碳点及其抗菌复合材料的研究进展

张文莉; 陈琳; 薛宝霞; 杨永珍; 张利; 刘旭光

doi:10.13801/j.cnki.fhclxb.20230306.001

碳点及其抗菌复合材料的研究进展

doi: 10.13801/j.cnki.fhclxb.20230306.001

张文莉¹,
陈琳^1, ,,
薛宝霞²,
杨永珍^1, ,,
张利³,
刘旭光⁴

1.
太原理工大学　新材料界面科学与工程教育部重点实验室，太原 030024
2.
太原理工大学　轻纺工程学院，晋中 030600
3.
山西白求恩医院　泌尿外科，太原 030032
4.
太原理工大学　材料科学与工程学院，太原 030024

基金项目: 山西浙大新材料与化工研究院项目(2021SX-FR010；2021SX-TD013)；山西省纳米药物可控缓释技术创新中心(202104010911026)；山西省自然科学基金(202203021211159；20210302124200；202103021224355)

详细信息

通讯作者:
陈琳，博士，副教授，硕士生导师，研究方向为纳米碳功能材料　E-mail: chenlin01@tyut.edu.cn

杨永珍，博士，教授，博士生导师，研究方向为纳米碳功能材料　E-mail：yyztyut@126.com

中图分类号: TB34；TB332
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出版历程
- 收稿日期: 2022-11-14
- 修回日期: 2023-02-15
- 录用日期: 2023-02-25
- 网络出版日期: 2023-03-06
- 刊出日期: 2023-07-15

Recent advances in carbon dots and their antibacterial composite materials

1.
Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of Education, Taiyuan University of Technology, Taiyuan 030024, China
2.
College of Tectile Engineering, Taiyuan University of Technology, Jinzhong 030600, China
3.
Urinary Surgery, Bethune Hospital of Shanxi Province, Taiyuan 030032, China
4.
College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China

Funds: Shanxi-Zheda Institute of New Materials and Chemical Engineering (2021SX-FR010; 2021SX-TD013); Shanxi Technology Innovation Center for Controlled and Sustained Release of Nano-drugs (202104010911026); Natural Science Foundation of Shanxi Province (202203021211159; 20210302124200; 202103021224355)

摘要

摘要: 抗菌剂是抑制细菌感染不可或缺的药物，传统抗菌剂抗生素的过度使用导致细菌的耐药性逐渐增强，严重威胁人类健康。碳点作为一种新型的纳米抗菌材料，具有抗菌能力强、原料来源广、细胞毒性低且生物相容性好等优点，将其与传统抗菌剂组合构建的新型纳米复合材料在抗菌领域表现出良好的应用前景。本文综述了碳点及其复合材料的抗菌机制与应用研究进展。首先，通过总结碳点的抗菌机制，系统分析了影响碳点抗菌性能的主要因素。其次，介绍碳点与传统抗菌剂相结合的新型纳米复合材料及其在抗菌领域的应用。最后，对碳点及其复合材料在抗菌应用研究中存在的问题进行总结并展望，为具有高效和长期抗菌性能的碳点复合材料的设计与合成提供借鉴经验。
- 碳点 /
- 抗菌材料 /
- 复合材料 /
- 抗菌机制 /
- 抗菌应用
Abstract: Antimicrobials are indispensable drugs to inhibit bacterial infection. The overuse of conventional antibacterial (antibiotics) leads to the gradual enhancement of antimicrobial resistance of bacteria, which poses a serious threat to human health. As a new type of nano antibacterial material, carbon dots have the advantages of high anti antibacterial ability, wide range of raw materials, low cytotoxicity and good biocompatibility. Novel nano composite materials constructed by combining carbon dots with traditional antibacterial agents show great application prospects in the antibacterial field. This paper reviews the research progress on antibacterial mechanisms and applications of carbon dots and their composites. Firstly, the main factors affecting on the antibacterial performance of carbon dots are systematically analyzed by summarizing their antibacterial mechanisms. Secondly, the new nano composite materials combining carbon dots with traditional antibacterial agents and their applications in the antibacterial field are introduced. Finally, problems in the antibacterial application research of carbon dots and their composites are summarized and prospects are put forward, so as to provide reference experience for the design and synthesis of carbon dot composites with efficient and long-time antibacterial properties.
- carbon dots /
- antibacterial materials /
- composite materials /
- antibacterial mechanisms /
- antibacterial application

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图 1 (a) 碳点(CDs)的核壳结构；(b) 细菌的基本结构

Figure 1. (a) Nuclear-shell structure of carbon dots (CDs); (b) Basic structure of bacteria

