2013 AIChE Annual Meeting

(413h) Molecular Recognition Using Nanotube-Adsorbed Polymer Complexes

Authors

Markita Landry - Presenter, University of California Berkeley
Jingqing Zhang, Massachusetts Institute of Technology
Paul W. Barone, Massachusetts Institute of Technology
Jong-Ho Kim, Hanyang University
Shangchao Lin, Massachusetts Institute of Technology
Zachary Ulissi, Massachusetts Institute of Technology
Dahua Lin, Massachusetts Institute of Technology
Bin Mu, Georgia Institute of Technology
Daniel A. Heller, Massachusetts Institute of Technology
Ardemis A. Boghossian, Massachusetts Institute of Technology
Andrew J. Hilmer, Massachusetts Institute of Technology
Alina Rwei, Massachusetts Institute of Technology
Allison Hinckley, Massachusetts Institute of Technology
Sebastian Kruss, Massachusetts Institute of Technology
Mia Shandell, Massachusetts Institute of Technology
Nitish Nair, Massachusetts Institute of Technology
Steven Blake, Massachusetts Institute of Technology
Fatih Sen, Massachusetts Institute of Technology
Selda Sen, Massachusetts Institute of Technology
Robert Croy, Massachusetts Institute of Technology
Deyu Li, Massachusetts Institute of Technology
Kyungsuk Yum, Massachusetts Institute of Technology
Jin-Ho Ahn, Massachusetts Institute of Technology
Hong Jin, Massachusettes Institute of Technology
John Essigmann, Massachusetts Institute of Technology
Daniel Blankschtein, Massachusetts Institute of Technology
Michael Strano, Massachusetts Institute of Technology



Molecular recognition is central to the design of therapeutics, chemical catalysis and sensor platforms, with the most common mechanisms involving biological structures such as antibodies1 and aptamers2,3.  The key to this molecular recognition is a folded and constrained heteropolymer pinned, via intra-molecular forces, into a unique three-dimensional orientation that creates a binding pocket or interface to recognize a specific molecule.  An alternate approach to constraining a polymer in three-dimensional space involves adsorbing it onto a cylindrical nanotube surface4-7.  To date, however, the molecular recognition potential of these structured, nanotube-associated complexes has been unexplored.  In this work, we demonstrate three distinct examples in which synthetic polymers enable unique and highly selective molecular recognition once adsorbed onto a single-walled carbon nanotube (SWCNT) surface.  The phenomenon is shown to be generic, with new recognition complexes demonstrated for riboflavin, l-thyroxine, and estradiol, predicted using a 2D thermodynamic model of surface interactions.  The dissociation constants are continuously tunable by perturbing the chemical structure of the heteropolymer. The sensing mechanism is confirmed by simultaneous dual-channel single-molecule imaging of the SWCNT and the heteropolymer. The complexes can be used as new types of sensors based on modulation of SWCNT photoemission, as demonstrated using a complex for real time spatio-temporal detection of riboflavin in murine macrophages. 

References

 

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2          Ellington, A. D. & Szostak, J. W. In vitro selection of RNA molecules that bind specific ligands. Nature 346, 818-822 (1990).

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4          Nish, A., Hwang, J., Doig, J. & Nicholas, R. Highly selective dispersion of single-walled carbon nanotubes using aromatic polymers. Nature Nanotechnology 2, 640-646 (2007).

5          Tsyboulski, D. et al. Self-Assembling Peptide Coatings Designed for Highly Luminescent Suspension of Single-Walled Carbon Nanotubes. J. Am. Chem. Soc 130, 17134-17140 (2008).

6          Zheng, M. et al. DNA-assisted dispersion and separation of carbon nanotubes. Nature Materials 2, 338-342 (2003).

7          Tu, X., Manohar, S., Jagota, A. & Zheng, M. DNA sequence motifs for structure-specific recognition and separation of carbon nanotubes. Nature 460, 250-253 (2009).