Antiadherent AgBDC Metal-Organic Framework Coating for Escherichia coli Biofilm Inhibition.

Surface microbial colonization and its potential biofilm formation are currently a major unsolved problem, causing almost 75% of human infectious diseases. Pathogenic biofilms are capable of surviving high antibiotic doses, resulting in inefficient treatments and, subsequently, raised infection prevalence rates. Antibacterial coatings have become a promising strategy against the biofilm formation in biomedical devices due to their biocidal activity without compromising the bulk material. Here, we propose for the first time a silver-based metal-organic framework (MOF; here denoted AgBDC) showing original antifouling properties able to suppress not only the initial bacterial adhesion, but also the potential surface contamination. Firstly, the AgBDC stability (colloidal, structural and chemical) was confirmed under bacteria culture conditions by using agar diffusion and colony counting assays, evidencing its biocide effect against the challenging E. coli, one of the main representative indicators of Gram-negative resistance bacteria. Then, this material was shaped as homogeneous spin-coated AgBDC thin film, investigating its antifouling and biocide features using a combination of complementary procedures such as colony counting, optical density or confocal scanning microscopy, which allowed to visualize for the first time the biofilm impact generated by MOFs via a specific fluorochrome, calcofluor.

Phase-Selective Microwave Assisted Synthesis of Iron(III) Aminoterephthalate MOFs.

Iron(III) aminoterephthalate Metal-Organic Frameworks (Fe-BDC-NH2 MOFs) have been demonstrated to show potential for relevant industrial and societal applications (i.e., catalysis, drug delivery, gas sorption). Nevertheless, further analysis is required in order to achieve their commercial production. In this work, a systematic synthetic strategy has been followed, carrying out microwave (MW) assisted hydro/solvothermal reactions to rapidly evaluate the influence of different reaction parameters (e.g., time, temperature, concentration, reaction media) on the formation of the benchmarked MIL-101-NH2, MIL-88B-NH2, MIL-53-NH2 and MIL-68-NH2 solids. Characterization of the obtained solids by powder X-ray diffraction, dynamic light scattering and transmission electron microscopy allowed us to identify trends to the contribution of the evaluated parameters, such as the relevance of the concentration of precursors and the impact of the reaction medium on phase crystallization. Furthermore, we presented here for the first time the MW assisted synthesis of MIL-53-NH2 in water. In addition, pure MIL-101-NH2 was also produced in water while MIL-88-NH2 was the predominant phase obtained in ethanol. Pure phases were produced with high space-time yields, unveiling the potential of MW synthesis for MOF industrialization.

An Ag-loaded photoactive nano-metal organic framework as a promising biofilm treatment.

Surface biofilm inhibition is still currently a considerable challenge. Among other organisms, Staphylococcus aureus is notable for its ability to form a strong biofilm with proved resistance to chemotherapy. Contamination of high-touch surfaces with S. aureus biofilm not only promotes disease spread but also generates tremendous health-associated costs. Therefore, development of new bactericidal and antiadhesive surface coatings is a priority. Considering that metal-organic frameworks (MOFs) have recently emerged as promising antibacterial agents, we originally report here the synthesis of a multi-active silver-containing nanoscaled MOF composite as a potential surface coating against S. aureus biofilm owing to a triple effect: intrinsic bactericide activity of the MOF, biocidal character of silver nanoparticles (AgNPs), and photoactivity after UVA irradiation. AgNPs were successfully entrapped within the benchmarked nanoscaled porous photoactive titanium(IV) aminoterephthalate MIL-125(Ti)NH2 using a simple and efficient impregnation-reduction method. After complete characterization of the composite thin film, its antibacterial and anti-adherent properties were fully evaluated. After UVA irradiation, the composite coating exhibited relevant bacterial inhibition and detachment, improved ligand-to-cluster charge transfer, and steady controlled delivery of Ag+. These promising results establish the potential of this composite as an active coating for biofilm treatment on high-touch surfaces (e.g., surgical devices, door knobs, and rail bars). STATEMENT OF SIGNIFICANCE: Surface contamination due to bacterial biofilm formation is still a demanding issue, as it causes severe disease spread. One possible solution is the development of antifouling and antibacterial surface coatings. In this work, we originally propose the use of photoactive metal-organic frameworks (MOFs) for biofilm treatment. The novelty of this work relies on the following: i) the treatment of strongly contaminated surfaces, as previous studies with MOFs have exclusively addressed biofilm prevention; ii) this pioneering work reports both antiadherent effect, which removes the biofilm, and bacterial inhibition; iii) our original successful strategy has never been proposed thus far, involving the multi-active combination of 1) intrinsic antibacterial effect of a photoactive titanium-based nanoMOF, 2) immobilization of biocide silver nanoparticles, and 3) improved anti-bioadherent effect upon irradiation of the composite coating.

Aqueous Stable Gold Nanostar/ZIF-8 Nanocomposites for Light-Triggered Release of Active Cargo Inside Living Cells.

A plasmonic core-shell gold nanostar/zeolitic-imidazolate-framework-8 (ZIF-8) nanocomposite was developed for the thermoplasmonic-driven release of encapsulated active molecules inside living cells. The nanocomposites were loaded, as a proof of concept, with bisbenzimide molecules as functional cargo and wrapped with an amphiphilic polymer that prevents ZIF-8 degradation and bisbenzimide leaking in aqueous media or inside living cells. The demonstrated molecule-release mechanism relies on the use of near-IR light coupled to the plasmonic absorption of the core gold nanostars, which creates local temperature gradients and thus, bisbenzimide thermodiffusion. Confocal microscopy and surface-enhanced Raman spectroscopy (SERS) were used to demonstrate bisbenzimide loading/leaking and near-IR-triggered cargo release inside cells, thereby leading to DNA staining.

Aqueous Synthesis of Copper(II)-Imidazolate Nanoparticles.

A green, simple, and efficient room-temperature aqueous synthetic route for the fabrication of novel porous coordination polymer nanoparticles (NPs) composed of Cu2+ and imidazolate was developed. Colloidal stability, morphology changes, and structural and chemical integrity of the developed NPs, in several solvents having different polarity, were investigated. Basic physicochemical properties of selected NPs (i.e., NP1, NP2, and NP3), such as size, optical and magnetic activity, porosity, thermal stability, structure, aging, and catalytic activity, were determined. Data indicate that the addition of the surfactant hexadecyltrimethylammonium bromide (CTAB) and the final solvent determine the size, morphology, and structure of the different NPs.