4.6 Article

Hybridization of Particulate Methane Monooxygenase by Methanobactin-Modified AuNPs

Journal

MOLECULES
Volume 24, Issue 22, Pages -

Publisher

MDPI
DOI: 10.3390/molecules24224027

Keywords

AuNPs; nanobiohybrids; electron donor; hydroquinone; methanobactin; particulate methane monooxygenase

Funding

  1. National Natural Science Foundation of China [21573055]
  2. Harbin University of Commerce [YJSCX2018-481HSD]
  3. state key laboratory for oxosynthesis and selective oxidation

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Particulate methane monooxygenase (pMMO) is a characteristic membrane-bound metalloenzyme of methane-oxidizing bacteria that can catalyze the bioconversion of methane to methanol. However, in order to achieve pMMO-based continuous methane-to-methanol bioconversion, the problems of reducing power in vitro regeneration and pMMO stability need to be overcome. Methanobactin (Mb) is a small copper-chelating molecule that functions not only as electron carrier for pMMO catalysis and pMMO protector against oxygen radicals, but also as an agent for copper acquisition and uptake. In order to improve the activity and stability of pMMO, methanobactin-Cu (Mb-Cu)-modified gold nanoparticle (AuNP)-pMMO nanobiohybrids were straightforwardly synthesized via in situ reduction of HAuCl4 to AuNPs in a membrane fraction before further association with Mb-Cu. Mb-Cu modification can greatly improve the activity and stability of pMMO in the AuNP-pMMO nanobiohybrids. It is shown that the Mb-Cu-modified AuNP-pMMO nanobiohybrids can persistently catalyze the conversion of methane to methanol with hydroquinone as electron donor. The artificial heterogeneous nanobiohybrids exhibited excellent reusability and reproducibility in three cycles of catalysis, and they provide a model for achieving hydroquinone-driven conversion of methane to methanol.

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