The enzymatic oxidation of graphene oxide.
The enzymatic oxidation of graphene oxide.
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DOI：
10.1021/nn103265h
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发表时间：
2011-03-22
期刊：
影响因子：
17.1
通讯作者：
Star A
中科院分区：
文献类型：
--
作者：
Kotchey GP;Allen BL;Vedala H;Yanamala N;Kapralov AA;Tyurina YY;Klein-Seetharaman J;Kagan VE;Star A
二维石墨碳是一种具有许多新兴应用的新材料，研究其化学性质是一个重要的目标。在这里，我们报告了一个新的现象-辣根过氧化物酶（HRP）的单层石墨碳的酶促氧化。在低浓度过氧化氢（~40 µM）的存在下，HRP催化氧化石墨烯的氧化，导致其底面形成孔洞。在相同的分析期间，HRP未能氧化化学还原的氧化石墨烯（RGO）。通过拉曼、紫外-可见光谱、EPR和FT-IR光谱、TEM、AFM、SDS-PAGE和GC-MS表征酶促氧化。计算对接研究表明，对于氧化石墨烯和RGO，HRP优先结合到基面而不是边缘。由于HRP在氧化石墨烯上的更动态的性质，HRP的血红素活性位点与RGO相比更接近氧化石墨烯，从而促进氧化石墨烯的基面的氧化。我们还研究了减少的中间产物，多孔还原氧化石墨烯（hRGO）的电子性质，使用场效应晶体管（FET）测量。虽然RGO表现出类似于单层石墨烯的V形传输特性，这归因于其零带隙，但hRGO表现出p型半导体行为，狄拉克点正移。这种p型行为使得hRGO（其可以被概念化为互连的石墨烯纳米带）成为FET传感器的潜在有吸引力的材料。
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, UV-Vis, EPR and FT-IR spectroscopy, TEM, AFM, SDS-PAGE, and GC-MS. Computational docking studies indicated that HRP was preferentially bound to the basal plane rather than the edge for both graphene oxide and RGO. Due 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.
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