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化学进展 2022, Vol. 34 Issue (11): 2540-2560 DOI: 10.7536/PC220332 前一篇   

• 综述 •

无抗生素纳米抗菌剂:现状、挑战与展望

漆晨阳, 涂晶*()   

  1. 武汉理工大学材料复合新技术国家重点实验室 武汉 430070
  • 收稿日期:2022-03-28 修回日期:2022-07-09 出版日期:2022-11-24 发布日期:2022-09-19
  • 通讯作者: 涂晶
  • 基金资助:
    国家自然科学基金项目(22005231); 中央高校基本科研专项资金(武汉理工大学)(2021IVA093); 中央高校基本科研专项资金(武汉理工大学)(2021IVB033)
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Antibiotic-Free Nanomaterial-Based Antibacterial Agents:Current Status, Challenges and Perspectives

Chenyang Qi, Jing Tu()   

  1. State key Laboratory of Advanced Technology for Material Synthesis and Processing, Wuhan University of Technology,Wuhan 430070, China
  • Received:2022-03-28 Revised:2022-07-09 Online:2022-11-24 Published:2022-09-19
  • Contact: Jing Tu
  • Supported by:
    National Natural Science Foundation of China(22005231); Fundamental Research Funds for the Central Universities (Wuhan University of Technology)(2021IVA093); Fundamental Research Funds for the Central Universities (Wuhan University of Technology)(2021IVB033)

耐药性细菌和生物膜相关的感染性疾病严重威胁全球公众健康。随着纳米技术在抗菌领域的渗透和发展,研发基于无抗生素的新型纳米抗菌剂在避免耐药性产生以及抗菌治疗方式的选择方面提供更多可能性。本文从细菌耐药性的产生机制出发,阐述利用纳米材料自身独特的理化性质,实现自体抗菌;作为纳米酶,利用类酶活性催化底物产生活性氧簇(ROS)等抗菌;随后讨论了构建随内源性/外源性环境刺激响应,以及协同多种新型治疗方式的智能纳米抗菌剂,实现高效抗菌。最后,提出了目前面临的挑战及临床应用前景,为开发更加安全、高效的纳米抗菌剂提供借鉴。

关键词： 细菌耐药性, 细菌生物膜, 纳米材料, 活性氧簇, 协同抗菌

Drug-resistance bacterial and biofilm-related infectious diseases pose a significant threat to the global public health. Focusing on the drug-resistance mechanisms of bacteria to antibiotics, we aim at presenting the research progress of nanomaterial-based antibacterial agents. This review starts with clarifying nanomaterials with unique physicochemical characteristics, which act as intrinsic antibacterial agents. Subsequently, we discuss nanomaterial-based artificial enzymes, which can kill bacteria with reactive oxygen species (ROS). Furthermore, nanomaterial-based multiple synergetic modality nanoplatforms are constructed to combat infections. These multifunctional antibacterial agents, either microenvironment-oriented or external stimulants responsive, coordinate new treatments for precise medication and integration of diagnoses and treatments. In addition, the challenges and clinical prospects of these nanomaterial-based antibacterial agents are discussed, providing new perspectives of developing safer and more efficient antibacterial agents.

