聚吡咯
催化作用
纳米颗粒
纳米结构
硫黄
化学工程
涂层
纳米技术
材料科学
氧化还原
氧化物
密度泛函理论
化学
选择性
无机化学
电化学
有机化学
电极
计算化学
物理化学
工程类
作者
Fuhao Jin,Hanqing Yin,Ru Feng,Wei Niu,Wanting Zhang,Jingquan Liu,Aijun Du,Wenrong Yang,Zhen Liu
标识
DOI:10.1016/j.jcis.2023.05.108
摘要
The development of electrocatalysts for N2 reduction reaction (NRR) is significant for scalable and renewable NH3 synthesis, but calls for a technology innovation to overcome the specific problems of low efficiency and poor selectivity. Herein, we prepare a core–shell nanostructure by coating polypyrrole (PPy) onto sulfur-doped iron oxide nanoparticles (denoted as S-Fe2O3@PPy) as the highly selective and durable electrocatalysts for NRR under ambient conditions. Sulfur doping and PPy coating remarkably improve the charge transfer efficiency of S-Fe2O3@PPy, and the interactions between PPy and Fe2O3 nanoparticles produce abundant oxygen vacancies as active sites for NRR. This catalyst achieves an NH3 production rate of 22.1 μg h−1 mgcat−1 and a very-high Faradic efficiency of 24.6%, surpassing other Fe2O3 based NRR catalysts. Density functional theory calculations show that the S-coordinated iron site can successfully activate the N2 molecule and optimize the energy barrier during the reduction process, resulting in a small theoretical limiting potential.
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