基于计算机的新型掺杂剂在 Fe 掺杂 Ni 氢氧化物 (NiFe OOH) 催化剂中用于析氧反应的发现。

In Silico Discovery of New Dopants for Fe-Doped Ni Oxyhydroxide (NiFe OOH) Catalysts for Oxygen Evolution Reaction.

机构信息

Materials and Process Simulation Center (MSC) and Joint Center for Artificial Photosynthesis (JCAP) , California Institute of Technology , Pasadena , California 91125 , United States.

出版信息

J Am Chem Soc. 2018 Jun 6;140(22):6745-6748. doi: 10.1021/jacs.8b02225. Epub 2018 May 21.

DOI:10.1021/jacs.8b02225

PMID:29749225

Abstract

The oxygen evolution reaction (OER) is critical to efficient water splitting to produce the H fuel for sustainable energy production. Currently, the best non-noble metal OER electrocatalyst in base conditions is the Fe-doped NiOOH (NiFe OOH), with an overpotential of η = 0.4, but much lower values are desired. We use density functional theory to determine the overall mechanism for the OER of NiFe OOH, concluding that promoting radical character on the metal-oxo bond is critical to efficient OER. Then we consider replacing Fe with 17 other transition metals of the Fe, Ru, and Os rows, where we find 3 new promising candidates: Co, Rh, and Ir, which we estimate to have η = 0.27, 0.15, and 0.02, respectively, all very much improved performance compared to Fe, making all three systems excellent candidates for experimental testing.

摘要

析氧反应（OER）对于高效水分解以生产可持续能源生产的 H 燃料至关重要。目前，在碱性条件下最好的非贵金属 OER 电催化剂是掺杂 Fe 的 NiOOH（NiFe OOH），其过电位为 η = 0.4，但人们希望得到更低的值。我们使用密度泛函理论来确定 NiFe OOH 的 OER 总机制，得出结论，促进金属-氧键上的自由基特性对于高效 OER 至关重要。然后，我们考虑用 Fe 、 Ru 和 Os 列中的其他 17 种过渡金属替代 Fe，在这些金属中，我们发现了 3 种有前途的新候选物：Co、Rh 和 Ir，我们估计它们的 η 值分别为 0.27、0.15 和 0.02，与 Fe 相比，所有这三种系统的性能都有了很大的提高，这使得这三种系统都成为实验测试的优秀候选物。