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Imidazole‐Grafted Nanogels for the Fabrication of Organic–Inorganic Protein Hybrids
Author(s) -
RodriguezAbetxuko Andoni,
MorantMiñana Maria Carmen,
LópezGallego Fernando,
Yate Luis,
Seifert Andreas,
Knez Mato,
Beloqui Ana
Publication year - 2018
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.201803115
Subject(s) - imidazole , biomineralization , materials science , mineralization (soil science) , thermal stability , hybrid material , chemical engineering , polymer chemistry , combinatorial chemistry , organic chemistry , chemistry , nanotechnology , nitrogen , engineering
Here, a platform for the development of highly responsive organic–inorganic enzyme hybrids is provided. The approach entails a first step of protein engineering, in which individual enzymes are armored with a porous nanogel decorated with imidazole motifs. In a second step, by mimicking the biomineralization mechanism, the assembly of the imidazole nanogels with CuSO 4 and phosphate salts is triggered. A full characterization of the new composites reveals the first reported example in which the assembly mechanism is triggered by the sum of Cu(II)–imidazole interaction and Cu 3 (PO 4 ) 2 inorganic salt formation. It is demonstrated that the organic component of the hybrids, namely the imidazole‐modified polyacrylamide hydrogel, provides a favorable spatial distribution for the enzyme. This results in enhanced conversion rates, robustness of the composite at low pH values, and a remarkable thermal stability at 65 °C, exhibiting 400% of the activity of the mineralized enzyme lacking the organic constituent. Importantly, unlike in previous works, the protocol applies to the use of a broad range of transition metal cations (including mono‐, di‐, and trivalent cations) to trigger the mineralization mechanism, which eventually broadens the chemical and structural diversity of organic–inorganic protein hybrids.