¹^,², Song-Bai WANG¹, Chuan DONG¹, Shao-Min SHUANG¹()

^1.School of Chemistry and Chemical Engineering，and Institute of Environmental Science，Shanxi University，Taiyuan 030006，China
^2.School of Public Health，Shanxi Key Laboratory of Environmental Health Impairment and Prevention，MOE Key Laboratory of Coal Environmental Pathogenicity and Prevention，Shanxi Medical University，Taiyuan 030001，China

Received:2023-11-28 Accepted:2024-05-06 Published:2024-07-01 Online:2024-08-03
Contact: Shao-Min SHUANG
About author:smshuang@sxu.edu.cn
Supported by:
the National Natural Science Foundation of China(22274090);the Research Project Supported by Shanxi Scholarship Cournil of China(2021-011)

Abstract

Abstract:

Nitrogen doped fluorescent carbon dots （N-CDs） with high quantum yield （QY=87.76%） were synthesized by solvothermal method using diphenylamino-4-benzaldehyde and o-phenylenediamine as raw materials and ethanol as solvent. The optical properties of N-CDs in organic solvents and aqueous solutions were investigated， indicating that N-CDs have good solvent dependence and chemical stability. The addition of water constructed a hydrogen bonding grid in N-CDs， thereby achieving a redshift in emission wavelength， and the N-CDs solution changes from blue to yellow. Furthermore， based on the reversible color change from blue to yellow of N-CDs fluorescent test strips， a portable air humidity visualization detection test strip was prepared. In addition， N-CDs can also be used for fluorescent ink， writing paper， and fluorescent flexible films， which expanding their applications in information transmission， advanced anti-counterfeiting encryption， and solid-state fluorescence.

Key words: Carbon dots, Solvent-dependent behavior, Paper-based sensing, Anti-counterfeiting

CLC Number:

O655

Sai CUI, Ya-Ting MENG, Song-Bai WANG, Chuan DONG, Shao-Min SHUANG. Preparation of Solvent-Dependent Carbon Dots for Water Content Detection and Anti-Counterfeiting[J]. Chinese Journal of Applied Chemistry, 2024, 41(7): 937-947.

Figures/Tables 14

Fig.1 （A） TEM image，（B） TEM size distribution，（C） AFM image and （D） AFM size distribution image of N-CDs

Fig.2 （A） XPS spectra of N-CDs； The high-resolution XPS spectra of （B） C1s，（C） N1s （D） O1s and （E） FT-IR spectrum of N-CDs

Fig.3 （A） The UV-visible absorption and excitation-emission spectra；（B） Fluorescence spectra at different excitation wavelengths；（C） 3D fluorescence spectra；（D） Fluorescence lifetime decay curve of N-CDs

Table 1 Relevant data of integrated fluorescence intensity and absorbance of Quinine sulfate and N-CDs at 360 nm excitation wavelength

	Quinine sulfate					N-CDs
Abs	0.018	0.024	0.025	0.031	0.043	0.013	0.023	0.029	0.044	0.050
Integrated FL intensity/a.u.	112.223	145.650	178.785	219.476	347.290	252.846	308.065	453.895	664.643	758.695
Grad	9 548.2				14 346
QY/%	56.1				87.76

Fig.4 Effect of （A） different xenon lamp irradiation times；（B） Storage time at room temperature on the fluorescence intensity of N-CDs

Fig.5 （A） The UV-visible absorpton spectra，（B） optimal fluorescence emission peak，（C） lmages in sunlight and ultraviolet light （The solvents from left to right are THF， acetone，DMF， DMSO， ethanol， methanol，water），（D） the emission peak position varies with relative polarity parameter （ETN） of N-CDs in different solvents

Fig.6 （A） The normalized fluorescence spectra；（B）Color coordinate graph of different water volume fraction；（C） The ultraviolet light images of N-CDs with water volume fraction （The volume fractions of water from left to right are 2%， 10%， 20%， 30%， 40%， 50%， 60%， 70%，80%， 90% and 98%， respectively）

Table 2 Chromaticity color coordinates （x， y） of CDs with different water volume fractions in EtOH

S. N	Water volume fractions in EtOH/%	（x， y）
1	2	（0.15， 0.12）
2	10	（0.18， 0.20）
3	20	（0.18， 0.22）
4	30	（0.20， 0.27）
5	40	（0.23， 0.37）
6	50	（0.23， 0.38）
7	60	（0.23， 0.38）
8	70	（0.26， 0.39）
9	80	（0.29， 0.41）
10	90	（0.33， 0.44）
11	98	（0.40， 0.50）

Fig.7 （A） Fluorescence spectra and （B） 3D fluorescence spectra of N-CDs in aqueous solution at different excitation wavelengths

Table 3 Determination of water volume fraction in Shanxi Fen Wine

Sample 1 （42° Shanxi Fen Wine）	Measured （φ/%）	Amount spiked （φ/%）	Amount measured （φ/%）	Recovery/%	RSD/% （n=6）
Fluorescence intensity method	60.41	10	73.64	104.60	0.38
		20	78.96	98.20	0.09
		30	90.70	100.32	0.06
Emission peak method	54.65	10	61.88	103.20	2.34
		20	81.62	109.34	2.32
		30	88.43	104.47	1.87

Table 4 Determination of water content in medicinal alcohol

Sample 2 （75% medicinal alcohol）	Measured （φ/%）	Amount spiked （φ/%）	Amount measured （φ/%）	Recovery/%	RSD/% （n=6）
Fluorescence intensity method	30.32	10	41.83	103.75	0.26
		20	49.74	98.85	0.29
		30	59.47	96.94	0.35
Emission peak method	26.41	10	37.18	102.11	1.34
		20	43.72	94.20	2.46
		30	63.61	112.76	2.85

Fig. 8 （A） Picture of the evaporation and drying process of N-CDs test strips soaked in ethanol under ultraviolet light （λ=365 nm）；（B） Pictures in the presence of ethanol， drying， and water；（C） Pictures of cyclic recovery capability （λ=365 nm）

Fig.9 Pictures of different water volume fraction of test paper under UV lamp

Fig.10 Anti-counterfeiting application of N-CDs：（A） N-CDs as fluorescent ink；（B） N-CDs as writing paper；（C） N-CDs test paper is designed as paper-cuttings；（D） N-CDs/PVA film

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Preparation of Solvent-Dependent Carbon Dots for Water Content Detection and Anti-Counterfeiting

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