Rational design of artificial Lewis pairs coupling with polyethylene glycol for efficient electrochemical ammonia synthesis

The FeOOH-150 nanorod with Lewis acid-base pairs (LPs) on the surface could effectively drive the nitrogen reduction reaction. PEG was introduced to serve as a local non-aqueous electrolyte system to inhibit HER, and DFT calculations revealed that the interaction of PEG with LPs can optimize nitroge...

Full description

Saved in:
Bibliographic Details
Published in:Journal of colloid and interface science 2023-11, Vol.649, p.166-174
Main Authors: Wang, Haifan, Yuan, Menglei, Zhang, Jingxian, Bai, Yiling, Zhang, Ke, Li, Bin, Zhang, Guangjin
Format: Article
Language:English
Subjects:
Electrochemical nitrogen reduction
Lewis acid-base pairs
Nitrogen adsorption configuration
Polyethylene glycol (PEG)
Citations: Items that this one cites
Items that cite this one
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:The FeOOH-150 nanorod with Lewis acid-base pairs (LPs) on the surface could effectively drive the nitrogen reduction reaction. PEG was introduced to serve as a local non-aqueous electrolyte system to inhibit HER, and DFT calculations revealed that the interaction of PEG with LPs can optimize nitrogen adsorption configuration and promoted eNRR process. [Display omitted] Ammonia (NH3) synthesis at mild conditions by electrocatalytic nitrogen reduction (eNRR) has received more attention and has been regarded as a promising alternative to the traditional Haber–Bosch process. Lewis acid-base pairs (LPs) can chemisorb and react with nitrogen by electronic interaction, while the tuning of the microenvironment near electrode can hinder hydrogen evolution reaction (HER) thus improving the selectivity of the eNRR. Herein, the FeOOH nanorod coupled with LPs on the surface (i.e., Fe, Fe–O) was synthesized, which could effectively drive eNRR. Meanwhile, polyethylene glycol (PEG) was introduced to serve as a local non-aqueous electrolyte system to inhibit HER. The prepared FeOOH-150 catalyst achieved outstanding eNRR performance with an NH3 yield rate of 118.07 μg h−1mgcat−1 and a Faradaic efficiency of 51.4 % at −0.6 V vs. RHE in 0.1 M LiClO4 + 20 % PEG. Both the experiment and DFT calculations revealed that the interaction of PEG with Lewis base sites could optimize nitrogen adsorption configuration and activation.
ISSN:0021-9797
1095-7103
DOI:10.1016/j.jcis.2023.06.097