Significantly Enhanced Hydrogen Evolution Activity of Freestanding Pd-Ru Distorted Icosahedral Clusters with less than 600 Atoms

Suli Liu; Qinghua Zhang; Jianchun Bao; Yafei Li; Zhihui Dai; Lin Gu

doi:10.1002/chem.201702913

Significantly Enhanced Hydrogen Evolution Activity of Freestanding Pd-Ru Distorted Icosahedral Clusters with less than 600 Atoms

Chemistry. 2017 Dec 22;23(72):18203-18207. doi: 10.1002/chem.201702913. Epub 2017 Nov 30.

Authors

Suli Liu¹, Qinghua Zhang², Jianchun Bao¹, Yafei Li¹, Zhihui Dai¹, Lin Gu^{2

3}

Affiliations

¹ Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials and Jiangsu Key Laboratory of Biofunctional Materials, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing, 210023, P. R. China.
² Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, P. R. China.
³ Collaborative Innovation Centre of Quantum Matter, School of Physical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.

PMID: 28741317
DOI: 10.1002/chem.201702913

Abstract

Freestanding metal nanoclusters can tune, precisely and effectively, the Gibbs free energy (ΔG_H ) of atomic hydrogen on the surface of materials. This enables the enhancement of hydrogen evolution activity. In this paper, we report a study of freestanding Pd-Ru distorted icosahedral clusters (ico-clusters) with less than 600 atoms by using a simple one-pot synthesis method. This Pd-Ru ico-cluster can be used as an efficient electrocatalyst for the hydrogen evolution reaction (HER) in acidic water, which is a promising alternative to Pt. The experimental and theoretical results suggest that the face-centered cubic (fcc) freestanding Pd-Ru distorted ico-clusters with less than 600 atoms ensure increased active edges and distorted defect sites, which reduce the coordination number for the atoms on the catalyst surface. Furthermore, Ru is a more effective hydrogen dissociation source, whereas Pd has a better hydrogen storage function. Pd-Ru can tune the ΔG_H of atomic hydrogen adsorbed on a catalyst and reach an optimal equilibrium state that improves the HER performance. Our studies represent a robust approach towards the development of freestanding Pd-Ru distorted ico-clusters and advanced catalysts with non-Pt content for HER and many other heterogeneous reactions.

Keywords: distorted clusters; electrocatalysts; freestanding clusters; hydrogen evolution; ruthenium.