DNA origami protection and molecular interfacing through engineered sequence-defined peptoids

Wang, Shih-Ting; Gray, Melissa A.; Xuan, Sunting; Lin, Yiyang; Byrnes, James; Nguyen, Andy I.; Todorova, Nevena; Stevens, Molly M.; Bertozzi, Carolyn R.; Zuckermann, Ronald N.; Gang, Oleg

doi:10.1073/pnas.1919749117

Title: DNA origami protection and molecular interfacing through engineered sequence-defined peptoids

Journal Article · Thu Mar 12 00:00:00 EDT 2020 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1919749117· OSTI ID:1604260

Wang, Shih-Ting; Gray, Melissa A.;

; Lin, Yiyang; Byrnes, James; Nguyen, Andy I.;

; Stevens, Molly M.;

;

; Gang, Oleg

DNA nanotechnology has established approaches for designing programmable and precisely controlled nanoscale architectures through specific Watson−Crick base-pairing, molecular plasticity, and intermolecular connectivity. In particular, superior control over DNA origami structures could be beneficial for biomedical applications, including biosensing, in vivo imaging, and drug and gene delivery. However, protecting DNA origami structures in complex biological fluids while preserving their structural characteristics remains a major challenge for enabling these applications. Here, we developed a class of structurally well-defined peptoids to protect DNA origamis in ionic and bioactive conditions and systematically explored the effects of peptoid architecture and sequence dependency on DNA origami stability. The applicability of this approach for drug delivery, bioimaging, and cell targeting was also demonstrated. A series of peptoids (PE1–9) with two types of architectures, termed as “brush” and “block,” were built from positively charged monomers and neutral oligo-ethyleneoxy monomers, where certain designs were found to greatly enhance the stability of DNA origami. Through experimental and molecular dynamics studies, we demonstrated the role of sequence-dependent electrostatic interactions of peptoids with the DNA backbone. We showed that octahedral DNA origamis coated with peptoid (PE2) can be used as carriers for anticancer drug and protein, where the peptoid modulated the rate of drug release and prolonged protein stability against proteolytic hydrolysis. Finally, we synthesized two alkyne-modified peptoids (PE8 and PE9), conjugated with fluorophore and antibody, to make stable DNA origamis with imaging and cell-targeting capabilities. Our results demonstrate an approach toward functional and physiologically stable DNA origami for biomedical applications.

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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; AC02-05CH11231; SC0008772; KP1605010

OSTI ID:: 1604260

Alternate ID(s):: OSTI ID: 1607714

Report Number(s):: BNL-213757-2020-JAAM

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Vol. 117 Journal Issue: 12; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 77 works

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