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The Enzymatic Oxidation of GrapheneOxide Gregg P. Kotchey,† Brett L. Allen,† Harindra Vedala,† Naveena Yanamala,‡,§ Alexander A. Kapralov,‡Yulia Y. Tyurina,‡ Judith Klein-Seetharaman,§ Valerian E. Kagan,‡ and Alexander Star†,*†Department of Chemistry, ‡Department of Environmental and Occupational Health, and §Department of Structural Biology, University of Pittsburgh, Pittsburgh,Pennsylvania, 15260 ABSTRACT Two-dimensional graphitic carbon is a new material with many emerging applications, and studying its chemical properties is an important goal. Here, we reported a new phenomenon;the enzymatic oxidation of a single layer of graphitic carbon by horseradish peroxidase (HRP). In the presence of low concentrations of hydrogen peroxide (～40 μM), HRP catalyzed the oxidation of graphene oxide, which resulted in the formation of holes on its basal plane. During the same period of analysis, HRP failed to oxidize chemically reduced graphene oxide (RGO). The enzymatic oxidation was characterized by Raman, ultraviolet-visible, electron paramagneticresonance, Fourier transform infrared s pectroscopy, transmission electron microscopy, atomic force microscopy, sodium dodecyl sulfate-polyacrylamide gel electrophoresis, and gas chromatography-mass spectrometry. Computational docking studies indicated that HRP was preferentially bound to the basal plane rather than the edge for both graphene oxide and RGO. Owing to the more dynamic nature of HRP on graphene oxide, the heme active site of HRP was in closer proximity to graphene oxide compared to RGO, thereby facilitating the oxidation of the basal plane of graphene oxide. We also studied the electronic properties of the reduced intermediate product, holey reduced graphene oxide (hRGO), using field-effect transistor (FET) measurements. While RGO exhibited a V-shaped transfer characteristic similar to a single layer of graphene that was attributed to its zero band gap, hRGO demonstrated a p-type semiconducting behavior with a positive shift in the Dirac points. This p-type behavior rendered hRGO, which can be conceptualized as interconnected graphene nanoribbons, as a potentially attractive material for FET sensors. KEYWORDS: graphene . oxidation . microscopy . peroxidase . field-effect transistor |
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作者名字没翻译，这东西没什么翻译的。重点是标题及摘要 The Enzymatic Oxidation of GrapheneOxide 石墨烯氧化物的酶促氧化 Department of Chemistry, ‡Department of Environmental and Occupational Health, and §Department of Structural Biology, University of Pittsburgh, Pittsburgh,Pennsylvania, 15260 匹兹堡大学，结构生物学部及环境和职业健康部，化学系 宾夕法尼亚州匹兹堡 15260 ABSTRACT 摘要 Two-dimensional graphitic carbon is a new material with many emerging applications, and studying its chemical properties is an important goal. 二维石墨碳是一种具有很多工业应用的新材料。研究其化学性质目标重大。 Here, we reported a new phenomenon;the enzymatic oxidation of a single layer of graphitic carbon by horseradish peroxidase (HRP). 本文报道了一种新新现象，即经辣根过氧化物酶HRP作用使，单层石墨碳的酶促氧化。 In the presence of low concentrations of hydrogen peroxide (～40 μM), HRP catalyzed the oxidation of graphene oxide, which resulted in the formation of holes on its basal plane. 当过氧化氢浓度低时 (～40 μM)，, HRP催化石墨烯氧化物的氧化，从而导致其底面空洞的形成。 During the same period of analysis, HRP failed to oxidize chemically reduced graphene oxide (RGO). 同一时期的分析表明， HRP不能氧化化学还原性石墨烯氧化物 (RGO) The enzymatic oxidation was characterized by Raman, ultraviolet-visible, electron paramagneticresonance, Fourier transform infrared s pectroscopy, transmission electron microscopy, atomic force microscopy, sodium dodecyl sulfate-polyacrylamide gel electrophoresis, and gas chromatography-mass spectrometry. 用拉曼，紫外可见吸收，电子顺磁共振，傅里叶变换红外光谱，透射电子显微镜法，原子力显微镜，聚丙烯酰胺凝胶电泳以及气相色谱-质谱来表征酶催氧化。 Computational docking studies indicated that HRP was preferentially bound to the basal plane rather than the edge for both graphene oxide and RGO. 计算对接研究表明，HRP优先绑定到石墨烯氧化物及RGO两者的底面，而不是边缘。 Owing to the more dynamic nature of HRP on graphene oxide, the heme active site of HRP was in closer proximity to graphene oxide compared to RGO, thereby facilitating the oxidation of the basal plane of graphene oxide. 由于石墨烯氧化物上有更多地动态特性，与RGO相比， HRP的血红素活性部位更接近于石墨烯氧化物。 We also studied the electronic properties of the reduced intermediate product, holey reduced graphene oxide (hRGO), using field-effect transistor (FET) measurements. 用过使用场效应晶体管测量，本文还研究了还原中间产物及多孔RGO的电子特性。 While RGO exhibited a V-shaped transfer characteristic similar to a single layer of graphene that was attributed to its zero band gap, hRGO demonstrated a p-type semiconducting behavior with a positive shift in the Dirac points. RGO呈现出与单层的石墨烯相似的V形传热性能，这是由于其零带隙，致使hRGO因在狄拉克点的正向位移而表现出p型半导体行为。 This p-type behavior rendered hRGO, which can be conceptualized as interconnected graphene nanoribbons, as a potentially attractive material for FET sensors. 这种p型行为显示出 hRGO 可以概念化为互相连接石墨烯纳米带，一种制作TET感应器的潜在的有吸引力的材料。 |
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