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ACS Appl Mater Interfaces. 2017 May 10;9(18):15286-15296. doi: 10.1021/acsami.7b02529. Epub 2017 Apr 28.

Directing Assembly and Disassembly of 2D MoS2 Nanosheets with DNA for Drug Delivery.

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Department of Chemical and Biomolecular Engineering, National University of Singapore , Singapore 117585, Singapore.
World Premier International (WPI) Research for Materials Nanoarchitectonics (MANA), National Institute for Materials Science (NIMS) , 1-1 Namiki, Tsukuba 305-0044, Japan.
Department of Biomedical Engineering, National University of Singapore , Singapore 117575, Singapore.
Centre for Advanced 2D Materials, Graphene Research Centre, National University of Singapore , Singapore 117546, Singapore.
Mechanobiology Institute, National University of Singapore , Singapore 117411, Singapore.
NUS Graduate School for Integrative Sciences and Engineering, National University of Singapore , Singapore 117456, Singapore.
Department of Physics, National University of Singapore , Singapore 117542, Singapore.


Layer-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.


3D cell culture; DNA functionalization; layer-by-layer assembly; molybdenum disulfide; targeted chemotherapy

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