am7b02529_si_001.pdf (1.55 MB)
Directing Assembly and Disassembly of 2D MoS2 Nanosheets with DNA for Drug Delivery
journal contribution
posted on 2017-04-28, 11:48 authored by Bang Lin Li, Magdiel I. Setyawati, Linye Chen, Jianping Xie, Katsuhiko Ariga, Chwee-Teck Lim, Slaven Garaj, David Tai LeongLayer-by-layer (LbL) self-assembled
stacked Testudo-like MoS2 superstructures
carrying cancer drugs are formed from nanosheets controllably assembled
with sequence-based DNA oligonucleotides. These superstructures can
disassemble autonomously in response to cancer cells’ heightened
ATP metabolism. First, we functionalize MoS2 nanosheets
(MoS2-NS) nanostructures with DNA oligonucleotides having
thiol-terminated groups (DNA/MoS2-NS) via strong binding
to sulfur atom defect vacancies on MoS2 surfaces. The driving
force to assemble into a higher-order DNA/MoS2-NS superstructure
is guided by a linker aptamer that induced interlayer assembly. In
the presence of target ATP molecules, these multilayer superstructures
disassembled as a consequence of stronger binding of ATP molecules
with the linking aptamers. This design plays a dual role of protection
and delivery by LbL stacked MoS2-NS similar in concept
to a Greek Testudo. These superstructures present
a protective armor-like shell of MoS2-NS, which still remains
responsive to small and infiltrating ATP molecules diffusing through
the protective MoS2-NS, contributing to an enhanced stimuli-responsive
drug release system for targeted chemotherapy.