Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes

Jingqing Zhang; Markita P. Landry; Paul W. Barone; Jong Ho Kim; Shangchao Lin; Zachary W. Ulissi; Dahua Lin; Bin Mu; Ardemis A. Boghossian; Andrew J. Hilmer; Alina Rwei; Allison C. Hinckley; Sebastian Kruss; Mia A. Shandell; Nitish Nair; Steven Blake; Fatih Şen; Selda Şen; Robert G. Croy; Deyu Li; Kyungsuk Yum; Jin Ho Ahn; Hong Jin; Daniel A. Heller; John M. Essigmann; Daniel Blankschtein; Michael S. Strano

doi:10.1038/nnano.2013.236

Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes

Jingqing Zhang, Markita P. Landry, Paul W. Barone, Jong Ho Kim, Shangchao Lin, Zachary W. Ulissi, Dahua Lin, Bin Mu, Ardemis A. Boghossian, Andrew J. Hilmer, Alina Rwei, Allison C. Hinckley, Sebastian Kruss, Mia A. Shandell, Nitish Nair, Steven Blake, Fatih Şen, Selda Şen, Robert G. Croy, Deyu LiKyungsuk Yum, Jin Ho Ahn, Hong Jin, Daniel A. Heller, John M. Essigmann, Daniel Blankschtein, Michael S. Strano^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

Abstract

Understanding molecular recognition is of fundamental importance in applications such as therapeutics, chemical catalysis and sensor design. The most common recognition motifs involve biological macromolecules such as antibodies and aptamers. The key to biorecognition consists of a unique three-dimensional structure formed by a folded and constrained bioheteropolymer that creates a binding pocket, or an interface, able to recognize a specific molecule. Here, we show that synthetic heteropolymers, once constrained onto a single-walled carbon nanotube by chemical adsorption, also form a new corona phase that exhibits highly selective recognition for specific molecules. To prove the generality of this phenomenon, we report three examples of heteropolymer-nanotube recognition complexes for riboflavin, L-thyroxine and oestradiol. In each case, the recognition was predicted using a two-dimensional thermodynamic model of surface interactions in which the dissociation constants can be tuned by perturbing the chemical structure of the heteropolymer. Moreover, these complexes can be used as new types of spatiotemporal sensors based on modulation of the carbon nanotube photoemission in the near-infrared, as we show by tracking riboflavin diffusion in murine macrophages.

Original language	English
Pages (from-to)	959-968
Number of pages	10
Journal	Nature Nanotechnology
Volume	8
Issue number	12
DOIs	https://doi.org/10.1038/nnano.2013.236
Publication status	Published - Dec 2013

Bibliographical note

Funding Information:
The authors thank L. Trudel for her assistance with cell culture. The authors thank D. Wittrup, C. Love and V. Sresht for discussions. This work made use of the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation (grant no. OCI-1053575). M.S.S. acknowledges a grant from the Army Research Office and support via award no. 64655-CH-ISN to the Institute for Solider Nanotechnologies. D.A.H. acknowledges the Damon Runyon Cancer Research Foundation. A.A.B. is funded by the National Defense Science & Engineering Graduate Fellowship. A.J.H. acknowledges funding from the Department of Energy SCGF programme (contract no. DE-AC05-06OR23100). Z.W.U. acknowledges support from the Department of Energy CSGF (DOE grant DE-FG02-97ER25308). M.P.L. acknowledges an NSF postdoctoral research fellowship (award no. DBI-1306229). S.K. was supported by a fellowship from the Deutsche Forschungsmeinschaft (DFG).

