Hyperbranched concave octahedron of PtIrCu nanocrystals with high-index facets for efficiently electrochemical ammonia oxidation reaction

Xu Lin; Xiaoran Zhang; Zhen Wang; Xinxin Zhu; Jinhui Zhu; Pinsong Chen; Taiyu Lyu; Changzheng Li; Zhi Qun Tian; Pei Kang Shen

doi:10.1016/j.jcis.2021.04.068

Hyperbranched concave octahedron of PtIrCu nanocrystals with high-index facets for efficiently electrochemical ammonia oxidation reaction

J Colloid Interface Sci. 2021 Nov:601:1-11. doi: 10.1016/j.jcis.2021.04.068. Epub 2021 Apr 17.

Authors

Affiliations

¹ Collaborative Innovation Center of Sustainable Energy Materials, School of Physical Science and Technology; Guangxi Key Laboratory of Electrochemical Energy Materials; Key Laboratory of New Processing Technology for Non-ferrous Metal and Materials, Ministry of Education, Guangxi University, Nanning, 530004, China.
² School of Mechanical Engineering, Guangxi University, Nanning 530004, China.
³ Collaborative Innovation Center of Sustainable Energy Materials, School of Physical Science and Technology; Guangxi Key Laboratory of Electrochemical Energy Materials; Key Laboratory of New Processing Technology for Non-ferrous Metal and Materials, Ministry of Education, Guangxi University, Nanning, 530004, China. Electronic address: tianzhiqun@gxu.edu.cn.

PMID: 34052723
DOI: 10.1016/j.jcis.2021.04.068

Abstract

Ammonia oxidation reaction (AOR) via electrocatalysis is one of the most efficient ways of utilizing ammonia (a zero-carbon fuel with high hydrogen content) for renewable energy systems. However, AOR seriously suffers from the slow kinetics, and low durability due to its multi-electron transfer process and the poison of the reaction intermediates (N_ads and NO_ads) to precious metal catalysts. Herein, hyperbranched concave octahedral nanodendrites of PtIrCu (HCOND) with high-index facets of {553}, {331} and {221} were developed for the first time using a solvothermal method. The HCOND possesses PtIr-rich edges and exhibit highly efficient AOR activity and stability in alkaline media, wherein their onset potential is 0.35 V vs.RHE, which is 60 mV and 160 mV lower than that of the PtIrCu nanoparticles (NPs) (0.41 V) and commercial Pt/C (0.51 V), respectively, and its high mass activity of 40.6 A g_PtIr^-1 at the 0.5 V vs.RHE is 10.3 times, 2.34 times higher than that of commercial Pt/C (3.9 A g_Pt^-1) and PtIrCu NPs (17.3 A g_PtIr^-1), respectively. In addition, its peak current density (122.9 A g_PtIr^-1) is only reduced by 17.7% after 2000-cycles accelerated durability test. Meanwhile, the performance of PtIrCu HCOND is also better than that of other previously reported morphologies of Pt based catalysts (eg. nanoparticles, nanocubes, nanofilm, nanoflowers). The improvement is critically ascribed to unique advantages of the specific HCOND structure including PtIr rich surface, high-index faceted nanodendrites, strong lattice strain and electronic effects. These characteristics endow the HCOND with great promise to reduce Pt and Ir loading dramatically in the practical application of direct ammonia fuel cells.

Keywords: Ammonia Oxidation Reaction; Fuel Cells; High-Index Facet; Nanocrystals; PtIr Alloy.