Synergistic Bacteria Killing through Photodynamic and Physical Actions of Graphene Oxide/Ag/Collagen Coating.

Researchers have widely agreed that the broad spectrum antibacterial activity of silver nanoparticles (AgNPs) can be predominantly ascribed to the action of Ag+. This study marks the first report detailing the rapid and highly efficient synergistic bacteria killing of AgNPs, which is achieved by inspiring AgNPs' strong photocatalytic capability to rapidly produce radical oxygen species using 660 nm visible light together with the innate antimicrobial ability of Ag+. These AgNPs were uniformly distributed into well-defined graphene oxide (GO) nanosheets through an in situ reduction of Ag+ and subsequently wrapped with a thin layer of type I collagen. In vivo subcutaneous tests demonstrated that 20 min irradiation of 660 nm visible light could achieve a high antibacterial efficacy of 96.3% and 99.4% on the implant surface against Escherichia coli and Staphylococcus aureus, respectively. In addition, the collagen could reduce the coatings' possible cytotoxicity. The results of this work can provide a highly effective and universal GO-based bioplatform for combination with inorganic antimicrobial NPs (i.e., AgNPs) with excellent photocatalytic properties, which can be utilized for facile and rapid in situ disinfection, as well as long-term prevention of bacterial infection through the synergistic bacteria killing of both 660-nm light-inspired photodynamic action and their innate physical antimicrobial ability.

[1]  M. Papi,et al.  Erratum: Biomimetic antimicrobial cloak by graphene-oxide agar hydrogel , 2017, Scientific Reports.

[2]  Jie Ren,et al.  Synthesis of {111} Facet-Exposed MgO with Surface Oxygen Vacancies for Reactive Oxygen Species Generation in the Dark. , 2017, ACS applied materials & interfaces.

[3]  Marco De Spirito,et al.  The graphene oxide contradictory effects against human pathogens , 2017, Nanotechnology.

[4]  Zhuo Chen,et al.  Synthesis of Multifunctional Cationic Poly(p-phenylenevinylene) for Selectively Killing Bacteria and Lysosome-Specific Imaging. , 2017, ACS applied materials & interfaces.

[5]  Yizhou Zhu,et al.  Construction of poly (vinyl alcohol)/poly (lactide-glycolide acid)/vancomycin nanoparticles on titanium for enhancing the surface self-antibacterial activity and cytocompatibility. , 2017, Colloids and surfaces. B, Biointerfaces.

[6]  A. Lee,et al.  Cobalt promoted TiO2/GO for the photocatalytic degradation of oxytetracycline and Congo Red , 2017 .

[7]  Jung-Sik Kim,et al.  Solvothermal synthesis of anatase TiO2-graphene oxide nanocomposites and their photocatalytic performance , 2016 .

[8]  Marco De Spirito,et al.  Biomimetic antimicrobial cloak by graphene-oxide agar hydrogel , 2016, Scientific Reports.

[9]  K. Yeung,et al.  Dopamine Modified Organic-Inorganic Hybrid Coating for Antimicrobial and Osteogenesis. , 2016, ACS applied materials & interfaces.

[10]  Marco De Spirito,et al.  The future development of bacteria fighting medical devices: the role of graphene oxide , 2016, Expert review of medical devices.

[11]  Yizhou Zhu,et al.  Surface functionalization of biomaterials by radical polymerization , 2016 .

[12]  H. Gu,et al.  Antibiotic-loaded, silver core-embedded mesoporous silica nanovehicles as a synergistic antibacterial agent for the treatment of drug-resistant infections. , 2016, Biomaterials.

[13]  Huijun Zhao,et al.  Synergistic photocatalytic inactivation mechanisms of bacteria by graphene sheets grafted plasmonic AgAgX (X = Cl, Br, I) composite photocatalyst under visible light irradiation. , 2016, Water research.

[14]  Minqiang Wang,et al.  The role of reduction extent of graphene oxide in the photocatalytic performance of Ag/AgX (X = Cl, Br)/rGO composites and the pseudo-second-order kinetics reaction nature of the Ag/AgBr system. , 2016, Physical chemistry chemical physics : PCCP.

[15]  Kuo Chu Hwang,et al.  Nano-graphene oxide-mediated In vivo fluorescence imaging and bimodal photodynamic and photothermal destruction of tumors. , 2016, Biomaterials.

