新型磁电催化纳米粒子的活性氮释放与抗菌性能研究

doi:10.15541/jim20240152

无机材料学报 ›› 2024, Vol. 39 ›› Issue (10): 1114-1124.DOI: 10.15541/jim20240152 CSTR: 32189.14.10.15541/jim20240152

新型磁电催化纳米粒子的活性氮释放与抗菌性能研究

张志民¹^,²(), 葛敏¹, 林翰¹^,²(), 施剑林¹^,²()

1.中国科学院上海硅酸盐研究所, 高性能陶瓷和超微结构国家重点实验室, 上海 200050
2.中国科学院大学材料科学与光电技术学院, 北京 100049

收稿日期:2024-03-27 修回日期:2024-04-15 出版日期:2024-10-20 网络出版日期:2024-10-09
通讯作者: 林翰, 副研究员. E-mail: linhan@mail.sic.ac.cn;
施剑林, 研究员. E-mail: jlshi@mail.sic.ac.cn
作者简介:张志民(1999-), 男, 硕士研究生. E-mail: zhangzhimin21@mails.ucas.ac.cn
基金资助:
国家自然科学基金(52372276)

Novel Magnetoelectric Catalytic Nanoparticles: RNS Release and Antibacterial Efficiency

ZHANG Zhimin¹^,²(), GE Min¹, LIN Han¹^,²(), SHI Jianlin¹^,²()

1. State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
2. Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing 100049, China

Received:2024-03-27 Revised:2024-04-15 Published:2024-10-20 Online:2024-10-09
Contact: LIN Han, associate professor. E-mail: linhan@mail.sic.ac.cn;
SHI Jianlin, professor. E-mail: jlshi@mail.sic.ac.cn
About author:ZHANG Zhimin (1999-), male, Master candidate. E-mail: zhangzhimin21@mails.ucas.ac.cn
Supported by:
National Natural Science Foundation of China(52372276)

摘要/Abstract

摘要：

相比于功能单一且易催生细菌耐药性的抗生素等药物, 具有催化活性的无机纳米功能材料凭借自身对感染微环境(弱酸、高H₂O₂含量)或外部物理刺激(激光、超声)的高响应性和广谱杀菌等优势, 在致病菌感染的治疗中占据愈发重要的地位。然而, 感染微环境酸性微弱且不稳定, 光、声信号功率密度过高会对人体细胞造成伤害, 而诸如交变磁场等非侵入性、高组织穿透性和易于远程控制的信号类型及其介导的磁电催化在抗菌中的应用尚未见报道。本研究将基于磁致伸缩-压电催化效应的交变磁场响应性纳米催化策略应用于抗菌, 并使用含氮基团L-精氨酸(LA)修饰CoFe₂O₄-BiFeO₃磁电纳米颗粒(BCFO)表面, 以实现磁电响应可控释放强杀菌物种活性氮(RNS)。在交变磁场中, BCFO同时产生羟基自由基(·OH)和超氧阴离子(·O₂^-)两种活性氧(ROS), 前者与LA反应产生一氧化氮(NO), 后者与NO反应生成RNS物种过氧亚硝酸根(ONOO^-)。作为高活性的硝化和氧化剂, ONOO^-可在生物友好的交变磁场下展现出比ROS更强的抗菌能力。本研究证实BCFO能产生ONOO^-, 并发挥更强的杀菌功效。这一研究不仅将磁电纳米催化医学策略用于抗菌, 还通过ROS向RNS转变显著提升了材料的抗菌性能。

关键词: 纳米催化医学, 磁电响应, 活性氮, 抗菌

Abstract:

Compared with antibiotics and other drugs with poor functionalities and risk to induce bacterial resistance, inorganic functional nanomaterials with catalytic activity occupy an increasingly important position in the treatment of pathogenic infections by advantages of high response to the infected microenvironment (e.g. weak acid, high H₂O₂ concentration) or external physical stimuli (e.g. laser, ultrasound) and broad-spectrum sterilization. However, the acidic infection microenvironment is weak and unstable, and light or sound signals with high power density will cause damage to human cells. In addition, antimicrobial applications of alternative magnetic field (AMF), a non-invasive signal type with high tissue penetration, convenience to be remotely controlled, and effective magnetoelectric catalysis based on AMF have not been reported. In this study, an AMF-responsive nanocatalytic strategy based on the magnetostrictive-piezoelectric catalytic effect was applied to antibacterial research, and the surface of CoFe₂O₄-BiFeO₃ magnetoelectric nanoparticles (BCFO) was modified with the nitrogen-containing group L-arginine (LA) to achieve a magneto-electric responsive controlled release of powerful bactericide reactive nitrogen species (RNS). In AMF, BCFO simultaneously generates reactive oxygen species (ROS) hydroxyl radical (·OH) and superoxide anion (·O₂^-). The former reacts with LA to release nitric oxide (NO), and the latter combines with NO to produce peroxynitrite (ONOO^-), a typical RNS. As a highly active nitrification and oxidation agent, ONOO^- could exhibit stronger antibacterial activity than ROS under biofriendly AMF. Successful production of ONOO^- and achievement of stronger bactericidal efficiency were validated in this study. This work not only applies magnetoelectric nanocatalysis for antibacterial purposes, but also significantly improves the antibacterial ability through the conversion of ROS to RNS.

