铜基氧化石墨烯上意外自发的水解离
Unexpectedly Spontaneous Water Dissociation on Graphene Oxide Supported by Copper Substrate
摘要：
水解离在科学领域中具有根本的重要性，并且在各种技术应用中引起了相当大的兴趣。然而，破坏水分子内的O-H键的高活化势垒已被确定为瓶颈，即使对于吸附在氧化石墨烯（GO）上的水也是如此。在此，使用密度泛函理论计算，我们证明了水分子可以在由铜衬底（111）表面支撑的GO（Copper-GO）上自发解离。该过程涉及质子从水转移到界面氧基团，以及与GO共价键合的氢氧化物。与GO上的水解离势垒相比，铜-GO上的水解离势垒显著降低至小于热波动或与热波动相当。这归因于铜基底和GO之间的轨道杂化相互作用，其增强了GO基面上的界面氧基团对水解离的反应活性。我们的工作提供了一种新的策略，通过衬底增强的反应活性的界面氧基团在GO上访问水解离，并表明衬底可以作为一个重要的关键，调整各种二维材料器件的催化性能。
英文摘要：
Water dissociation is of fundamental importance in scientific fields and has drawn considerable interest in diverse technological applications. However, the high activation barrier of breaking the O-H bond within the water molecule has been identified as the bottleneck, even for the water adsorbed on the graphene oxide (GO). Herein, using the density functional theory calculations, we demonstrate that the water molecule can be spontaneously dissociated on GO supported by the (111) surface of the copper substrate (Copper-GO). This process involves a proton transferring from water to the interfacial oxygen group, and a hydroxide covalently bonding to GO. Compared to that on GO, the water dissociation barrier on Copper-GO is significantly decreased to be less than or comparable to thermal fluctuations. This is ascribed to the orbital-hybridizing interaction between copper substrate and GO, which enhances the reaction activity of interfacial oxygen groups along the basal plane of GO for water dissociation. Our work provides a novel strategy to access water dissociation via the substrate-enhanced reaction activity of interfacial oxygen groups on GO and indicates that the substrate can serve as an essential key to tuning the catalytic performance of various two-dimensional material devices.
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