Contents

1 Introduction

2 Drug-resistance mechanisms

3 Antibiotic-free nanomaterial-based antibacterial agents

3.1 Intrinsic antibacterial agents

3.2 Nanozyme

3.3 Intelligent responsive nanomaterial-based antibacterial agents

4 Conclusion and future perspectives

Key words: bacterial drug-resistance, bacterial biofilm, nanomaterials, reactive oxygen species, synergistic antibacterial
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图1 根据ISI web of science上搜索主题“nanomaterials”和“antibacterial agent”获得的统计数据(2011—2021)
Fig. 1 The statistics of the paper indexed in the ISI web of science by the topic of “nanomaterials” and “antibacterial agent”
图2 细菌耐药性的产生机制[2,6,40? ~42].(a)浮游细菌的耐药途径和(b)细菌生物膜的形成
Fig. 2 General DR mechanisms[2,6,40? ~42].(a) The DR pathways for planktonic bacteria and (b) Formation of biofilms
图3 纳米抗菌剂的多种抗菌机制[2,6,7,54,55]
Fig. 3 Antibacterial mechanisms of nanomaterials[2,6,7,54,55]
图4 两亲性QC和QCS衍生物均相合成胶束和QCS胶束抗菌、愈合伤口示意图[72]
Fig. 4 Schematic illustration of homogeneous synthesis of micelles with amphiphilic QC and QCS derivatives and QCS micelles for antibacterial and wound healing[72]. Copyright 2022, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
图5 (a) M-Art M制备过程; Fe-Art M中Fe2N6O作为催化中心通过(b)类POD和(c)类HPO催化产生·O2-和HClO; (d) MRSA与Fe-Art M共孵育后的SEM图像; (e)不同Art Ms捕获的MRSA数量; (g)不同Art Ms作用后的活/死细菌比率; (f) V-Art M和(h) Fe-Art M作用于MRSA活/死染色的共聚焦激光扫描显微镜(CLSM)图像的3D重建[81]
Fig. 5 (a) The preparation process of M-Art M; Fe2N6O as a catalytic center in Fe-Art M for the production of·O2-and HClO through (b) POD-like and (c) HPO-like catalytic pathways; (d) SEM images after MRSA co-incubation with Fe-Art M; (e) number of MRSAs captured by different Art Ms; (g) different Art Ms act on live/dead bacteria ratios; 3D reconstructions from confocal laser scanning microscopy (CLSM) images of (f) V-Art M and (h) Fe-Art M when treated with MRSA[81]. Copyright 2021, Springer Nature
图6 (a) L-Arg/GOx@CuBDC的制备和(b)增强协同杀灭细菌的自激活双级联反应机制[83]
Fig. 6 (a) Synthetic process for L-Arg/GOx@CuBDC and (b) the self-activated double-cascade reaction mechanism for enhanced synergistic bacteria killing[83]. Copyright 2020, American Chemical Society
表1 微环境响应型纳米抗菌剂的总结
Table 1 Summary of microenvironment-responsive nanomaterial-based antibacterial agents
Nanomaterials Triggers Responsive units Bactericidal moieties Bacteria/Biofilm ref
rAgNAs pH PEG-PSB-PALA Ag+ MRSA 90
AgNPs-LA-OB pH LA-OB Ag+ E.coli/S. aureus/S. aureus biofilm 91
AgNCs pH POEC-SH Ag+ E.coli/MRSA 92
IKFQFHFD-based nanofiber networks pH IKFQFHFD Cypate(PTT) E. coli/ B. subtilis/S. aureus/
P. aeruginosa/MRSA/MRSA biofilm		 89
MBP-Ce6 NSs pH MnO2 Ce6(PDT) MRSA biofilm 93
CGNs pH P(GEMADA-co-DMA)-b-PBMA CS(PTT),guanidyl S. aureus biofilm 94
PCB-Au NRs pH PCB Au NRs(PTT) E.coli/ S. aureus/MRSA 95
