Chloride-accelerated Cu-Fenton chemistry for biofilm removal

Wang, Li; Miao, Yanni; Lu, Mang; Shan, Zhi; Lu, Shan; Hou, Jiaojiao; Yang, Qiumei; Liang, Xinmiao; Zhou, Tao; Curry, Dennis E.; Oakes, Ken D.; Zhang, Xu

doi:10.1039/c7cc00928c

Cited by 22 publications

(6 citation statements)

References 75 publications

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“…Overall, CuFe 5 O 8 NCs exhibited excellent destructive effects on eDNA and biofilm by catalyzing the •OH generation in situ , which was as expected. Recently, some effective strategies, such as antibacterial nanoparticle coating, DNase, , antibiotic-loaded nanoparticles, DNase-mimetic artificial enzyme (DMAE), oxidase-like or peroxidase-like nanomaterials, − haloperoxidase-like nanomaterials, and photothermal nanomaterials, ,, were applied to combat the stubborn biofilms by killing bacteria, inhibiting bacterial adhesion, or triggering the degradation of EPS (nucleic acids, proteins, and polysaccharides) in biofilms (Table S1). The immunosuppressive state induced by biofilm was often overlooked, and few studies have focused on immunoregulation or immunotherapy for biofilm-associated infections (Table S1).…”

Section: Results and Discussionmentioning

confidence: 99%

Space-Selective Chemodynamic Therapy of CuFe₅O₈ Nanocubes for Implant-Related Infections

et al. 2020

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Implant-related infections (IRIs) are a serious complication after orthopedic surgery, especially when a biofilm develops and establishes physical and chemical barriers protecting bacteria from antibiotics and the hosts local immune system. Effectively eliminating biofilms is essential but difficult, as it requires not only breaking the physical barrier but also changing the chemical barrier that induces an immunosuppressive microenvironment. Herein, tailored to a biofilm microenvironment (BME), we proposed a space-selective chemodynamic therapy (CDT) strategy to combat IRIs using metastable CuFe5O8 nanocubes (NCs) as smart Fenton-like reaction catalysts whose activity can be regulated by pH and H2O2 concentration. In the biofilm, extracellular DNA (eDNA) was cleaved by high levels of hydroxyl radicals (•OH) catalyzed by CuFe5O8 NCs, thereby disrupting the rigid biofilm. Outside the biofilm with relatively higher pH and lower H2O2 concentration, lower levels of generated •OH effectively reversed the immunosuppressive microenvironment by inducing pro-inflammatory macrophage polarization. Biofilm fragments and exposed bacteria were then persistently eliminated through the collaboration of pro-inflammatory immunity and •OH. The spatially selective activation of CDT and synergistic immunomodulation exerted excellent effects on the treatment of IRIs in vitro and in vivo. The anti-infection strategy is expected to provide a method to conquer IRIs.

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Section: Results and Discussionmentioning

confidence: 99%

Space-Selective Chemodynamic Therapy of CuFe₅O₈ Nanocubes for Implant-Related Infections

et al. 2020

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“…To find out which of the major EPS components in S. aureus biofilms interacted with ZW-MSPMs, the interaction of herring sperm DNA [as an eDNA mimic in the EPS matrix ( 46 , 47 )] and amyloid fibrils [endogenous to S. aureus biofilms ( 48 – 50 )] with ZW-MSPMs was investigated using different in vitro methods. In an acidic environment, positively charged ZW-MSPMs in PBS (pH 5.0) interacted significantly better with DNA ( Fig.…”

Section: Resultsmentioning

confidence: 99%

Self-targeting, zwitterionic micellar dispersants enhance antibiotic killing of infectious biofilms—An intravital imaging study in mice

Tian

Liu

et al. 2020

Sci. Adv.

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Extracellular polymeric substances (EPS) hold infectious biofilms together and limit antimicrobial penetration and clinical infection control. Here, we present zwitterionic micelles as a previously unexplored, synthetic self-targeting dispersant. First, a pH-responsive poly(ε-caprolactone)-block-poly(quaternary-amino-ester) was synthesized and self-assembled with poly(ethylene glycol)-block-poly(ε-caprolactone) to form zwitterionic, mixed-shell polymeric micelles (ZW-MSPMs). In the acidic environment of staphylococcal biofilms, ZW-MSPMs became positively charged because of conversion of the zwitterionic poly(quaternary-amino-ester) to a cationic lactone ring. This allowed ZW-MSPMs to self-target, penetrate, and accumulate in staphylococcal biofilms in vitro. In vivo biofilm targeting by ZW-MSPMs was confirmed for staphylococcal biofilms grown underneath an implanted abdominal imaging window through direct imaging in living mice. ZW-MSPMs interacted strongly with important EPS components such as eDNA and protein to disperse biofilm and enhance ciprofloxacin efficacy toward remaining biofilm, both in vitro and in vivo. Zwitterionic micellar dispersants may aid infection control and enhance efficacy of existing antibiotics against remaining biofilm.

