Ehlert Christopher, Piras Anna, Schleicher Juliette, Gryn'ova Ganna
Heidelberg Institute for Theoretical Studies (HITS gGmbH), Schloss-Wolfsbrunnenweg 35, 69118 Heidelberg, Germany.
Interdisciplinary Center for Scientific Computing, Heidelberg University, Im Neuenheimer Feld 205, 69120 Heidelberg, Germany.
J Phys Chem Lett. 2023 Jan 19;14(2):476-480. doi: 10.1021/acs.jpclett.2c03481. Epub 2023 Jan 10.
Heteroatom-doped polyaromatic hydrocarbons (or nanographenes) are promising molecular electrocatalysts for the oxygen reduction reaction (ORR). Here, we use density functional theory to investigate the first step of the ORR pathway (chemisorption) for a set of molecules with experimentally determined catalytic activities. Weak chemisorption is found for only negatively charged catalysts, and a strong correlation is observed between the computed electron affinities and experimental catalytic activities for a range of B- and B,N-doped polyaromatic hydrocarbons. The electron affinity is put forward as a simple activity descriptor of charged (activated) catalysts on an electrode.
杂原子掺杂的多环芳烃（或纳米石墨烯）是用于氧还原反应（ORR）的有前景的分子电催化剂。在此，我们使用密度泛函理论来研究一组具有实验测定催化活性的分子的ORR途径的第一步（化学吸附）。仅对带负电荷的催化剂发现了弱化学吸附，并且在一系列B和B，N掺杂的多环芳烃的计算电子亲和能与实验催化活性之间观察到强相关性。电子亲和能被提出作为电极上带电（活化）催化剂的简单活性描述符。
