Gono Patrick, Pasquarello Alfredo
Chair of Atomic Scale Simulation (CSEA), Ecole Polytechnique Fédérale de Lausanne (EPFL), CH-1015 Lausanne, Switzerland.
J Chem Phys. 2021 Jan 14;154(2):024706. doi: 10.1063/5.0036019.
The outstanding performance of NiOOH/FeOOH-based oxygen evolution reaction (OER) catalysts is rationalized in terms of a bifunctional mechanism involving two distinct active sites. In this mechanism, the OOH reaction intermediate, which unfavorably affects the overall OER activity due to the linear scaling relationship, is replaced by O adsorbed at the active site on FeOOH and H adsorbed at the NiOOH substrate. Here, we use the computational hydrogen electrode method to assess promising models of both the FeOOH catalyst and the NiOOH hydrogen acceptor. These two materials are interfaced in various ways to evaluate their performance as bifunctional OER catalysts. In some cases, overpotentials as low as 0.16 V are found, supporting the bifunctional mechanism as a means to overcome the limitations imposed by linear scaling relationships.
基于NiOOH/FeOOH的析氧反应（OER）催化剂的卓越性能可通过涉及两个不同活性位点的双功能机制来解释。在该机制中，由于线性标度关系而对整体OER活性产生不利影响的OOH反应中间体，被吸附在FeOOH活性位点上的O和吸附在NiOOH基底上的H所取代。在此，我们使用计算氢电极方法来评估FeOOH催化剂和NiOOH氢受体的潜在模型。这两种材料以各种方式结合，以评估它们作为双功能OER催化剂的性能。在某些情况下，发现过电位低至0.16 V，这支持了双功能机制是克服线性标度关系所带来限制的一种手段。
