Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 283, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119591
Keywords
Single-atom catalysts; Electrocatalytic CO2 reduction; Fluorine; Ultrathin nanosheets
Funding
- National Natural Science Foundation of China (NSFC) [21901246, 21905278]
- Natural Science Foundation of Fujian Province [2019J05158]
Ask authors/readers for more resources
The synthesis of a fluorine-tuned single-atom catalyst with ultrathin nanosheet morphology and high Ni content led to a remarkable electrocatalytic performance for CO2-to-CO conversion. The incorporation of F dopants modulates the electron configuration of active sites, reducing the energy barrier for CO2 activation and promoting the formation of the key *COOH intermediate.
A fluorine-tuned single-atom catalyst with an ultrathin nanosheet morphology (only similar to 1.25 nm) and high Ni content of 5.92 wt% was fabricated by a polymer-assisted pyrolysis approach. The synthetic approach not only controls the establishment of the ultrathin nanosheet structure for achieving high surface communication, but also incorporates F dopants to manipulate the electronic structure of the metalloporphyrin-like active sites (Ni-N-4). As a result, such catalyst with unique structural features exhibits a remarkable electrocatalytic performance for CO2-to-CO conversion with the Faradaic efficiency (FE) over 95 % in a wide potential range and an outstanding CO evolution rate of 1146 mmol g(cat)(-1) h(-1) at -0.97 V vs. RHE. The in situ attenuated total reflectioninfrared spectroscopy (ATR-IR) and theoretical calculations further demonstrate that the F-doping modulates the electron configuration of the central Ni-N-4 sites and thereby reduces the energy barrier for CO2 activation, which is favorable to the generation of the key *COOH intermediate.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available