Ag+-GCS-PDA@GNRs pH GCS Ag+、GNRs(PTT) MRSA/E.coli 96
MCS@PDA@GCS pH GCS Cu2+、PDA(PTT) MRSA/E.coli 97
FePAgPG pH GCS Ag+、Fe3O4/PDA(PTT) S. mutants/S. mutants biofilm 98
Pd(H)@ZIF-8 pH ZIF-8 Zn2+、H2 H. pylori 99
ICGZnS NPs pH ZnS NPs Zn2+、H2S、ICG(PDT) MRSA biofilm 100
DCPNAs pH Cu2O NPs Dextran、·OH S. aureus/Salmonella typhimurium 101
CuFe5O8 NCs pH/H2O2 Cu/Fe ·OH E.coli/S. aureus biofilm 102
Cu2O NPs H2S/H2O2 Cu2O NPs ·OH、Cu9S8 NPs(PTT) MRSA 103
AA@Ru@HA-MoS2 Hydase HA ·OH、Ru NPs(PTT) MDR S. aureus/P. aeruginosa 104
CHFH Hydase HA ·OH、CuS NPs(PTT) S. aureus 105
UCMB-LYZ-HP Hydase HA ε-PL、MB(PDT) MRSA 106
Ru-Se@GNP-RBCM Gelatinase GNPs Ru-Se NPs MRSA/E. coli 107
Ag-MONs GSH Ag-MONs Ag+ E.coli/S. aureus 28
图7 (a) pH响应性纳米抗菌剂(rAgNAs)的构建以及机制; (b)不同pH值PBS中rAgNAs的透过率; (c) rAgNAs的表面电荷随pH值的变化; (d) pH=7.4和5.5(n = 3)时的累积Ag+释放量[90]
Fig. 7 (a) The construction and mechanism of pH-responsive nanomaterial-based antibacterial agents (rAgNAs); (b) transmittance of rAgNAs in PBS with different pH values; (c) surface charge of rAgNAs along with changes in the pH value; (d) cumulative silver ion release amount at pH=7.4 and 5.5 (n = 3)[90]. Copyright 2019, American Chemical Society
图8 (a) CuFe5O8 NCs的制备以及(b)抗生物膜和免疫调节机制[102]
Fig. 8 (a) The synthesis process of CuFe5O8NCs and (b) anti-biofilm and immunomodulatory mechanisms[102]. Copyright 2020, American Chemical Society
图9 (a)红光触发的胶束纳米粒子释放NO[129]; (b)可见光介导的PCNO胶束中NO和CO的共释放[130]
Fig. 9 (a) Red light-triggered NO release from micellar nanoparticles[129] Copyright 2021, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim; (b) visible light-mediated co-release of NO and CO from PCNO micelles[130]. Copyright 2022, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
表2 光衍生的多模式协同抗菌治疗
Table 2 Photo-derived multimodal synergistic antibacterial therapy
Synergistic antibacterial therapy Light(wavelength/power/time) Bacteria/Biofilm(Antibacterial concentration) ref
MoS2-BNN6 NO/PTT 808 nm, 1 W/cm2, 10min Ampr E. coli/E. faecalis/S. aureus(MoS2:200 μg/mL, BNN6:80 μg/mL) 133
SNP-PB NO/PTT 808 nm, 1 W/cm2, 5min S. aureus/E. coli(>2 mg/mL) 134
SNP@MOF@Au-Mal NO/PTT 808 nm, 1.5 W/cm2, 7min P. aeruginosa(80 μg/mL) 135
MPDA@GSNO NO/PTT 808 nm, 0.75 W/cm2, 10min S. aureus/E. coli 143
GNS/HPDA-BNN6 NO/PTT 808 nm, 1.5 W/cm2, 10min S. aureus/E. coli/MRSA(100 μg/mL) 132
α-CD-Ce6-NO-DA NO/PDT 660 nm, 0.2 W/cm2, 1min MRSA biofilms(Ce6:40 μg/mL, NO:80 μg/mL) 144
UCNP@PCN@LA-PVDF NO/PDT 980 nm, 2.5 W/cm2, 5min P. aeruginosa/S. aureus 145
Ce6&CO@FADP CO/PDT 665 nm, 11 W/cm2, 8min S. aureus/E. coli(200 μg/mL)S. aureus/E. coli biofilms(800 μg/mL) 146
Ce6@Arg-ADP NO/PDT 665 nm, 115 mW/cm2, 30min MRSA/E. coli(32 μg/mL); MRSA/E. coli biofilms 125
