Graphdiyne (GDY) is recently synthesized two-dimensional carbon allotrope with hexagonal rings cross-linked by diacetylene through introducing butadiyne linkages (−C≡C–C≡C−) to form 18-C hexagons and is emerging to be fundamentally interesting and particularly useful in various research fields. In this study, we for the first time find that GDY can be used as an electrode material with reactivity tunable by electronic states and surface chemistry of GDY. To demonstrate this, GDY is oxidized into graphdiyne oxide (GDYO) that is then chemically and electrochemically reduced into chemically reduced GDYO (cr-GDYO) and electrochemically reduced GDYO (er-GDYO), respectively. Electrode reactivity of GDY and its derivatives (i.e., GDYO, cr-GDYO, and er-GDYO) is studied with hexaammineruthenium chloride ([Ru(NH₃)₆]Cl₃) and potassium ferricyanide (K₃Fe(CN)₆) as redox probes. We find that electron transfer kinetics of the redox probes employed here at GDYs depends on the density of electronic state (DOS) and the synergetic effects of the surface chemistry as well as the hydrophilicity of the materials, and that the electron transfer kinetics at cr-GDYO and er-GDYO are faster than those at GDY and GDYO, and quite comparable with those at carbon nanotubes and graphene and its derivatives (i.e., GO, cr-GO, and er-GO). These properties, combined with the unique electronic and chemical structures of GDY, essentially enable GDY as a new kind of electrode material for fundamental studies on carbon electrochemistry and various electroanalytical applications.

中文翻译：

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Graphdiyne作为电极材料：调整电子状态和表面化学以改善电极反应性

石墨二炔（Graphyyne（GDY））是最近合成的二维碳同素异形体，具有通过引入丁二炔键（-C≡C-C≡C-）形成18-C六边形的二乙炔交联的六角环。在各种研究领域中很有用。在本研究中，我们首次发现GDY可用作具有可通过GDY的电子态和表面化学性质进行调节的反应性的电极材料。为了证明这一点，将GDY氧化为氧化石墨烯（GDYO），然后将其化学和电化学还原为化学还原的GDYO（cr-GDYO）和电化学还原的GDYO（er-GDYO）。用六氨合氯化钌（[Ru（NH ₃）₆ ] Cl ₃）和铁氰化钾（K ₃ Fe（CN）₆）作为氧化还原探针。我们发现，此处在GDYs处使用的氧化还原探针的电子转移动力学取决于电子态（DOS）的密度和表面化学的协同作用以及材料的亲水性，并且在cr- GDYO和er-GDYO的速度比GDY和GDYO的快，并且与碳纳米管和石墨烯及其衍生物（即GO，cr-GO和er-GO）的可比性相当。这些特性与GDY独特的电子和化学结构相结合，从根本上使GDY成为一种新型电极材料，可用于碳电化学和各种电分析应用的基础研究。