TY - JOUR
T1 - Stimuli-responsive degrafting of polymer brushes via addressable catecholato-metal attachments
AU - Agergaard, Asger Holm
AU - Pedersen, Steen Uttrup
AU - Birkedal, Henrik
AU - Daasbjerg, Kim
PY - 2020/9/21
Y1 - 2020/9/21
N2 - Catecholato-metal complexes are widely used in functional materials such as hydrogels, where the dynamic nature of the coordination bonds between catechol and metal ions contributes to self-healing and stimuli-responsive properties. Herein, we translate the pH-controlled speciation of such complexes known from bulk to a surface counterpart. We create catecholato-metal attachments by electrografting catechol to glassy carbon surfaces, enabling binding of Al3+ or Fe3+ and, subsequently, dopamine. When binding dopamine, pH determines whether bis- or tris-catecholato-metal species dominate. Polymer brushes of poly(methyl methacrylate) are grown from these attachments and subsequently detached by electro-oxidation of the catechol, causing the catecholato-metal complex to disintegrate. This study shows that the catecholato-metal complex retains its pH- and oxidation-responsive properties when confined to the surface, and that catechol-based polymer brush interfaces constitute a versatile approach toward on-demand renewal of smart surfaces.
AB - Catecholato-metal complexes are widely used in functional materials such as hydrogels, where the dynamic nature of the coordination bonds between catechol and metal ions contributes to self-healing and stimuli-responsive properties. Herein, we translate the pH-controlled speciation of such complexes known from bulk to a surface counterpart. We create catecholato-metal attachments by electrografting catechol to glassy carbon surfaces, enabling binding of Al3+ or Fe3+ and, subsequently, dopamine. When binding dopamine, pH determines whether bis- or tris-catecholato-metal species dominate. Polymer brushes of poly(methyl methacrylate) are grown from these attachments and subsequently detached by electro-oxidation of the catechol, causing the catecholato-metal complex to disintegrate. This study shows that the catecholato-metal complex retains its pH- and oxidation-responsive properties when confined to the surface, and that catechol-based polymer brush interfaces constitute a versatile approach toward on-demand renewal of smart surfaces.
UR - http://www.scopus.com/inward/record.url?scp=85092371434&partnerID=8YFLogxK
U2 - 10.1039/D0PY00916D
DO - 10.1039/D0PY00916D
M3 - Journal article
SN - 1759-9954
VL - 11
SP - 5572
EP - 5577
JO - Polymer Chemistry
JF - Polymer Chemistry
IS - 35
ER -