期刊
ADVANCED FUNCTIONAL MATERIALS
卷 28, 期 35, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201803115
关键词
biomineralization; nanobiohybrids; nanoflowers; protein stabilization; single enzyme nanogels
类别
资金
- Spanish Ministry of Economy and Competitiveness (MINECO)
- FEDER [MAT2017-88808-R]
- Maria de Maeztu Units of Excellence Programme [MDM-2016-0618]
- Diputacion de Guipuzcoa
- Spanish Ministry of Economy and Competitiveness (MINECO) [MAT2016-77393-R]
- FEDER funds
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 CuSO4 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(PO4)(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 degrees 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.
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