Unexpected catalytic activity of nanorippled graphene.
Unexpected catalytic activity of nanorippled graphene.
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DOI：
10.1073/pnas.2300481120
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发表时间：
2023-03-21
影响因子：
11.1
通讯作者：
Geim, A. K.
中科院分区：
文献类型：
--
作者：
Sun, P. Z.;Xiong, W. Q.;Bera, A.;Timokhin, I.;Wu, Z. F.;Mishchenko, A.;Sellers, M. C.;Liu, B. L.;Cheng, H. M.;Janzen, E.;Edgar, J. H.;V. Grigorieva, I.;Yuan, S. J.;Geim, A. K.
石墨烯是一种孤立的石墨原子平面，通常被认为会继承石墨的大部分性质。据报道，就这两种材料的化学活性而言，这些预期是错误的。事实上，石墨是自然界中已知的最惰性的材料之一。相比之下，这里显示的石墨烯分解分子氢的能力与已知的最好的催化剂一样强。这归因于这样一个事实，即石墨烯单分子膜不是平坦的(就像在石墨中一样)，但不可避免地具有纳米级的波纹，作为氢气分解的活性位置。这一结果对所有天生非平坦的二维(2D)材料都有意义，这些材料可能表现出与它们的体相对应物非常不同的化学和催化性能。石墨是化学惰性最强的材料之一。它的基本成分，单层石墨烯，通常被认为会继承母体材料的大部分性质，包括化学惰性。在这里，我们表明，与石墨不同，无缺陷单层石墨烯在裂解分子氢方面表现出很强的活性，这与金属和其他已知的催化该反应的催化剂相当。我们将这种意想不到的催化活性归因于表面波纹(纳米级波纹)，这一结论得到了理论支持。纳米颗粒很可能在其他涉及石墨烯的化学反应中发挥作用，而且由于纳米颗粒是原子薄晶体固有的，因此通常对二维(2D)材料来说可能是重要的。
Graphene, an isolated atomic plane of graphite, is generally expected to inherit most of graphite’s properties. These expectations are reported to be wrong as far as chemical activity of the two materials is concerned. Indeed, graphite is one of the most inert materials known in nature. In contrast, graphene is shown here to dissociate molecular hydrogen as strongly as the best catalysts known for this reaction. This is attributed to the fact that graphene monolayers are not flat (as within graphite) but unavoidably have nanoscale ripples that serve as active sites for hydrogen splitting. The results have implications for all two-dimensional (2D) materials that being inherently nonflat may exhibit chemical and catalytic properties very different from their bulk counterparts. Graphite is one of the most chemically inert materials. Its elementary constituent, monolayer graphene, is generally expected to inherit most of the parent material’s properties including chemical inertness. Here, we show that, unlike graphite, defect-free monolayer graphene exhibits a strong activity with respect to splitting molecular hydrogen, which is comparable to that of metallic and other known catalysts for this reaction. We attribute the unexpected catalytic activity to surface corrugations (nanoscale ripples), a conclusion supported by theory. Nanoripples are likely to play a role in other chemical reactions involving graphene and, because nanorippling is inherent to atomically thin crystals, can be important for two-dimensional (2D) materials in general.
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