DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Templated Mesoporous Silica Outer Shell for Controlled Silver Release of a Magnetically Recoverable and Reusable Nanocomposite for Water Disinfection

Journal Article · · ACS Applied Materials and Interfaces

Here, we encapsulated Fe3O4@SiO2@Ag (MS-Ag), a bifunctional magnetic silver core–shell structure, with an outer mesoporous silica (mS) shell to form an Fe3O4@SiO2@2Ag@mSiO2 (MS-Ag-mS) nanocomposite using a cationic CTAB (cetyltrimethylammonium bromide) micelle templating strategy. The mS shell acts as protection to slow down the oxidation and detachment of the AgNPs and incorporates channels to control the release of antimicrobial Ag+ ions. Results of TEM, STEM, HRSEM, EDS, BET, and FTIR showed the successful formation of the mS shells on MS-Ag aggregates 50–400 nm in size with highly uniform pores ~4 nm in diameter that were separated by silica walls ~2 nm thick. Additionally, the mS shell thickness was tuned to demonstrate controlled Ag+ release; an increase in shell thickness resulted in an increased path length required for Ag+ ions to travel out of the shell, reducing MS-Ag-mS’ ability to inhibit E. coli growth as illustrated by the inhibition zone results. Through a shaking test, the MS-Ag-mS nanocomposite was shown to eradicate 99.99+% of a suspension of E. coli at 1 × 106 CFU/mL with a silver release of less than 0.1 ppb, well under the EPA recommendation of 0.1 ppm. This high biocidal efficiency with minimal silver leach is ascribed to the nanocomposite’s mS shell surface characteristics, including having hydroxyl groups and possessing a high degree of structural periodicity at the nanoscale or “smoothness” that encourages association with bacteria and retains high Ag+ concentration on its surface and in its close proximity. Furthermore, the nanocomposite demonstrated consistent antimicrobial performance and silver release levels over multiple repeated uses (after being recovered magnetically because of the oxidation-resistant silica-coated magnetic Fe3O4 core). It also proved effective at killing all microbes from Long Island Sound surface water. The described MS-Ag-mS nanocomposite is highly synergistic, easy to prepare, and readily recoverable and reusable and offers structural tunability affecting the bioavailability of Ag+, making it excellent for water disinfection that will find wide applications.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
1841115
Report Number(s):
BNL-222613-2022-JAAM
Journal Information:
ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 40 Vol. 13; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (69)