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图 2 CDs抗菌机制示意图

Figure 2. Schematic diagram of antibacterial mechanisms of CDs

ROS—Reaction oxygen species

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图 3 光诱导CDs产生活性氧(ROS)的原理图

Figure 3. Schematic diagram of the reaction oxygen species (ROS) generation by light-induced CDs

hv—Light; VB—Valence band; CB—Conduction band; S₀—Ground singlet state; S₁—Excited singlet state; T₁—Excited triplet state

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图 4 (a) 通过不同分子量截留(MWCO)再生纤维素透析袋分离不同尺寸的CDs；(b) 小粒径葡萄糖酸氯己定CDs (CGCDs)(s-CGCDs)、中粒径CGCDs(m-CGCDs)和大粒径CGCDs (l-CGCDs)进入细菌细胞时的扩散能力示意图^[48]

Figure 4. (a) Separating CDs of different sizes through different molecular weight cutoff (MWCO) regenerated cellulose dialysis bags; (b) Schematic diagram of the diffusion ability of small particle size chlorhexidine gluconate CDs (CGCDs) (s-CGCDs), middle particle size CGCDs (m-CGCDs), and large particle size CGCDs (l-CGCDs) into bacterial cells^[48]

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图 5 Ag掺杂CDs (a) 和CDs/银纳米颗粒(Ag NPs)复合材料 (b) 的合成示意图^[66]

Figure 5. Schematic diagram of the synthesis of Ag-doped CDs (a) and CDs/silver nanoparticles (Ag NPs) composites (b)^[66]

PEI—Polyethylenimine

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图 6 (a) 薄膜透明度随两亲性牛奶衍生CDs (ACMCD)负载的银纳米颗粒(ACMCD-Ag)的掺杂水平而变化；(b) ACMCD-Ag/聚甲基丙烯酸甲酯(ACMCD-Ag/PMMA)薄膜的照片(掺杂量2wt%)^[92]

Figure 6. (a) Transparency of thin films as a function of amphipathy cow milk-derived CDs (ACMCD) supported silver nanoparticles (ACMCD-Ag) doping level; (b) Photograph of the ACMCD-Ag/polymethylmethacrylate (ACMCD-Ag/PMMA) thin film product (Doping amount 2wt%)^[92]

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图 7 纤维素纳米纤维(CNF)基包衣的橘子(a)和草莓(b)在储存时的外观变化^[111]

Figure 7. Appearance change of tangerines (a) and strawberries (b) coated with the cellulose nanofiber (CNF)-based films during storage^[111]

GCD—Glucose CDs; NGCD—N-functionalized CDs

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图 8 (a) ε-聚(L-赖氨酸) CDs@氧化葡聚糖(PL-CD@ODA)水凝胶的SEM图像；(b) PL-CD@ODA水凝胶被压碎和愈合的照片；(c) PL-CD@ODA水凝胶的可注射性^[115]

Figure 8. (a) SEM images of ε-poly(L-lysine) CD@oxidized dextran (PL-CD@ODA) hydrogels; (b) Photographs of PL-CD@ODA hydrogel being crushed and healing; (c) Injectability of PL-CD@ODA hydrogel^[115]

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表 1 表面功能化CDs的功能化试剂、制备方法、结构和抗菌性能

Table 1. Functional reagents, synthetic methods, structure, and antibacterial properties of surface-functionalized CDs

Functional reagents		Synthetic methods	Surface-functionalized CDs	Size/nm	Zeta potential/mV	Bacteria	MIC/ (μg·mL⁻¹)	Ref.
Ammonium	GTA	Ultrasound	Q-CQDs	4	+10	E. coli	32	[52]
						P. aeruginosa	64
						S. aureus	8
						MRSA	8
	DDA	Solvothermal	qCQDs	3	—	S. aureus	25	[54]
						MRSA	25
						E. coli	50
						P. aeruginosa	50
	TAA	Microwave	CDs-C9	6.5	+7.5	E. coli	7.9	[55]
	TAA	Microwave	CDs-C9	6.5	+7.5	S. aureus	3.1	[55]
Amine	Cadaverine	Microwave	CCQDs	3	0-2	E. coli	9.7	[57]
	Cadaverine	Microwave	CCQDs	3	—	S. aureus	4.8
	Histamine	Microwave	HCQDs	4.6	0-2	E. coli	6.9
	Histamine	Microwave	HCQDs	4.6	—	S. aureus	6.9
	Putrescine	Microwave	PCQDs	4	0-2	S. aureus	3.4
	Spermine	Microwave	SCQDs	8	0-2	S. aureus	6.5
	TTDDA	Microwave	NH₂-FCDs	—	+10.5	E. coli	>5000	[58]
	EDA	Solvothermal	EDA-CDs	4-5	—	B. subtilis	64	[59]
	EDA	Solvothermal	EDA-CDs	4-5	—	E. coli	64	[59]
	AG	Hydrothermal	AG/CA-CDs	4.3	—	P. aeruginosa	500	[60]
Quaternary ammonium compound	BS-12	Solvothermal	CDs-C₁₂	4	−11.6	S. aureus	8	[61]
						B. subtilis	12
						E. coli	>200
						P. aeruginosa	>200
Antibiotic	AMP	Hydrothermal	CDs-AMP	44	−8	E. coli	14	[62]
Notes: GTA—Glycidyl trimethyl ammonium chloride; DDA—Dimethyl diallyl ammonium chloride; TAA—Diazonium salts bearing tetraalkylammonium moieties; TTDDA—4,7,10-trioxa-1,13-tridecanediamine; EDA—2,2'-(ethylenedioxy) bis (ethylamine); AG—Amino guanidine; MIC—Minimal inhibitory concentration; BS-12—Lauryl betaine; AMP—Ampicillin; CA—Citric acid; MRSA—Methicillin-resistant staphylococcus aureus; Q-CQDs, qCQDs—Quaternized carbon quantum dots; CDs-C9—CDs with different alkyl chains (C9); CCQDs, HCQDs, PCQDs, SCQDs—Cadaverine-, histamine-, putrescine-, spermine-CQDs; NH₂-FCDs—Amine-coated CDs.

