Two-Dimensional N-Doped Carbon with Embedded Microfluidic-Architected Fe, Mo Nanodots toward Efficient Electrocatalytic Nitrogen Reduction

• Published in: ACS sustainable chemistry & engineering 2024-01, Vol.12 (4), p.1694-1704
• Main Authors: Liu, Hengyuan, Liu, Yingzhe, Zeng, Xuecheng, Yu, Xude, Xu, Jianhong
• Format: Article
• Language: English
• ISSN: 2168-0485; 2168-0485
• DOI: 10.1021/acssuschemeng.3c07338

Electrocatalytic nitrogen reduction reaction (ENRR) is emerging as a promising routine for the sustainable production of ammonia. Hindered by the strong triple bond in N2 and unfavorable hydrogen evolution reaction, it is critical to develop efficient catalysts with excellent activity and selectivity. Herein, we propose a novel microfluidic platform that achieves the continuous synthesis and morphology regulation of a two-dimensional heterocatalyst FeMo/g-C3N4 through a precipitation process in a confined space. Owing to the rapid mixing and microfluidic manipulation, FeMo/g-C3N4 maintains an overwhelmingly favorable structure compared to the batch methods. Benefiting from the ultrasmall active sites (0.86 nm), homogeneous nanodot distribution, and abundant 2D surface, the promoted N2 chemisorption and competitive ENRR performance can be simultaneously ensured, as confirmed by the experimental studies. By varying the applied working potential, the optimal ammonia yield can be determined as 33.25 μg h–1 mgcat. –1 at −1.2 V. This work innovatively opens a pathway for morphological fine structural tuning of two-dimensional heterocatalysts, further promoting the ENRR field’s development.