High Catalytic Activity of Co-centered 2D Metal Organic
Frameworks toward Bifunctional Oxygen Evolution and Reduction Reactions:
Rationalized by Spin Polarization Effect
posted on 2023-12-12, 18:11authored byLiang Hu, Feifan Wang, Yu Jing
CoX4 (X = NH, S, and O) motifs have demonstrated their
high catalytic activity in the platforms of metal organic frameworks
(MOFs), however, the underlying reason is still unrevealed. Herein,
we propose monolayers constructed by linking TMNxO4‑x motifs (TM = Fe,
Co, Ni, Cu) with trioxotriangulenes (TOTs) as suitable models to clarify
the structure–property–performance relationship of 2D
MOFs for the oxygen evolution/reduction reaction (OER/ORR). The highly
robust catalytic activity of CoNxO4‑x for both the OER and the ORR has
been confirmed, even surpassing that of most previously reported 2D
MOFs and SACs. This activity is attributed to the moderate interaction
between Co and the key intermediate species, which can be modulated
by the coordinating atoms. We reveal spin momentum as a reliable activity
descriptor in rationalizing the OER/ORR activity, which can be extended
to many other 2D MOFs. The elucidated structure–activity relationship
is significant for the development of effective bifunctional OER/ORR
electrocatalysts.