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表 2 杂原子掺杂CDs的原料、结构和抗菌性能

Table 2. Feedstock, structure, and antibacterial properties of heteroatom-doped CDs

Classification		Dopant	Carbon source	Heteroatom- doped CDs	Size/nm	Zeta potential/ mV	Bacteria	Antibacterial properties	Ref.
Metal doping	Ag	AgNO₃	CA, PEI	Ag- doped CDs	1.8	+25.0	E. coli	MIC: 50 μg·mL⁻¹	[66]
			CA, PEI	Ag- doped CDs	1.8	+25.0	S. aureus	MIC: 15 μg·mL⁻¹	[66]
			Cannabis sativa	Ag@CDs	—	—	E. coli	MIC: 42 μg·mL⁻¹	[67]
			Cannabis sativa	Ag@CDs	—	—	S. aureus	MIC: 42 μg·mL⁻¹	[67]
			Dopamine, cysteine	NSCDAg	—	−44.0	E. coli	MIC: 8 μg·mL⁻¹	[68]
			Dopamine, cysteine	NSCDAgAc	—	−29.0	E. coli	MIC: 8 μg·mL⁻¹	[68]
	Ce	Ce(NO₃)₃	CA	Ce-CNDs	2-4	—	S. aureus	MIC: 200 μg·mL⁻¹	[79]
	Cu	Cu(CH₃COO)₂·H₂O	Tea	Cu-CDs	0.9	—	S. aureus	MIC: 156 μg·mL⁻¹	[80]
	Zn	(CH₃COO)₂Zn	CA, EDA	Zn-CDs	1.8	—	S. aureus	SR: 89% (Blue light: 40 min)	[81]
Non-metal doping	N	DETA	Glucose	NCQDs	5	+23.0	S. aureus	DIZ: 15.5 mm	[72]
		DETA	Glucose	NCQDs	5	+23.0	MRSA	DIZ: 14.5 mm	[72]
		Polyvinylpyrrolidone		N-CQDs	6.5	−6.5	E. coli	MIC: 32 μg·mL⁻¹	[74]
		PVAm	CA	CA∶ PVAm C-dots	12.6	+29.0	E. coli	MIC: 1.56 mg·mL⁻¹	[75]
							S. aureus	MIC: 1.56 mg·mL⁻¹
							B. subtilis	MIC: 0.75 mg·mL⁻¹
		Melamine, EDTA		g-CNQDs	2	−36.0	E. coli	SR: 99% (100 μg·mL⁻¹)	[76]
		Melamine, EDTA		g-CNQDs	2	−36.0	S. aureus	SR: 90% (100 μg·mL⁻¹)	[76]
		Urea	Glucose	NGCD	5.6	−3.8	E. coli	MIC: 19 μg·mL⁻¹	[77]
	B	H₃BO₃	Glucose	BGCD	6.2	−18.0	E. coli	MIC: 156 μg·mL⁻¹	[77]
	S	Poly (sodium-4-styrene sulfonate)		S-CQDs	6.5	−47.2	E. coli	MIC: 32 μg·mL⁻¹	[74]
		(NH₄)₂S₂O₈	Glucose	S-CDs	6.9	−5.5	E. coli	MIC: 156 μg·mL⁻¹	[77]
		Na₂S₂O₈	Turmeric	SGCD	8.5	+4.5	E. coli	DIZ: 14 mm	[83]
	P	H₃PO₄	m-Aminophenol	P- doped CQDs	3.4	+23.1	E. coli	MIC: 1.23 mg·mL⁻¹	[84]
	P	H₃PO₄	m-Aminophenol	P- doped CQDs	3.4	+23.1	S. aureus	MIC: 1.44 mg·mL⁻¹	[84]
Co-doping	N, S	Urea, thiourea	CA	N, S- doped CNDs	—	—	E. coli	SR: 68% (500 μg·mL⁻¹)	[11]
	Ag, N	AgNO₃, NH₃∙H₂O	CA	Ag, N-CQDs	5~9	—	E. coli	MIC: 250 μg·mL⁻¹	[85]
	Ag, N	AgNO₃, NH₃∙H₂O	CA	Ag, N-CQDs	5~9	—	S. aureus	MIC: 200 μg·mL⁻¹	[85]
	Ag, S	MPA, AgNO₃	CA	Ag@S-GQDs	28	—	S. aureus	MIC: 35 μg·mL⁻¹	[86]
Notes：DETA—Diethylenetriamine; PVAm—Polyethyleneamine; EDTA—Ethylene diamine tetraacetic acid; MPA—3-mercaptopropionic acid; SR—Sterilization rate; DIZ—Diameters of inhibition zone; NSCDs—Heteroatom (N and S) doped CDs; CNDs—Carbon nanodots; CQDs—Carbon quantum dots; GCD—Glucose CDs; GQD—Graphene quantum dots.