TPP-HF micelles CO/PDT 650 nm, 26 mW/cm2, 30min S. aureus/MRSA(0.1 g/L)/E. coli 136
MAO+ZI PDT/I 808 nm,1 W/cm2, 10min S. aureus 147
CuTCPP-Fe2O3 PDT/Fe3+/Cu2+ 660 nm, 20min P. gingivalis/F. nucleatum/S. aureus 148
Ti-RP-IR780-RGDC PTT/PDT 808 nm, 0.5 W/cm2, 10min S. aureus biofilms 149
MOF-PDA PTT/PDT 660 nm, 0.7 W/cm2, 20min S. aureus/E. coli 140
Ti-MoS2-IR780-PDA-RGDC PTT/PDT 808 nm, 0.5 W/cm2, 20min S. aureus biofilms 137
UCNPs@PFC-55 PTT/PDT 980 nm, 1.5 W/cm2 E. coli 150
CuS@BSA/rGO-PDA PTT/PDT 808 nm, 1 W/cm2, 10min S. aureus/E. coli 142
CuS@HKUST-PDA PTT/PDT 808 nm, 20min S. aureus/E. coli(300 mg/L) 141
SCN-Zn2+@GO PTT/PDT 808 nm, 1 W/cm2, 10min, 660 nm S. aureus/E. coli(50 μg/mL) 151
ZIF-8-ICG PTT/Zn2+ 808 nm,1 W/cm2,30min MRSA(15.6 μg/mL) 152
ZnO-CNP-TRGL PTT/Zn2+ 808 nm, 2 W/cm2, 5min S. aureus/E. coli(50 μg/mL) 153
HuA@ZIF-8 PTT/Zn2+ 808 nm, 20min S. aureus/E. coli(1000 μg/mL) 154
GNR-PDA@Zn PTT/Zn2+ 808 nm, 1.5 W/cm2, 5min S. aureus/E. coli 155
Au-Ag@SiO2 NCs PTT/Ag+ 808 nm, 1 W/cm2, 5min S. aureus/E. coli(128 μg/mL) 156
Ag-Bi@SiO2 NPs PTT/Ag+ 808 nm,1 W/cm2, 15min MRSA(128 μg/mL)/MRSA biofilms 157
Au/Ag NRs PTT/Ag+ 1064 nm, 0.8 W/cm2, 10min MRSA(100 μM Ag) 158
PB@PDA@Ag PTT/Ag+ 808 nm, 1 W/cm2, 5min S. aureus/MRSA/MRSA biofilms/E. coli/Ampr E. coli(200 μg/mL PB) 159
GSNCs-Cyh PTT/Ag+ 1064 nm, 0.75 W/cm2, 10min MRSA/MDR E. coli 160
C-Zn/Ag PTT/Zn2+/Ag+ 808 nm, 3 W/cm2, 10min S. aureus/E. coli(0.16 mg/mL) 161
CNSs@FeS2 PTT/Fe2+ 808 nm, 2.5 W/cm2, 10min S. aureus/E. coli/S. typhimurium/P. aeruginosa/S. mutants/M. albicans(500 μg/mL) 162
CP@WS2 NFs PTT/CDT 808 nm, 1 W/cm2, 10min S. aureus/E. coli(100 μg/mL) 163
Au/MoO3-x PTT/CDT 808 nm, 1 W/cm2, 10min MRSA(128 μg/mL) 164
RCF PTT/CDT 1064 nm, 0.5 W/cm2, 5min MRSA(256 μg/mL)/S. aureus(256 μg/mL)/E. coli(128 μg/mL) 165
Ni@Co-NC PTT/CDT 808 nm,1 W/cm2, 5min MRSA(62.5 μg/mL) 166
Cu SASs/NPC PTT/CDT 808 nm, 1 W/cm2, 10min E. coli/MRSA(300 μg/mL) 167
AI-MPDA PTT/PDT/NO 808 nm,1 W/cm2, 10min S. aureus biofilms(0.2 mg/mL) 35
GNR@mSiO2-SNO/ICG PTT/PDT/NO 808 nm, 1 W/cm2, 5min P. gingivalis/F. nucleatum/S. gordonii biofilm 168
ICG&CO@G3KBPY PTT/PDT/CO 808 nm, 1 W/cm2, 5min MRSA/MRSA biofilms(150 μg/mL) 169
DNase-AuNCs PTT/PDT/DNase I 808 nm, 2 W/cm2, 10min S. aureus/P. aeruginosa/S. epidermidis/E. coli biofilms(400 μg/mL) 170
MoS2/ICG/Ag PTT/PDT/Ag+ 808 nm, 1 W/cm2, 10min S. aureus(150 μg/mL)/E. coli(250 μg/mL) 171
AgB NDs PTT/PDT/Ag+ 808 nm, 1 W/cm2, 5min MRSA(250 μg/mL) 172
CuFe2O4/GO PTT/PDT/CDT 808 nm, 1 W/cm2, 10min S. aureus/E. coli 173
Ag-PCN@Ti3C2-BC PTT/PDT/Ag+ 780 nm S. aureus/E. coli 174
ZnO/CDots/g-C3N4 PTT/PDT/Zn2+ visible light, 1 W/cm, 15min S. aureus/E. coli(200 μg/mL) 175
CuS/GO PTT/PDT/Cu2+ 0.2 W/cm2, 15min S. aureus/E. coli 176
ZnDMZ PTT/PDT/Zn2+ 660 nm, 0.45 W/cm2, 20min S. aureus 177