[16]  Yong Han,et al.  Antibacterial Activity of Silver Doped Titanate Nanowires on Ti Implants. , 2016, ACS applied materials & interfaces.

[17]  Yibing Xie,et al.  Visible‐light‐driven self‐cleaning SERS substrate of silver nanoparticles and graphene oxide decorated nitrogen‐doped titania nanotube array , 2016 .

[18]  Xueji Zhang,et al.  Strong Antibacterial Polydopamine Coatings Prepared by a Shaking-assisted Method , 2016, Scientific Reports.

[19]  Zhenkun Zhang,et al.  Surface-Adaptive, Antimicrobially Loaded, Micellar Nanocarriers with Enhanced Penetration and Killing Efficiency in Staphylococcal Biofilms. , 2016, ACS nano.

[20]  Hsiu-Yao Cheng,et al.  Reversible Association of Nitro Compounds with p-Nitrothiophenol Modified on Ag Nanoparticles/Graphene Oxide Nanocomposites through Plasmon Mediated Photochemical Reaction. , 2016, ACS applied materials & interfaces.

[21]  H. Peng,et al.  Large-area chemical vapor deposition-grown monolayer graphene-wrapped silver nanowires for broad-spectrum and robust antimicrobial coating , 2016, Nano Research.

[22]  S. G. Harroun,et al.  Self‐Assembly of Antimicrobial Peptides on Gold Nanodots: Against Multidrug‐Resistant Bacteria and Wound‐Healing Application , 2015 .

[23]  Ivan Mfouo-Tynga,et al.  Comparative study between the photodynamic ability of gold and silver nanoparticles in mediating cell death in breast and lung cancer cell lines. , 2015, Journal of photochemistry and photobiology. B, Biology.

[24]  Xiaoying Zhu,et al.  Layer-by-layer assemblies for antibacterial applications. , 2015, Biomaterials science.

[25]  D. Mccarthy,et al.  Silver/Reduced Graphene Oxide Hydrogel as Novel Bactericidal Filter for Point‐of‐Use Water Disinfection , 2015 .

[26]  V. Rotello,et al.  Nanoparticle-Stabilized Capsules for the Treatment of Bacterial Biofilms. , 2015, ACS nano.

[27]  Arunava Gupta,et al.  Plasmonic Enhancement of Photoactivity by Gold Nanoparticles Embedded in Hematite Films , 2015 .

[28]  Suck Won Hong,et al.  Stimulated myoblast differentiation on graphene oxide-impregnated PLGA-collagen hybrid fibre matrices , 2015, Journal of Nanobiotechnology.

[29]  B. Hong,et al.  Covalent conjugation of mechanically stiff graphene oxide flakes to three-dimensional collagen scaffolds for osteogenic differentiation of human mesenchymal stem cells , 2015 .

[30]  W. Liu,et al.  High-performance asymmetric supercapacitors based on multilayer MnO2 /graphene oxide nanoflakes and hierarchical porous carbon with enhanced cycling stability. , 2015, Small.

[31]  R. Advíncula,et al.  On the antibacterial mechanism of graphene oxide (GO) Langmuir-Blodgett films. , 2015, Chemical communications.

[32]  K. Chatterjee,et al.  Chemical functionalization of graphene to augment stem cell osteogenesis and inhibit biofilm formation on polymer composites for orthopedic applications. , 2015, ACS applied materials & interfaces.

[33]  Robert J. Ono,et al.  Brush‐Like Polycarbonates Containing Dopamine, Cations, and PEG Providing a Broad‐Spectrum, Antibacterial, and Antifouling Surface via One‐Step Coating , 2014, Advanced materials.

[34]  P. Chu,et al.  Polymeric nanoarchitectures on Ti-based implants for antibacterial applications. , 2014, ACS applied materials & interfaces.

[35]  Xianlong Zhang,et al.  Synergistic effects of dual Zn/Ag ion implantation in osteogenic activity and antibacterial ability of titanium. , 2014, Biomaterials.

[36]  H. Abrahamse,et al.  Photodynamic ability of silver nanoparticles in inducing cytotoxic effects in breast and lung cancer cell lines , 2014 .

[37]  C. Fan,et al.  Laundering durable antibacterial cotton fabrics grafted with pomegranate-shaped polymer wrapped in silver nanoparticle aggregations , 2014, Scientific Reports.

[38]  A. D. Todd,et al.  Harnessing the chemistry of graphene oxide. , 2014, Chemical Society reviews.

