Screening highly active perovskites for hydrogen-evolving reaction via unifying ionic electronegativity descriptor
Guan, Zhou, Huang, Dong, Wang, Zhou, Shao (2019) Screening highly active perovskites for hydrogen-evolving reaction via unifying ionic electronegativity descriptor Nat Commun (IF: 16.6) 10(1) 3755
Full text
Click the PDF icon to view the full text of the paper
Abstract
Facile and reliable screening of cost-effective, high-performance and scalable electrocatalysts is key for energy conversion technologies such as water splitting. ABO3-δ 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+δ 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.
Links
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6704169http://www.ncbi.nlm.nih.gov/pubmed/31434892
http://dx.doi.org/10.1038/s41467-019-11847-w
