title: Integration of molecular and enzymatic catalysts on graphene for biomimetic generation of antithrombotic species.
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.
authors: 1] Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, USA [2].
authors: Teng
authors: T
authors: Xue
authors: 1] Department of Chemistry, The University of Michigan, 930 N. University, Ann Arbor, Michigan 48109, USA [2].
authors: Bo
authors: B
authors: Peng
authors: Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA.
authors: Min
authors: M
authors: Xue
authors: Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA.
authors: Xing
authors: X
authors: Zhong
authors: Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, USA.
authors: Chin-Yi
authors: CY
authors: Chiu
authors: Department of Chemistry, The University of Michigan, 930 N. University, Ann Arbor, Michigan 48109, USA.
authors: Si
authors: S
authors: Yang
authors: Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA.
authors: Yongquan
authors: Y
authors: Qu
authors: Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, USA.
authors: Lingyan
authors: L
authors: Ruan
authors: Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA.
authors: Shan
authors: S
authors: Jiang
authors: Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, USA.
authors: Sergey
authors: S
authors: Dubin
authors: 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.
authors: Richard B
authors: RB
authors: Kaner
authors: 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.
authors: Jeffrey I
authors: JI
authors: Zink
authors: Department of Chemistry, The University of Michigan, 930 N. University, Ann Arbor, Michigan 48109, USA.
authors: Mark E
authors: ME
authors: Meyerhoff
authors: 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.
authors: Xiangfeng
authors: X
authors: Duan
authors: 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.
authors: Yu
authors: Y
authors: Huang
mesh_terms: D001120:Arginine / Q000378:metabolism*; D001234:Aspergillus niger / Q000201:enzymology*; D040761:Biomimetic Materials; D002384:Catalysis; D005343:Fibrinolytic Agents / Q000378:metabolism*; D005656:Fungal Proteins / Q000737:chemistry / Q000378:metabolism*; D005947:Glucose / Q000378:metabolism*; D005949:Glucose Oxidase / Q000737:chemistry / Q000378:metabolism*; D006108:Graphite / Q000737:chemistry; D006427:Hemin / Q000737:chemistry; D006861:Hydrogen Peroxide; D009589:Nitrogen Oxides / Q000378:metabolism*
chemical_list: D005343:Fibrinolytic Agents; D005656:Fungal Proteins; D009589:Nitrogen Oxides; D006427:Hemin; D006108:Graphite; D001120:Arginine; D006861:Hydrogen Peroxide; D005949:Glucose Oxidase; C039900:nitroxyl; D005947:Glucose