Montoya Joseph H, Doyle Andrew D, Nørskov Jens K, Vojvodic Aleksandra
Energy Technologies Area, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, USA.
Phys Chem Chem Phys. 2018 Jan 31;20(5):3813-3818. doi: 10.1039/c7cp06539f.
The reactivity of solid oxide surfaces towards adsorption of oxygen and hydrogen is a key metric for the design of new catalysts for electrochemical water splitting. In this paper, we report on trends in the adsorption energy of different adsorbed intermediates derived from the oxidation and reduction of water for ternary ABO oxides in the cubic perovskite structure. Our findings support a previously reported trend that rationalizes the observed lower bound in oxygen evolution (OER) overpotentials from correlations in OH* and OOH* adsorption energies. In addition, we report hydrogen adsorption energies that may be used to estimate hydrogen evolution (HER) overpotentials along with potential metrics for electrochemical metastability in reducing environments. We also report and discuss trends between atom-projected density of states and adsorption energies, which may enable a design criteria from the local electronic structure of the active site.
固体氧化物表面对氧和氢吸附的反应性是设计用于电化学水分解的新型催化剂的关键指标。在本文中，我们报道了立方钙钛矿结构中三元ABO氧化物水氧化和还原衍生的不同吸附中间体吸附能的趋势。我们的研究结果支持了先前报道的一种趋势，该趋势通过OH和OOH吸附能的相关性合理化了观察到的析氧（OER）过电位下限。此外，我们报告了氢吸附能，其可用于估计析氢（HER）过电位以及还原环境中电化学亚稳性的潜在指标。我们还报告并讨论了原子投影态密度与吸附能之间的趋势，这可能从活性位点的局部电子结构得出设计标准。