Key words: nanocatalytic medicine, magnetoelectric response, reactive nitrogen species, antibacterial

中图分类号:

TB34
R613

张志民, 葛敏, 林翰, 施剑林. 新型磁电催化纳米粒子的活性氮释放与抗菌性能研究[J]. 无机材料学报, 2024, 39(10): 1114-1124.

ZHANG Zhimin, GE Min, LIN Han, SHI Jianlin. Novel Magnetoelectric Catalytic Nanoparticles: RNS Release and Antibacterial Efficiency[J]. Journal of Inorganic Materials, 2024, 39(10): 1114-1124.

图/表 10

图1 BCFO-LA产生ONOO-及抗菌机理示意图

Fig. 1 Schematic diagram of the ONOO- generating and antibacterial mechanisms of BCFO-LA BCFO: CoFe2O4-BiFeO3 magnetoelectric nanoparticles; LA: L-arginine

图2 BCFO的形貌、成分与结构表征

Fig. 2 Morphology, component and construction characterizations of BCFO (a-c) TEM (a), HRTEM (b) and bright field (c) images of BCFO; (d) Element mappings of BCFO; (e) Molar percentages of metal elements in BCFO according to ICP-OES; (f) XRD pattern of BCFO; (g-i) Total (g),Fe2p (h) and O1s (i) XPS spectra of BCFO; Colorful figures are available on website

图3 BCFO的性能检测

Fig. 3 Performance evaluation of BCFO (a) Hysteresis loops of CFO and BCFO in AMF (1 emu/g = 104 G/g, 1 Oe = 79.577472 A/m); (b) Piezoresponsive amplitude and phase curves of BCFO; (c) EPR patterns of DMPO solutions with different treatments; (d) UV-Vis absorption spectra of DPBF treated by BCFO under AMF at different time points

图4 BCFO在交变磁场中的理论模拟

Fig. 4 Theoretical simulation of BCFO in AMF (a-e) COMSOL simulations of magnetization (a), von Mises stress (b), volumetric strain (c), displacement (d), and electric potential (e) produced by BCFO in AMF; (f-h) Relationships between AMF and volumetric strain (f), AMF and displacement (g) as well as volumetric strain and electric potential (h) in BCFO derived from COMSOL

图5 BCFO-LA的制备表征与ONOO-产生性能

Fig. 5 Preparation, characterization and ONOO--generation property of BCFO-LA (a) Preparing processes of PLGA-TK-LA (EDCl: 1-Ethyl-3-(3-dimethylaminopropyl)carbodiimide hydrochloride; NHS: N-Hydroxysuccinimide; DMF: N,N-Dimethylformamide; DCC: N,N'-Dicylohexylcarbodiimide; DMAP: 4-Dimethylaminopyridine); (b) 1H NMR spectrum of PLGA-TK-LA; (c) Schematic diagram of BCFO-LA preparation (BCFO: CoFe2O4-BiFeO3, cobalt ferrite-bismuth ferrite); (d) TEM image of BCFO-LA with negative staining, where the shaded area circled by dotted line refers to PLGA-TK-LA; (e) Hydraulic diameter distributions of BCFO-LA; (f) Fluorescence emission spectra of L-tyrosine probe after co-incubated with BCFO-LA at different time points under AMF (B = 1.7 mT, λex = 265 nm)

图6 BCFO-LA的抗菌性能

Fig. 6 Antibacterial performance of BCFO-LA (a, b) Plate-spreading photos (a) and survival rates (b) of S. aureus treated by BCFO; (c, d) Plate-spreading photos (c) and survival rates (d) of S. aureus treated by BCFO-LA; (e, f) Flow cytometry results of DCFH-DA stained S. aureus (e) and relative DCF fluorescence intensities (f)

图S1 CFO的形貌和物相表征

Fig. S1 Morphology and phase characterizations of CFO (a, b) TEM image (a) and XRD pattern (b) of CFO; (c, d) TEM image (c) and XRD pattern (d) of CFO coated with BFO precursor

图S2 BCFO的形貌表征

Fig. S2 Morphology characterization of BCFO (a) SEM image of BCFO; (b) Dark field image of BCFO derived from HRTEM

图S3 CFO和BCFO的粒径分布

Fig. S3 Size distributions of CFO and BCFO (a, b) Size distributions of CFO (a) and BCFO (b) according to TEM images

图S4 交变磁场对细菌存活率的影响

Fig. S4 Influence of AMF on bacterial survival rates Plate-spreading photos (a) and survival rates (b) of S. aureus treated by AMF

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新型磁电催化纳米粒子的活性氮释放与抗菌性能研究

Novel Magnetoelectric Catalytic Nanoparticles: RNS Release and Antibacterial Efficiency

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