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Zhang, J., Landry, M. P., Barone, P. W., Kim, J. H., Lin, S., Ulissi, Z. W., Lin, D., Mu, B., Boghossian, A. A., Hilmer, A. J., Rwei, A., Hinckley, A. C., Kruss, S., Shandell, M. A., Nair, N., Blake, S., Şen, F., Şen, S., Croy, R. G., ... Strano, M. S. (2013). Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes. Nature Nanotechnology, 8(12), 959-968. https://doi.org/10.1038/nnano.2013.236

@article{413be957137042bc9b845f969b0e4e3d,

title = "Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes",

abstract = "Understanding molecular recognition is of fundamental importance in applications such as therapeutics, chemical catalysis and sensor design. The most common recognition motifs involve biological macromolecules such as antibodies and aptamers. The key to biorecognition consists of a unique three-dimensional structure formed by a folded and constrained bioheteropolymer that creates a binding pocket, or an interface, able to recognize a specific molecule. Here, we show that synthetic heteropolymers, once constrained onto a single-walled carbon nanotube by chemical adsorption, also form a new corona phase that exhibits highly selective recognition for specific molecules. To prove the generality of this phenomenon, we report three examples of heteropolymer-nanotube recognition complexes for riboflavin, L-thyroxine and oestradiol. In each case, the recognition was predicted using a two-dimensional thermodynamic model of surface interactions in which the dissociation constants can be tuned by perturbing the chemical structure of the heteropolymer. Moreover, these complexes can be used as new types of spatiotemporal sensors based on modulation of the carbon nanotube photoemission in the near-infrared, as we show by tracking riboflavin diffusion in murine macrophages.",

author = "Jingqing Zhang and Landry, {Markita P.} and Barone, {Paul W.} and Kim, {Jong Ho} and Shangchao Lin and Ulissi, {Zachary W.} and Dahua Lin and Bin Mu and Boghossian, {Ardemis A.} and Hilmer, {Andrew J.} and Alina Rwei and Hinckley, {Allison C.} and Sebastian Kruss and Shandell, {Mia A.} and Nitish Nair and Steven Blake and Fatih {\c S}en and Selda {\c S}en and Croy, {Robert G.} and Deyu Li and Kyungsuk Yum and Ahn, {Jin Ho} and Hong Jin and Heller, {Daniel A.} and Essigmann, {John M.} and Daniel Blankschtein and Strano, {Michael S.}",

note = "Funding Information: The authors thank L. Trudel for her assistance with cell culture. The authors thank D. Wittrup, C. Love and V. Sresht for discussions. This work made use of the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation (grant no. OCI-1053575). M.S.S. acknowledges a grant from the Army Research Office and support via award no. 64655-CH-ISN to the Institute for Solider Nanotechnologies. D.A.H. acknowledges the Damon Runyon Cancer Research Foundation. A.A.B. is funded by the National Defense Science & Engineering Graduate Fellowship. A.J.H. acknowledges funding from the Department of Energy SCGF programme (contract no. DE-AC05-06OR23100). Z.W.U. acknowledges support from the Department of Energy CSGF (DOE grant DE-FG02-97ER25308). M.P.L. acknowledges an NSF postdoctoral research fellowship (award no. DBI-1306229). S.K. was supported by a fellowship from the Deutsche Forschungsmeinschaft (DFG).",

year = "2013",

month = dec,

doi = "10.1038/nnano.2013.236",

language = "English",

volume = "8",

pages = "959--968",

journal = "Nature Nanotechnology",

issn = "1748-3387",

publisher = "Nature Publishing Group",

number = "12",

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Zhang, J, Landry, MP, Barone, PW, Kim, JH, Lin, S, Ulissi, ZW, Lin, D, Mu, B, Boghossian, AA, Hilmer, AJ, Rwei, A, Hinckley, AC, Kruss, S, Shandell, MA, Nair, N, Blake, S, Şen, F, Şen, S, Croy, RG, Li, D, Yum, K, Ahn, JH, Jin, H, Heller, DA, Essigmann, JM, Blankschtein, D & Strano, MS 2013, 'Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes', Nature Nanotechnology, vol. 8, no. 12, pp. 959-968. https://doi.org/10.1038/nnano.2013.236

TY - JOUR

T1 - Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes

AU - Zhang, Jingqing

AU - Landry, Markita P.

AU - Barone, Paul W.

AU - Kim, Jong Ho

AU - Lin, Shangchao

AU - Ulissi, Zachary W.

AU - Lin, Dahua

AU - Mu, Bin

AU - Boghossian, Ardemis A.

AU - Hilmer, Andrew J.

AU - Rwei, Alina

AU - Hinckley, Allison C.