Self-Assembled Highly Ordered Spherical Mesoporous Silica/Gold Nanocomposites journal April 2002
Superparamagnetic Ag@Co-Nanocomposites on Granulated Cation Exchange Polymeric Matrices with Enhanced Antibacterial Activity for the Environmentally Safe Purification of Water journal December 2012
Core-Shell Synthesis of a Novel, Spherical, Mesoporous Silica/Platinum Nanocomposite: Pt/PVP@MCM-41 journal October 2004
Antimicrobial Activity of Silver Nanocrystals Encapsulated in Mesoporous Silica Nanoparticles journal May 2009
Magnetic Nanoparticles: Synthesis, Protection, Functionalization, and Application journal February 2007
Polysaccharide-based silver nanoparticles synthesized by Klebsiella oxytoca DSM 29614 cause DNA fragmentation in E. coli cells journal February 2016
Rattle-type silica colloidal particles prepared by a surface-protected etching process journal July 2009
Enhanced antibacterial activity of bifunctional Fe3O4-Ag core-shell nanostructures journal December 2009
Silver nanoparticles-decorated and mesoporous silica coated single-walled carbon nanotubes with an enhanced antibacterial activity for killing drug-resistant bacteria journal January 2020
Direct observation of electron-beam-induced densification and hardening of silica nanoballs by in situ transmission electron microscopy and finite element method simulations journal October 2014
Antibiotic-loaded, silver core-embedded mesoporous silica nanovehicles as a synergistic antibacterial agent for the treatment of drug-resistant infections journal September 2016
Evaluation of the antibacterial activity of Ag/Fe 3 O 4 nanocomposites synthesized using starch journal June 2016
Investigation of formation of silica-coated magnetite nanoparticles via sol–gel approach journal July 2005
Facile synthesis of Fe3O4/SiO2 composite nanoparticles from primary silica particles journal March 2008
Immobilizing silver nanoparticles onto the surface of magnetic silica composite to prepare magnetic disinfectant with enhanced stability and antibacterial activity journal February 2011
Deposition of silver nanoparticles on silica spheres and rods journal October 2012
E. coli interactions, adhesion and transport in alumino-silica clays journal June 2017
Boosting antibacterial activity with mesoporous silica nanoparticles supported silver nanoclusters journal November 2019
Facile loading of Ag nanoparticles onto magnetic microsphere by the aid of a tannic acid—Metal polymer layer to synthesize magnetic disinfectant with high antibacterial activity journal January 2018
Efficient disinfection of Escherichia coli in water by silver loaded alumina journal September 2008
The magnetic and oxidation behavior of bare and silica-coated iron oxide nanoparticles synthesized by reverse co-precipitation of ferrous ion (Fe2+) in ambient atmosphere journal March 2014
Silica-based mesoporous materials; emerging designer adsorbents for aqueous pollutants removal and water treatment journal August 2018
Effect of magnetic nanoparticles and silver-loaded magnetic nanoparticles on advanced wastewater treatment and disinfection journal April 2020
Antibacterial activity of silver nanoparticles: A surface science insight journal June 2015
A novel green synthesis of Fe3O4-Ag core shell recyclable nanoparticles using Vitis vinifera stem extract and its enhanced antibacterial performance journal January 2015
Superparamagnetic iron oxide nanoparticles for full-color photonic materials with tunable properties journal September 2019
Disinfection of various bacterial pathogens using novel silver nanoparticle-decorated magnetic hybrid colloids journal December 2017
Characterisation of biosynthesised silver nanoparticles by scanning electrochemical microscopy (SECM) and voltammetry journal January 2015
Magnetic nanoparticles: Essential factors for sustainable environmental applications journal May 2013
Bacterial Inactivation Using Silver-Coated Magnetic Nanoparticles as Functional Antimicrobial Agents journal October 2011
Concentration Ranges of Antibacterial Cations for Showing the Highest Antibacterial Efficacy but the Least Cytotoxicity against Mammalian Cells: Implications for a New Antibacterial Mechanism journal August 2015
Preparing and Testing a Magnetic Antimicrobial Silver Nanocomposite for Water Disinfection To Gain Experience at the Nanochemistry–Microbiology Interface journal December 2016
Spectroscopic Evaluation of Removal Efficiency for a Pharmaceutical Pollutant in Water Using a Magnetite-Activated Carbon Nanocomposite journal March 2019
Core–Shell Silver Nanoparticles in Endodontic Disinfection Solutions Enable Long-Term Antimicrobial Effect on Oral Biofilms journal September 2017
Core–Shell AgCl@SiO 2 Nanoparticles: Ag(I)-Based Antibacterial Materials with Enhanced Stability journal May 2016
Water as the Solvent in the Stober Process for Forming Ultrafine Silica Shells on Magnetite Nanoparticles journal August 2019
On the Shelf Life and Aging Stability of Mesoporous Silica: Insights on Thermodynamically Stable MCM-41 Structure from Assessment of 12-Year-Old Samples journal October 2012
Removal of Aromatic Pollutant Surrogate from Water by Recyclable Magnetite-Activated Carbon Nanocomposite: An Experiment for General Chemistry journal July 2014
Occurrence of a New Generation of Disinfection Byproducts journal December 2006
Superparamagnetic High-Magnetization Microspheres with an Fe 3 O 4 @SiO 2 Core and Perpendicularly Aligned Mesoporous SiO 2 Shell for Removal of Microcystins journal January 2008
Synthesis and Characterization of Antibacterial Ag−SiO 2 Nanocomposite journal February 2007
Self-Assembly of Mesoporous Nanoscale Silica/Gold Composites journal July 2003
Silver Nanowires Can Be Directly Coated with Amorphous Silica To Generate Well-Controlled Coaxial Nanocables of Silver/Silica journal February 2002
Single-Step Coating of Mesoporous Silica on Cetyltrimethyl Ammonium Bromide-Capped Nanoparticles journal January 2008
Negligible Particle-Specific Antibacterial Activity of Silver Nanoparticles journal July 2012
Permeable Silica Shell through Surface-Protected Etching journal September 2008
Ordered mesoporous molecular sieves synthesized by a liquid-crystal template mechanism journal October 1992
Science and technology for water purification in the coming decades journal March 2008
Aggregation and sedimentation of magnetite nanoparticle clusters journal January 2016
A mechanistic study of silica-etching by hot water journal January 2018
Mesoporous silica-protected silver nanoparticle disinfectant with controlled Ag + ion release, efficient magnetic separation, and effective antibacterial activity journal January 2019
Nanostructured silver decorated hollow silica and their application in the treatment of microbial contaminated water at room temperature journal January 2019
Synthesis of monodisperse spherical silica particles with solid core and mesoporous shell: mesopore channels perpendicular to the surface journal January 2007
A facile one-pot synthesis of uniform core–shell silver nanoparticle@mesoporous silica nanospheres journal January 2011
A new synthesis of well-dispersed, core–shell Ag@SiO2 mesoporous nanoparticles using amino acids and sugars journal January 2013
Performance of silver nanoparticle fixed on magnetic iron nanoparticles () in water disinfection journal April 2018
Excellent antimicrobial properties of silver-loaded mesoporous silica SBA-15 journal February 2014
Relevance of Topographic Parameters on the Adhesion and Proliferation of Human Gingival Fibroblasts and Oral Bacterial Strains journal February 2019
Synthesis, Characterization, and Antibacterial Activity of Silver-Doped Silica Nanocomposite Particles journal January 2011
Effect of Solvents on the Preparation of Silica-Coated Magnetic Particles journal November 2001
Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report) journal October 2015
Micro- and Nanotopography Sensitive Bacterial Attachment Mechanisms: A Review journal February 2019
Magnetically Recoverable and Reusable Antimicrobial Nanocomposite Based on Activated Carbon, Magnetite Nanoparticles, and Silver Nanoparticles for Water Disinfection journal June 2017
Magnetically Recoverable and Reusable Titanium Dioxide Nanocomposite for Water Disinfection journal August 2021
Effect of Ethanol on Ag@Mesoporous Silica Formation by In Situ Modified Stöber Method journal May 2018
Mesoporous Silica Nanoparticles: A Comprehensive Review on Synthesis and Recent Advances journal August 2018
Microbial hitchhikers: dynamics of bacterial populations in ballast water during a trans-Pacific voyage of a bulk carrier journal January 2010
Approaches for determining the effects of UV radiation on microorganisms in ballast water journal June 2013
Reusable Magnetic Nanocomposite Sponges for Removing Oil from Water Discharges journal August 2017