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表 3 CDs复合材料的抗菌性能

Table 3. Antibacterial properties of CDs composites

Classification		Antimicrobial	Composite	MIC/(μg·mL⁻¹); SR/%; DIZ/mm		Ref.
Classification		Antimicrobial	Composite	E. coli	S. aureus	Ref.
CDs/antibiotic		RUT	CDs-RUT	180 μg·mL⁻¹ (Dark)	170 μg·mL⁻¹ (Dark)	[105]
CDs/antibiotic		RUT	CDs-RUT	150 μg·mL⁻¹ (Light)	100 μg·mL⁻¹ (Light)	[105]
CDs/native compound		CS	N-doped C-dot (CS)	90.00% (100 μL)	92.00% (100 μL)	[109]
		CS	N, S doped C-dot (CS)	41.53% (100 μL)	48.54% (100 μL)	[109]
		Cur	CQDs/Cur	—	>99.9%	[110]
CDs/inorganic compound	CDs/Ag NPs	Ag NPs	CDs/Ag NPs	20 μg·mL⁻¹	5 μg·mL⁻¹	[66]
			Ag NPs/CDs	40 μg·mL⁻¹	20 μg·mL⁻¹	[90]
			ACMCD-Ag	10 μg·mL⁻¹	5 μg·mL⁻¹	[92]
			CDs/Ag NPs	12-13 mm	13-15 mm	[93]
			CQDs/Ag NPs	10.88 mm	11.22 mm	[94]
			Ag NPs-ACNPs	63.64%	93.49%	[95]
			Ag-GQDs	—	25 μg·mL⁻¹	[96]
	CDs/metallic oxide	ZnO	ZnO@CQDs	6 mg·mL⁻¹	8 mg·mL⁻¹	[102]
	CDs/peroxide	H₂O₂	H₂O₂/CDs	88% (0.59 mM H₂O₂/8 μg·mL⁻¹ CDs)	—	[59]
	CDs/Fe	Fe	Fe-CDs	99.85%	99.68%	[106]
CDs/organic compound	CDs/dye	MB	CDs/MB	100%(1 μg·mL⁻¹ MB/5 μg·mL⁻¹ CDs)	—	[107]
		TB	CDs/TB	100%(1 μg·mL⁻¹ TB/ 5 μg·mL⁻¹ CDs)	—	[107]
		BODIPY	BODIPY@n-CDs	—	256 μg·mL⁻¹	[108]
		BODIPY	BODIPY@p-CDs	—	128 μg·mL⁻¹	[108]
	CDs/polymer	PVA	N-doped C-dot (PVA)	47.53% (100 μL)	36.49% (100 μL)	[109]
		PVA	N, S doped C-dot (PVA)	56.47% (100 μL)	46.51% (100 μL)
		PS	N-doped C-dot (PS)	70.50% (100 μL)	39.86% (100 μL)
		PS	N, S doped C-dot (PS)	61.65% (100 μL)	39.41% (100 μL)
Notes：RUT—Rutin; CS—Chitosan; Cur—Curcumin; MB—Methylene blue; TB—Toluidine blue; BODIPY—Fluoroborondipyrrole; PVA—Polyvinyl alcohol; PS—Polysulfonatestyrene; ACMCD—Amphiphilic cow milk-derived CDs; ACNPs—Activated carbon nanoparticle.

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