General π‐Electron‐Assisted Strategy for Ir, Pt, Ru, Pd, Fe, Ni Single‐Atom Electrocatalysts with Bifunctional Active Sites for Highly Efficient Water Splitting. (10th July 2019)

• Record Type: Journal Article
• Authors: Lai, Wei‐Hong; Zhang, Li‐Fu; Hua, Wei‐Bo; Indris, Sylvio; Yan, Zi‐Chao; Hu, Zhe; Zhang, Binwei; Liu, Yani; Wang, Li; Liu, Min; Liu, Rong; Wang, Yun‐Xiao; Wang, Jia‐Zhao; Hu, Zhenpeng; Liu, Hua‐Kun; Chou, Shu‐Lei; Dou, Shi‐Xue
• Is Part Of: Angewandte Chemie. Volume 131:Number 34(2019)
• Page Start: 11994
• Page End: 11999
• Publication Date: 2019-07-10
• Subjects: Bifunktionale aktive Zentren -- Doppeldomänen -- Einzelatomkatalyse -- Elektrokatalyse -- Wasserspaltung; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.201904614
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: Both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) are crucial to water splitting, but require alternative active sites. Now, a general π‐electron‐assisted strategy to anchor single‐atom sites (M=Ir, Pt, Ru, Pd, Fe, Ni) on a heterogeneous support is reported. The M atoms can simultaneously anchor on two distinct domains of the hybrid support, four‐fold N/C atoms (M@NC), and centers of Co octahedra (M@Co), which are expected to serve as bifunctional electrocatalysts towards the HER and the OER. The Ir catalyst exhibits the best water‐splitting performance, showing a low applied potential of 1.603 V to achieve 10 mA cm −2 in 1.0 m KOH solution with cycling over 5 h. DFT calculations indicate that the Ir@Co (Ir) sites can accelerate the OER, while the Ir@NC3 sites are responsible for the enhanced HER, clarifying the unprecedented performance of this bifunctional catalyst towards full water splitting. Abstract : Doppelt gemoppelt : Die Wasserstoff‐ und die Sauerstoffentwicklungsreaktion sind essenziell für die Wasserspaltung, benötigen aber unterschiedliche aktive Zentren. Hier wird eine allgemeine, durch π‐Elektronen vermittelte Strategie vorgestellt, um Einzelatomzentren (M=Ir, Pt, Ru, Pd, Fe, Ni) auf heterogenen Materialien zu verankern. Die M‐Atome können dabei an verschiedenen Stellen des Hybridmaterials verankert werden.