Spatially Confined Assembly of Monodisperse Ruthenium Nanoclusters in a Hierarchically Ordered Carbon Electrode for Efficient Hydrogen Evolution

Zhong-Li Wang; Keju Sun; Joel Henzie; Xianfeng Hao; Cuiling Li; Toshiaki Takei; Yong-Mook Kang; Yusuke Yamauchi

doi:10.1002/anie.201801467

Spatially Confined Assembly of Monodisperse Ruthenium Nanoclusters in a Hierarchically Ordered Carbon Electrode for Efficient Hydrogen Evolution

Angew Chem Int Ed Engl. 2018 May 14;57(20):5848-5852. doi: 10.1002/anie.201801467. Epub 2018 Apr 14.

Authors

Zhong-Li Wang¹, Keju Sun², Joel Henzie¹, Xianfeng Hao², Cuiling Li¹, Toshiaki Takei¹, Yong-Mook Kang³, Yusuke Yamauchi^{4

5}

Affiliations

¹ International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba, Ibaraki, 305-0044, Japan.
² College of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao, 066004, China.
³ Department of Energy and Materials Engineering, Dongguk University-Seoul, Seoul, 04620, South Korea.
⁴ School of Chemical Engineering & Australian Institute for Bioengineering and Nanotechnology (AIBN), The University of Queensland, Brisbane, QLD 4072, Australia.
⁵ Department of Plant & Environmental New Resources, Kyung Hee University, Gyeonggi-do, 17104, South Korea.

PMID: 29656420
DOI: 10.1002/anie.201801467

Abstract

The redox units of polyaniline (PAni) are used cooperatively, and in situ, to assemble ruthenium (Ru) nanoclusters in a hierarchically ordered carbon electrode. The oxidized quinonoid imine (QI) units in PAni bond Ru complex ions selectively, whereas reduced benzenoid amine (BA) units cannot. By electrochemically tuning the ratio of QI to BA, Ru complexes are spatially confined in the outer layer of hierarchical PAni frameworks. Carbonization of Ru-PAni hybrids induces nucleation on the outer surface of the carbon support, generating nearly monodisperse Ru nanoclusters. The optimized catalyst has a low loading of approximately 2 wt % Ru, but exhibits a mass activity for the hydrogen evolution reaction that is about 6.8 times better than commercial 20 wt % Pt/C catalyst.

Keywords: electrocatalysis; integrated electrodes; metal nanoclusters; polyaniline; ruthenium.

Publication types

Research Support, Non-U.S. Gov't