化学
电催化剂
过电位
电泳剂
催化作用
卟啉
配体(生物化学)
组合化学
合理设计
亲核细胞
光化学
化学物理
纳米技术
有机化学
物理化学
电化学
电极
材料科学
生物化学
受体
作者
Daiki Nishiori,Jan Paul Menzel,Nicholas R. Armada,Edgar A. Reyes Cruz,Brent L. Nannenga,Víctor S. Batista,Gary F. Moore
摘要
The design of efficient electrocatalysts is limited by scaling relationships governing trade-offs between thermodynamic and kinetic performance metrics. This ″iron law″ of electrocatalysis arises from synthetic design strategies, where structural alterations to a catalyst must balance nucleophilic versus electrophilic character. Efforts to circumvent this fundamental impasse have focused on bioinspired applications of extended coordination spheres and charged sites proximal to a catalytic center. Herein, we report evidence for breaking a molecular scaling relationship involving electrocatalysis of the oxygen reduction reaction (ORR) by leveraging ligand design. We achieve this using a binuclear catalyst (a diiron porphyrin), featuring a macrocyclic ligand with extended electronic conjugation. This ligand motif delocalizes electrons across the molecular scaffold, improving the catalyst's nucleophilic and electrophilic character. As a result, our binuclear catalyst exhibits low overpotential and high catalytic turnover frequency, breaking the traditional trade-off between these two metrics.
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