Co-assembly of liposomes, Dendrimersomes, and Polymersomes with amphiphilic Janus dendrimers conjugated to Mono- and Tris-Nitrilotriacetic Acid (NTA, TrisNTA) enhances protein recruitment

Xiao, Qi; Rivera-Martinez, Naomi; Raab, Calvin J.; Bermudez, Jessica G.; Good, Matthew C.; Klein, Michael L.; Percec, Virgil

doi:10.1016/j.giant.2021.100089

Title: Co-assembly of liposomes, Dendrimersomes, and Polymersomes with amphiphilic Janus dendrimers conjugated to Mono- and Tris-Nitrilotriacetic Acid (NTA, TrisNTA) enhances protein recruitment

Journal Article · 24 December 2021 · Giant

DOI: https://doi.org/10.1016/j.giant.2021.100089 · OSTI ID:1991570

Xiao, Qi ^[1]; Rivera-Martinez, Naomi ^[2]; Raab, Calvin J. ^[2]; Bermudez, Jessica G. ^[2]; Good, Matthew C. ^[2]; Klein, Michael L. ^[3]; Percec, Virgil ^[2]

Univ. of Pennsylvania, Philadelphia, PA (United States); Temple Univ., Philadelphia, PA (United States)
Univ. of Pennsylvania, Philadelphia, PA (United States)
Temple Univ., Philadelphia, PA (United States)

Metal-chelating ligands such as nitrilotriacetic acid (NTA) bind to polyhistidine-tagged (His-tagged) proteins. Lipids conjugated to NTA are widely used to decorate the surface of liposomes with proteins in cell biology applications. Multivalent NTA ligands such as tris-nitrilotriacetic acid (TrisNTA) display higher affinities than the monovalent NTA when co-assembled with phospholipids and cholesterol in liposomes. However, there is a limited number of available lipids conjugated to NTA and only few are commercially available. Additionally, their activity diminishes during storage or upon exposure to air. Here we report a library of five amphiphilic Janus dendrimers conjugated to NTA (JD-NTA) and three to TrisNTA (JD-TrisNTA). Both JD-NTA and JD-TrisNTA are indefinitely stable at room temperature in air and preliminary results demonstrate that they co-assemble with phospholipids and cholesterol into liposomes, with Janus dendrimers into dendrimersomes, and with block copolymers into polymersomes. The resulting hybrid liposomes co-assembled with JD-NTA display up to thirty-fold higher activity towards His-tagged fluorescent proteins when compared to lipid-NTAs. Hybrid liposomes co-assembled with JD-TrisNTA exhibit even higher binding affinity to His-tagged proteins and can function at much lower ligand concentration in hybrid liposomes than those containing JD-NTA. These preliminary results demonstrate the power of modular synthesis of JD-NTA or JD-TrisNTA to provide highly efficient new tools for biological reconstitution and synthetic cell biology as well as for nanomedicine.

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Research Organization:: Univ. of Pennsylvania, Philadelphia, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0007063; DMR-2104554; DMR-1807127; DMR-1720530

OSTI ID:: 1991570

Journal Information:: Giant, Vol. 9; ISSN 2666-5425

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Poly(Oxazoline)s with Tapered Minidendritic Side Groups as Models for the Design of Synthetic Macromolecules with Tertiary Structure. A Demonstration of the Limitations of Living Polymerization in the Design of 3-D Structures Based on Single Polymer Chains Percec, Virgil; Holerca, Marian N.; Uchida, Satoshi Biomacromolecules, Vol. 2, Issue 3 https://doi.org/10.1021/bm015559l	journal	August 2001
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Spherical Supramolecular Minidendrimers Self-Organized in an “Inverse Micellar”-like Thermotropic Body-Centered Cubic Liquid Crystalline Phase Yeardley, Duncan J. P.; Ungar, Goran; Percec, Virgil Journal of the American Chemical Society, Vol. 122, Issue 8 https://doi.org/10.1021/ja993915q	journal	March 2000
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Molecular Structure of Helical Supramolecular Dendrimers Peterca, Mihai; Percec, Virgil; Imam, Mohammad R. Journal of the American Chemical Society, Vol. 130, Issue 44 https://doi.org/10.1021/ja806524m	journal	October 2008
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Designing Libraries of First Generation AB ₃ and AB ₂ Self-Assembling Dendrons via the Primary Structure Generated from Combinations of (AB) _y −AB ₃ and (AB) _y −AB ₂ Building Blocks Percec, Virgil; Mitchell, Catherine M.; Cho, Wook-Dong Journal of the American Chemical Society, Vol. 126, Issue 19 https://doi.org/10.1021/ja049846j	journal	May 2004
Exploring and Expanding the Structural Diversity of Self-Assembling Dendrons through Combinations of AB, Constitutional Isomeric AB2, and AB3 Biphenyl-4-Methyl Ether Building Blocks Percec, Virgil; Holerca, Marian N.; Nummelin, Sami Chemistry - A European Journal, Vol. 12, Issue 24 https://doi.org/10.1002/chem.200600178	journal	August 2006
Expanding the Structural Diversity of Self-Assembling Dendrons and Supramolecular Dendrimers via Complex Building Blocks Percec, Virgil; Won, Betty C.; Peterca, Mihai Journal of the American Chemical Society, Vol. 129, Issue 36 https://doi.org/10.1021/ja073714j	journal	August 2007
Supramolecular Structural Diversity among First-Generation Hybrid Dendrimers and Twin Dendrons Percec, Virgil; Rudick, Jonathan G.; Peterca, Mihai Chemistry - A European Journal, Vol. 14, Issue 11 https://doi.org/10.1002/chem.200701658	journal	April 2008
Elucidating the Structure of the Pm $\bar 3$ n Cubic Phase of Supramolecular Dendrimers through the Modification of their Aliphatic to Aromatic Volume Ratio Percec, Virgil; Peterca, Mihai; Tsuda, Yusuke Chemistry - A European Journal, Vol. 15, Issue 36 https://doi.org/10.1002/chem.200901324	journal	September 2009
Hollow Spherical Supramolecular Dendrimers Percec, Virgil; Peterca, Mihai; Dulcey, Andrés E. Journal of the American Chemical Society, Vol. 130, Issue 39 https://doi.org/10.1021/ja8034703	journal	October 2008
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