AU - Kruss, Sebastian

AU - Shandell, Mia A.

AU - Nair, Nitish

AU - Blake, Steven

AU - Şen, Fatih

AU - Şen, Selda

AU - Croy, Robert G.

AU - Li, Deyu

AU - Yum, Kyungsuk

AU - Ahn, Jin Ho

AU - Jin, Hong

AU - Heller, Daniel A.

AU - Essigmann, John M.

AU - Blankschtein, Daniel

AU - Strano, Michael S.

N1 - Funding Information: The authors thank L. Trudel for her assistance with cell culture. The authors thank D. Wittrup, C. Love and V. Sresht for discussions. This work made use of the Extreme Science and Engineering Discovery Environment (XSEDE), which is supported by National Science Foundation (grant no. OCI-1053575). M.S.S. acknowledges a grant from the Army Research Office and support via award no. 64655-CH-ISN to the Institute for Solider Nanotechnologies. D.A.H. acknowledges the Damon Runyon Cancer Research Foundation. A.A.B. is funded by the National Defense Science & Engineering Graduate Fellowship. A.J.H. acknowledges funding from the Department of Energy SCGF programme (contract no. DE-AC05-06OR23100). Z.W.U. acknowledges support from the Department of Energy CSGF (DOE grant DE-FG02-97ER25308). M.P.L. acknowledges an NSF postdoctoral research fellowship (award no. DBI-1306229). S.K. was supported by a fellowship from the Deutsche Forschungsmeinschaft (DFG).

PY - 2013/12

Y1 - 2013/12

N2 - Understanding molecular recognition is of fundamental importance in applications such as therapeutics, chemical catalysis and sensor design. The most common recognition motifs involve biological macromolecules such as antibodies and aptamers. The key to biorecognition consists of a unique three-dimensional structure formed by a folded and constrained bioheteropolymer that creates a binding pocket, or an interface, able to recognize a specific molecule. Here, we show that synthetic heteropolymers, once constrained onto a single-walled carbon nanotube by chemical adsorption, also form a new corona phase that exhibits highly selective recognition for specific molecules. To prove the generality of this phenomenon, we report three examples of heteropolymer-nanotube recognition complexes for riboflavin, L-thyroxine and oestradiol. In each case, the recognition was predicted using a two-dimensional thermodynamic model of surface interactions in which the dissociation constants can be tuned by perturbing the chemical structure of the heteropolymer. Moreover, these complexes can be used as new types of spatiotemporal sensors based on modulation of the carbon nanotube photoemission in the near-infrared, as we show by tracking riboflavin diffusion in murine macrophages.

AB - Understanding molecular recognition is of fundamental importance in applications such as therapeutics, chemical catalysis and sensor design. The most common recognition motifs involve biological macromolecules such as antibodies and aptamers. The key to biorecognition consists of a unique three-dimensional structure formed by a folded and constrained bioheteropolymer that creates a binding pocket, or an interface, able to recognize a specific molecule. Here, we show that synthetic heteropolymers, once constrained onto a single-walled carbon nanotube by chemical adsorption, also form a new corona phase that exhibits highly selective recognition for specific molecules. To prove the generality of this phenomenon, we report three examples of heteropolymer-nanotube recognition complexes for riboflavin, L-thyroxine and oestradiol. In each case, the recognition was predicted using a two-dimensional thermodynamic model of surface interactions in which the dissociation constants can be tuned by perturbing the chemical structure of the heteropolymer. Moreover, these complexes can be used as new types of spatiotemporal sensors based on modulation of the carbon nanotube photoemission in the near-infrared, as we show by tracking riboflavin diffusion in murine macrophages.

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U2 - 10.1038/nnano.2013.236

DO - 10.1038/nnano.2013.236

M3 - Article

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AN - SCOPUS:84890446448

SN - 1748-3387

VL - 8

SP - 959

EP - 968

JO - Nature Nanotechnology

JF - Nature Nanotechnology

IS - 12

ER -

Molecular recognition using corona phase complexes made of synthetic polymers adsorbed on carbon nanotubes

Abstract

Bibliographical note

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