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Progress in Chemistry 2022, Vol. 34 Issue (11): 2540-2560 DOI: 10.7536/PC220332 Previous Articles   

• Review •

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: Revised: Online: Published:
  • 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)
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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
Fig. 1 The statistics of the paper indexed in the ISI web of science by the topic of “nanomaterials” and “antibacterial agent”
Fig. 2 General DR mechanisms[2,6,40? ~42].(a) The DR pathways for planktonic bacteria and (b) Formation of biofilms
Fig. 3 Antibacterial mechanisms of nanomaterials[2,6,7,54,55]
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
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
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
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
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
Fig. 8 (a) The synthesis process of CuFe5O8NCs and (b) anti-biofilm and immunomodulatory mechanisms[102]. Copyright 2020, American Chemical Society
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
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
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
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
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
Fig. 13 Fabrication and antibacterial mechanism of pathogen receptor membrane-coated (112)- and (100)-faceted CuFeSe2 nanocrystals[181]. Copyright 2021, American Chemical Society
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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