General π-electron-assisted strategy for single-atom (Ir, Pt, Ru, Pd, Fe, and Ni) electrocatalysts with bi-functional active sites toward highly efficient water splitting

Authors

Weihong Lai, University of WollongongFollow
Li-Fu Zhang, Nankai University
Wei-Bo Hua, Karlsruhe Institute of Technology
Sylvio Indris, Karlsruhe Institute of Technology
Zichao Yan, University of WollongongFollow
Zhe Hu, University of Wollongong, Nankai UniversityFollow
Binwei Zhang, University of WollongongFollow
Yani Liu, University of Wollongong, Beihang UniversityFollow
Li Wang, University of WollongongFollow
Min Liu, Beijing University of TechnologyFollow
Rong Liu, Western Sydney University
Yunxiao Wang, University of WollongongFollow
Jiazhao Wang, University of WollongongFollow
Zhenpeng Hu, Nankai University
Hua-Kun Liu, University of WollongongFollow
Shulei Chou, University of WollongongFollow
Shi Xue Dou, University of WollongongFollow

RIS ID

137938

Publication Details

Lai, W., Zhang, L., Hua, W., Indris, S., Yan, Z., Hu, Z., Zhang, B., Liu, Y., Wang, L., Liu, M., Liu, R., Wang, Y., Wang, J., Hu, Z., Liu, H., Chou, S. & Dou, S. (2019). General p-Electron-Assisted Strategy for Ir, Pt, Ru, Pd, Fe, Ni Single- Atom Electrocatalysts with Bifunctional Active Sites for Highly Efficient Water Splitting. Angewandte Chemie-international Edition, 58 (34), 11868-11873.

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 pelectron- assisted strategy to anchor single-atom sites (M=Ir, Pt, Ru, Pd, Fe, Ni) on a heterogeneous support is reported. The Matoms 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 1.603V to achieve 10 mAcm@2 in 1.0m 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.

Grant Number

ARC/LP120200432, ARC/DE170100928, ARC/LE0237478