Dynamic active-site generation of atomic iridium stabilized on nanoporous metal phosphides for water oxidation

• Published in: Nature communications Vol. 11; no. 1; pp. 2701 - 9
• Main Authors: Jiang, Kang, Luo, Min, Peng, Ming, Yu, Yaqian, Lu, Ying-Rui, Chan, Ting-Shan, Liu, Pan, de Groot, Frank M. F., Tan, Yongwen
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 01.06.2020; Nature Publishing Group; Nature Portfolio
• Subjects: 147/135; 147/143; 639/301/299/161/886; 639/301/299/886; Absorption spectroscopy; Atomic structure; Catalysts; Catalytic activity; Coupling; Electronic structure; Fourier transforms; Humanities and Social Sciences; Iridium; Ligands; Materials science; Metal oxides; multidisciplinary; Oxidation; Oxygen; Oxygen evolution reactions; Phosphides; Reconstruction; Science; Science (multidisciplinary); Single atom catalysts; Water splitting; X ray absorption; X-ray absorption spectroscopy
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-020-16558-1

Designing efficient single-atom catalysts (SACs) for oxygen evolution reaction (OER) is critical for water-splitting. However, the self-reconstruction of isolated active sites during OER not only influences the catalytic activity, but also limits the understanding of structure-property relationships. Here, we utilize a self-reconstruction strategy to prepare a SAC with isolated iridium anchored on oxyhydroxides, which exhibits high catalytic OER performance with low overpotential and small Tafel slope, superior to the IrO 2 . Operando X-ray absorption spectroscopy studies in combination with theory calculations indicate that the isolated iridium sites undergo a deprotonation process to form the multiple active sites during OER, promoting the O–O coupling. The isolated iridium sites are revealed to remain dispersed due to the support effect during OER. This work not only affords the rational design strategy of OER SACs at the atomic scale, but also provides the fundamental insights of the operando OER mechanism for highly active OER SACs. Direct observation of the atomic and electronic structure of a single-atom catalyst is essential. Here, the authors report an oxyhydroxide stabilized iridium catalyst with superior oxygen evolution catalytic activity and identify the isolated iridium sites which promote the H 2 O attack and O–O coupling.