[39]  Jinqing Wang,et al.  A Novel Wound Dressing Based on Ag/Graphene Polymer Hydrogel: Effectively Kill Bacteria and Accelerate Wound Healing , 2014 .

[40]  Lingzhou Zhao,et al.  Antibacterial effects and biocompatibility of titanium surfaces with graded silver incorporation in titania nanotubes. , 2014, Biomaterials.

[41]  Jason A Inzana,et al.  3D printing of composite calcium phosphate and collagen scaffolds for bone regeneration. , 2014, Biomaterials.

[42]  Huang-Hao Yang,et al.  Multifunctional Fe₃O₄@polydopamine core-shell nanocomposites for intracellular mRNA detection and imaging-guided photothermal therapy. , 2014, ACS nano.

[43]  J. Xin,et al.  Multifunctional organically modified graphene with super-hydrophobicity , 2014, Nano Research.

[44]  Shuhong Yu,et al.  Bio-inspired in situ growth of monolayer silver nanoparticles on graphene oxide paper as multifunctional substrate. , 2013, Nanoscale.

[45]  Tao Chen,et al.  Nanotechnology in plant disease management: DNA-directed silver nanoparticles on graphene oxide as an antibacterial against Xanthomonas perforans. , 2013, ACS nano.

[46]  Jie Yin,et al.  Ag/AgBr/rGO nanocomposite: Synthesis and its application in photocatalysis , 2013 .

[47]  Kwang S. Kim,et al.  Stable platinum nanoclusters on genomic DNA–graphene oxide with a high oxygen reduction reaction activity , 2013, Nature Communications.

[48]  A. Talyzin,et al.  Effect of synthesis method on solvation and exfoliation of graphite oxide , 2013 .

[49]  X. Qu,et al.  New Horizons for Diagnostics and Therapeutic Applications of Graphene and Graphene Oxide , 2013, Advanced materials.

[50]  Zhe Zhang,et al.  Mussel-inspired functionalization of graphene for synthesizing Ag-polydopamine-graphene nanosheets as antibacterial materials. , 2013, Nanoscale.

[51]  Li Li,et al.  Green synthesis of graphene/Ag nanocomposites , 2012 .

[52]  Pedro J J Alvarez,et al.  Negligible particle-specific antibacterial activity of silver nanoparticles. , 2012, Nano letters.

[53]  Stella M. Marinakos,et al.  Mechanism of silver nanoparticle toxicity is dependent on dissolved silver and surface coating in Caenorhabditis elegans. , 2012, Environmental science & technology.

[54]  M. B. Cardoso,et al.  Size-selective silver nanoparticles: future of biomedical devices with enhanced bactericidal properties , 2011 .

[55]  Shu-Hong Yu,et al.  Facile synthesis of silver@graphene oxide nanocomposites and their enhanced antibacterial properties , 2011 .

[56]  Pinaki Sengupta,et al.  Synthesis of silver nanoparticles in an aqueous suspension of graphene oxide sheets and its antimicrobial activity. , 2011, Colloids and surfaces. B, Biointerfaces.

[57]  Omid Akhavan,et al.  Toxicity of graphene and graphene oxide nanowalls against bacteria. , 2010, ACS nano.

[58]  Z. Deng,et al.  Noncovalent DNA decorations of graphene oxide and reduced graphene oxide toward water-soluble metal–carbon hybrid nanostructures via self-assembly , 2010 .

[59]  S. Okabe,et al.  In vitro toxicity of silver nanoparticles at noncytotoxic doses to HepG2 human hepatoma cells. , 2009, Environmental science & technology.

[60]  Zhiqiang Hu,et al.  Role of sulfide and ligand strength in controlling nanosilver toxicity. , 2009, Water research.

[61]  Younan Xia,et al.  Facile synthesis of Ag nanocubes and Au nanocages , 2007, Nature Protocols.

[62]  J. Song,et al.  Does the Antibacterial Activity of Silver Nanoparticles Depend on the Shape of the Nanoparticle? A Study of the Gram-Negative Bacterium Escherichia coli , 2007, Applied and Environmental Microbiology.

[63]  Uday Narayan Maiti,et al.  Three‐Dimensional Shape Engineered, Interfacial Gelation of Reduced Graphene Oxide for High Rate, Large Capacity Supercapacitors , 2014, Advanced materials.

[64]  J. Bryers Bacterial biofilms. , 1993, Current opinion in biotechnology.