Integration of molecular and enzymatic catalysts on graphene for biomimetic generation of antithrombotic species

Teng Xue; Bo Peng; Min Xue; Xing Zhong; Chin-Yi Chiu; Si Yang; Yongquan Qu; Lingyan Ruan; Shan Jiang; Sergey Dubin; Richard B Kaner; Jeffrey I Zink; Mark E Meyerhoff; Xiangfeng Duan; Yu Huang

doi:10.1038/ncomms4200

Integration of molecular and enzymatic catalysts on graphene for biomimetic generation of antithrombotic species

Nat Commun. 2014:5:3200. doi: 10.1038/ncomms4200.

Authors

Teng Xue¹, Bo Peng², Min Xue³, Xing Zhong³, Chin-Yi Chiu⁴, Si Yang⁵, Yongquan Qu³, Lingyan Ruan⁴, Shan Jiang³, Sergey Dubin³, Richard B Kaner⁶, Jeffrey I Zink⁷, Mark E Meyerhoff⁵, Xiangfeng Duan⁷, Yu Huang⁸

Affiliations

¹ 1] Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, USA [2].
² 1] Department of Chemistry, The University of Michigan, 930 N. University, Ann Arbor, Michigan 48109, USA [2].
³ Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA.
⁴ Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, USA.
⁵ Department of Chemistry, The University of Michigan, 930 N. University, Ann Arbor, Michigan 48109, USA.
⁶ 1] Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, USA [2] Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA [3] California NanoSystems Institute, University of California, Los Angeles, California 90095, USA.
⁷ 1] Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA [2] California NanoSystems Institute, University of California, Los Angeles, California 90095, USA.
⁸ 1] Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, USA [2] California NanoSystems Institute, University of California, Los Angeles, California 90095, USA.

Abstract

The integration of multiple synergistic catalytic systems can enable the creation of biocompatible enzymatic mimics for cascading reactions under physiologically relevant conditions. Here we report the design of a graphene-haemin-glucose oxidase conjugate as a tandem catalyst, in which graphene functions as a unique support to integrate molecular catalyst haemin and enzymatic catalyst glucose oxidase for biomimetic generation of antithrombotic species. Monomeric haemin can be conjugated with graphene through π-π interactions to function as an effective catalyst for the oxidation of endogenous L-arginine by hydrogen peroxide. Furthermore, glucose oxidase can be covalently linked onto graphene for local generation of hydrogen peroxide through the oxidation of blood glucose. Thus, the integrated graphene-haemin-glucose oxidase catalysts can readily enable the continuous generation of nitroxyl, an antithrombotic species, from physiologically abundant glucose and L-arginine. Finally, we demonstrate that the conjugates can be embedded within polyurethane to create a long-lasting antithrombotic coating for blood-contacting biomedical devices.

Publication types

Research Support, N.I.H., Extramural

MeSH terms

Arginine / metabolism*
Aspergillus niger / enzymology*
Biomimetic Materials
Catalysis
Fibrinolytic Agents / metabolism*
Fungal Proteins / chemistry
Fungal Proteins / metabolism*
Glucose / metabolism*
Glucose Oxidase / chemistry
Glucose Oxidase / metabolism*
Graphite / chemistry
Hemin / chemistry
Hydrogen Peroxide
Nitrogen Oxides / metabolism*

Substances

Fibrinolytic Agents
Fungal Proteins
Nitrogen Oxides
Hemin
Graphite
Arginine
Hydrogen Peroxide
Glucose Oxidase
nitroxyl
Glucose

Abstract

Publication types

MeSH terms

Substances

Grants and funding