Electrocatalytic nitrogen reduction to ammonia by atomically precise Cu6 nanoclusters supported on graphene oxide

Aamir Shehzad; Chaonan Cui; Ran Cheng; Zhixun Luo

doi:10.1039/d4nr01984a

Electrocatalytic nitrogen reduction to ammonia by atomically precise Cu₆ nanoclusters supported on graphene oxide

Nanoscale. 2024 Aug 7;16(30):14441-14447. doi: 10.1039/d4nr01984a.

Authors

Aamir Shehzad^{1

2}, Chaonan Cui¹, Ran Cheng^{1

2}, Zhixun Luo^{1

2}

Affiliations

¹ State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China. chncui@iccas.ac.cn.
² School of Chemistry, University of Chinese Academy of Sciences, Beijing 100049, China.

PMID: 39012338
DOI: 10.1039/d4nr01984a

Abstract

The electrocatalytic nitrogen reduction reaction (NRR) enables the production of ammonia by the use of renewable energy, providing a direct method for nitrogen fixation. Nevertheless, the NRR process under ambient conditions is often impeded by inertness of N₂ and the occurrence of hydrogen evolution as a byproduct in aqueous electrolytes, resulting in a diminished reaction rate and reduced efficiency. In this study, we synthesized Cu₆(SMPP)₆ nanoclusters (Cu₆ NCs for short) and immobilized them on graphene oxide (GO) to investigate their electrocatalytic nitrogen reduction reaction (ENRR) using an H-cell setup. The GO-supported Cu₆ NCs exhibit enhanced catalysis with a high NH₃ yield rate of 4.8 μg h^-1 cm^-2 and a high faradaic efficiency up to 30.39% at -1.1 V. Quantum chemistry calculations reveal that the Cu₆S₆ cluster on GO support facilitates the N₂ adsorption and NN bond activation with a surmountable energy barrier for the potential-determining step (N₂* → NNH*).