TY - JOUR
T1 - Quantifying guest–host dynamics in supramolecular assemblies to analyze their robustness
AU - Bastings, Maartje M.C.
AU - Hermans, Thomas M.
AU - Spiering, A.J.H.
AU - Kemps, Erwin W.L.
AU - Albertazzi, Lorenzo
AU - Kurisinkal, Eva E.
AU - Dankers, Patricia Y.W.
PY - 2019/1/1
Y1 - 2019/1/1
N2 - The most basic function of synthetic microenvironments for tissue engineering is to act as a physical substrate for cell attachment, migration, and proliferation, similar to the natural cell environment. Functionalization of supramolecular materials with guest compounds that display the same recognition moieties is a common strategy to introduce biofunctionality. However, besides a robust interaction with the material, a certain level of dynamics needs to be conserved for an adaptive interface toward the living environment. A balance between robust material functionalization and dynamic cell interaction needs to be met. The detailed analysis hereof using a ureido-pyrimidinone (UPy) poly(ethylene glycol) system in dilute and transient network regime is demonstrated. Monovalent and bivalent UPy-functionalized guest molecules are designed and their interaction with UPy-host fibers is evaluated. Analysis of guest interaction in the dilute state by microfluidics, and in the gel state, by fluorescence recovery after photobleaching and fluorescence resonance energy transfer is proven to be suitable to quantify the local and ensemble guest mobility. The results demonstrate that the interaction of bioactive moieties through supramolecular host–guest chemistry yields a dynamic system, which is stronger for divalent guests but risks unintended leakage in the case of functional monomeric units.
AB - The most basic function of synthetic microenvironments for tissue engineering is to act as a physical substrate for cell attachment, migration, and proliferation, similar to the natural cell environment. Functionalization of supramolecular materials with guest compounds that display the same recognition moieties is a common strategy to introduce biofunctionality. However, besides a robust interaction with the material, a certain level of dynamics needs to be conserved for an adaptive interface toward the living environment. A balance between robust material functionalization and dynamic cell interaction needs to be met. The detailed analysis hereof using a ureido-pyrimidinone (UPy) poly(ethylene glycol) system in dilute and transient network regime is demonstrated. Monovalent and bivalent UPy-functionalized guest molecules are designed and their interaction with UPy-host fibers is evaluated. Analysis of guest interaction in the dilute state by microfluidics, and in the gel state, by fluorescence recovery after photobleaching and fluorescence resonance energy transfer is proven to be suitable to quantify the local and ensemble guest mobility. The results demonstrate that the interaction of bioactive moieties through supramolecular host–guest chemistry yields a dynamic system, which is stronger for divalent guests but risks unintended leakage in the case of functional monomeric units.
KW - Fluorescence Resonance Energy Transfer
KW - Polyethylene Glycols/chemistry
KW - Pyrimidinones/chemistry
KW - Tissue Engineering
UR - http://www.scopus.com/inward/record.url?scp=85057973820&partnerID=8YFLogxK
U2 - 10.1002/mabi.201800296
DO - 10.1002/mabi.201800296
M3 - Article
C2 - 30511809
AN - SCOPUS:85057973820
VL - 19
JO - Macromolecular Bioscience
JF - Macromolecular Bioscience
SN - 1616-5187
IS - 1
M1 - 1800296
ER -