In
this work, 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@Ag@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.