Two-Dimensional Boridene Nanosheets for Efficient Electrochemical Nitrogen Fixation Under Ambient Conditions

ChemSusChem. 2024 Oct 9:e202401912. doi: 10.1002/cssc.202401912. Online ahead of print.

Abstract

The carbon-free electrocatalytic nitrogen reduction reaction (NRR) is an alternative technology to the current Haber-Bosch method, that can be conducted under ambient conditions, and directly converting water and nitrogen (N₂) into ammonia (NH₃). However, the limited activity and selectivity of NH₃ electrosynthesis hinder the practical applications of NRR. In this study, we present a novel type of electrocatalyst called boridene nanosheets enriched with metal vacancies that are specifically designed for efficient electrocatalytic NRR under ambient conditions. Electrochemical testing in a 0.1 M phosphate-buffered saline (PBS) electrolyte demonstrates that boridene exhibits a high Faradaic efficiency of 66.7 % for NH₃ production at -0.2 V vs. RHE, with a maximum NH₃ yield rate of 23.6 μg h-1 mgcat -1 at -0.4 V vs. RHE. Durability tests show that boridene maintains significant stability throughout multiple cycles of NRR. Mechanistic insights are obtained through in situ Fourier transform infrared spectroscopy, revealing that boridene exhibits a preference for the distal pathway during the process of NRR. These findings highlight the potential of boridene as an efficient and stable catalyst for sustainable NH₃ synthesis.

Keywords: Ammonia synthesis; Boridene; Nitrogen fixation; Nitrogen reduction reaction; Two-dimensional catalyst.