MoO3-x NDs PTT/PDT/CDT 808 nm, 2 W/cm2, 20min MRSA/ESBL-producing E. coli(90 μg/mL) 178
ICG-ZnS NPs PTT/H2S/Zn2+ 808 nm, 1 W/cm2, 10min MRSA biofilm(32 μg/mL) 100
DNase-CO@MPDA NPs PTT/CO/DNase I 808 nm, 1 W/cm2, 10min MRSA biofilms(200 μg/mL) 179
Fe3O4@MoS2-Ag PTT/CDT/Ag+ 808 nm, 1 W/cm2, 15min S. aureus/B. subtilis/MRSA/C. albicans 180
SM@CuFeSe2 PTT/CDT/immunity 808 nm, 4 W/cm2, 15min S. aureus 181
FPMLC PTT/carvacrol/LYZ 808 nm, 3 W/cm2, 10min S. aureus/E. coli(100 μg/mL) 182
CuS/Cur PTT/PDT/SDT/Cur/Cu2+ 808 nm, 0.5 W/cm2, 15min S. aureus/E. coli(2 mg/mL) 183
图10 (a)核壳UCNPs@PFC-55的制备和(b)从UCNPs“核”到PFC-55“壳”的RET过程以实现NIR响应的光热和光动力效应[150]
Fig. 10 (a) Fabrication of core-shell UCNPs@PFC-55; (b) the RET process from UCNPs“core” to PFC-55“shell” for achieving NIR-response photothermal and photodynamic effects[150]. Copyright 2021, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
图11 (a) RCF纳米杂化物的制备和协同抗菌机制; (b)用RCF (0~1024 μg/mL)处理的MRSA形成的细菌菌落平板照片,有或无NIR照射和H2O2; (c) MRSA在用RCF处理后通过平板计数法测定的不同组中的相应细菌存活率[165]
Fig. 11 (a) Preparation of RCF nanohybrid and the antibacterial mechanism; (b) photographs of bacterial colonies formed by MRSA treated with RCF (0~1024 μg/mL) with or without NIR irradiation and H2O2; (c) the corresponding bacterial viabilities of MRSA after treatment with RCF in different groups determined by the plate counting method[165]. Copyright 2021, American Chemical Society
图12 (a) DNase-CO@MPDA NPs的制备和(b) DNase I参与,CO增强PTT的 MRSA生物膜消除机制[179]
Fig. 12 (a) The preparation of DNase-CO@MPDA NPs; (b) the MRSA biofilm elimination mechanism based on DNase I participation and CO-potentiated PTT[179]. Copyright 2021, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
图13 病原体受体膜包覆(112)和(100)面CuFeSe2纳米晶体的制备及抗菌机制[181]
Fig. 13 Fabrication and antibacterial mechanism of pathogen receptor membrane-coated (112)- and (100)-faceted CuFeSe2 nanocrystals[181]. Copyright 2021, American Chemical Society
图14 (a) RBC-HNTM-Pt@Au的合成、声催化机制以及通过高效SDT治疗骨髓炎; (b)不同条件处理后的MRSA菌落数和(c)相应SEM图像及活/死细菌荧光染色图像; (d)不同条件处理后MRSA内蛋白释放量; (e)用US+1-RBC-HNTM-Pt@Au、US+2-RBC-HNTM-Pt@Au和US+3-RBC-HNTM-Pt@Au处理后的MRSA菌落数及(f), (g)细胞活力(1d、3d)[190]
Fig. 14 (a) Synthesis of RBC-HNTM-Pt@Au, sonocatalytic mechanism, and the treatment of osteomyelitis by efficient SDT; (b) number of MRSA colonies treated under different conditions and (c) the corresponding SEM images and fluorescent staining images of live/dead bacteria; (d) the amount of MRSA protein leaked after treatment under different conditions; (e) number of MRSA colonies and (f),(g) cell viability (1 and 3 days) after treatment with US + 1-RBC-HNTM-Pt@Au, US + 2-RBC-HNTM-Pt@Au, and US + 3-RBC-HNTM-Pt@Au[190]. Copyright 2021, American Chemical Society
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