Screening highly active perovskites for hydrogen-evolving reaction via unifying ionic electronegativity descriptor.

ABSTRACT: Facile and reliable screening of cost-effective, high-performance and scalable electrocatalysts is key for energy conversion technologies such as water splitting. ABO3-? perovskites, with rich constitutions and structures, have never been designed via activity descriptors for critical hydrogen evolution reaction (HER). Here, we apply coordination rationales to introduce A-site ionic electronegativity (AIE) as an efficient unifying descriptor to predict the HER activities of 13 cobalt-based perovskites. Compared with A-site structural or thermodynamic parameter, AIE endows the HER activity with the best volcano trend. (Gd0.5La0.5)BaCo2O5.5+? predicted from an AIE value of?~2.33 exceeds the state-of-the-art Pt/C catalyst in electrode activity and stability. X-ray absorption and computational studies reveal that the peak HER activities at a moderate AIE value of?~2.33 can be associated with the optimal electronic states of active B-sites via inductive effect in perovskite structure (~200?nm depth), including Co valence, Co-O bond covalency, band gap and O 2p-band position.

SUBMITTER: Guan D 

PROVIDER: S-EPMC6704169 | biostudies-literature | 2019 Aug

REPOSITORIES: biostudies-literature