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“…Consequently, • OH and O2 •are detectable only at low static concentrations in the system (they occasionally escape the catalytic cycle, as detectable through reaction with coumarin or XTT, respectively), while 1 O2 leaves the cycle as an end product. Chlorination was occasionally detected in the system, 33,38 but only at lower pH values with high concentrations of Cu and Clin a manner different from the other three ROS; thus, Cl • is not considered an intermediate. A mechanism governing 1 O2 generation within the catalytic cycle is proposed in Fig.…”

Section: Mechanistic Understandingmentioning

confidence: 92%

“…As demonstrated in our previous work, 1 O2 was used either for ultrasensitive colorimetric detection of Cu ions in water samples 33 or for antibacterial or anti-biofilm applications. 38 Importantly, as a selective oxidant and electrophile, it has been widely employed for organic synthesis, such as Diels-Alder 2+2 and 2+4 cycloadditions and ene-like reactions. 1,13,[39][40][41][42] Herein, we demonstrate its application for selective synthesis of 1,4-benzoquinone (BQ) directly from phenol (PhOH), serving as a simple model of the selective oxidation of phenolic compounds, important intermediates for the pharmaceutical industry.…”

mentioning

confidence: 99%

Selective Generation of Singlet Oxygen in Chloride Accelerated Copper Fenton Chemistry

Carrier¹,

Nganou²,

Oakley³

et al. 2018

Preprint

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Singlet oxygen (1O2), a widely used reactive oxygen species (ROS) in industry and biomedical applications, plays a fundamental role throughout nature. We report a novel method to generate 1O2selectively and efficiently through copper-based Fenton chemistry under circumneutral conditions enhanced by chloride as co-catalyst, with reactivity completely different than that observed in classical iron-based Fenton chemistry. The mechanism of its formation was elucidated through the kinetic studies of orthogonally reactive reporter molecules, i.e., singlet oxygen sensor green, 4-hydroxy-2,2,6,6-tetramethylpiperidine, and phenol, and selective ROS quenchers. This method selectively generates 1O2in situneither relying on photosensitization nor resulting in side reactions, and together with the mechanistic understanding of the Cu-Fenton reaction, not only opens new possibilities in many industries, such as organic synthesis and antimicrobial treatments, but also provides insight into Cu and H2O2containing chemical, environmental, and biological systems.

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Chloride-accelerated Cu-Fenton chemistry for biofilm removal

Abstract: Biofilms present challenges to numerous industries. Herein, a simple approach was developed based on chloride-accelerated Fenton chemistry, where copper oxide nanoparticles facilitate efficient generation of reactive chlorine species for biofilm removal.

Cited by 22 publications

References 75 publications

Space-Selective Chemodynamic Therapy of CuFe₅O₈ Nanocubes for Implant-Related Infections

Space-Selective Chemodynamic Therapy of CuFe₅O₈ Nanocubes for Implant-Related Infections

Self-targeting, zwitterionic micellar dispersants enhance antibiotic killing of infectious biofilms—An intravital imaging study in mice

Selective Generation of Singlet Oxygen in Chloride Accelerated Copper Fenton Chemistry

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Chloride-accelerated Cu-Fenton chemistry for biofilm removal

Abstract: Biofilms present challenges to numerous industries. Herein, a simple approach was developed based on chloride-accelerated Fenton chemistry, where copper oxide nanoparticles facilitate efficient generation of reactive chlorine species for biofilm removal.

Cited by 22 publications

References 75 publications

Space-Selective Chemodynamic Therapy of CuFe5O8 Nanocubes for Implant-Related Infections

Space-Selective Chemodynamic Therapy of CuFe5O8 Nanocubes for Implant-Related Infections

Self-targeting, zwitterionic micellar dispersants enhance antibiotic killing of infectious biofilms—An intravital imaging study in mice

Selective Generation of Singlet Oxygen in Chloride Accelerated Copper Fenton Chemistry

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Space-Selective Chemodynamic Therapy of CuFe₅O₈ Nanocubes for Implant-Related Infections

Space-Selective Chemodynamic Therapy of CuFe₅O₈ Nanocubes for Implant-Related Infections