Jiangsu National Synergetic Innovation Center for Advanced Materials (SICAM), State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, No. 5 Xin Mofan Road, 210009, Nanjing, P.R. China.
Department of Applied Mathematics, Research School of Physics and Engineering, Australian National University, Canberra, ACT, 0200, Australia.
Nat Commun. 2019 Jan 11;10(1):149. doi: 10.1038/s41467-018-08117-6.
Efficient electrocatalysts for hydrogen evolution reaction are key to realize clean hydrogen production through water splitting. As an important family of functional materials, transition metal oxides are generally believed inactive towards hydrogen evolution reaction, although many of them show high activity for oxygen evolution reaction. Here we report the remarkable electrocatalytic activity for hydrogen evolution reaction of a layered metal oxide, Ruddlesden-Popper-type SrRuO with alternative perovskite layer and rock-salt SrO layer, in an alkaline solution, which is comparable to those of the best electrocatalysts ever reported. By theoretical calculations, such excellent activity is attributed mainly to an unusual synergistic effect in the layered structure, whereby the (001) SrO-terminated surface cleaved in rock-salt layer facilitates a barrier-free water dissociation while the active apical oxygen site in perovskite layer promotes favorable hydrogen adsorption and evolution. Moreover, the activity of such layered oxide can be further improved by electrochemistry-induced activation.
高效的析氢反应电催化剂是通过水分解实现清洁制氢的关键。作为一类重要的功能材料,过渡金属氧化物通常被认为对析氢反应没有活性,尽管其中许多物质对析氧反应表现出很高的活性。在这里,我们报道了层状金属氧化物 Ruddlesden-Popper 型 SrRuO 具有独特的析氢反应电催化活性,在碱性溶液中具有与以往报道的最佳电催化剂相当的活性。通过理论计算,这种优异的活性主要归因于层状结构中的一种不寻常的协同效应,其中在岩盐层中 SrO 终止的(001)表面易于无阻碍地进行水离解,而钙钛矿层中的活性顶角氧位则促进了有利的氢吸附和演化。此外,通过电化学诱导活化可以进一步提高这种层状氧化物的活性。