American Chemical Society

Microscopic-Level Insights into the Mechanism of Enhanced NH3 Synthesis in Plasma-Enabled Cascade N2 Oxidation–Electroreduction System

Posted on 2022-05-19 - 07:04
Integrated/cascade plasma-enabled N2 oxidation and electrocatalytic NOx (where x = 2, 3) reduction reaction (pNOR-eNOxRR) holds great promise for the renewable synthesis of ammonia (NH3). However, the corresponding activated effects and process of plasma toward N2 and O2 molecules and the mechanism of eNOxRR to NH3 are unclear and need to be further uncovered, which largely limits the large-scale deployment of this process integration technology. Herein, we systematically investigate the plasma-enabled activation and recombination processes of N2 and O2 molecules, and more meaningfully, the mechanism of eNOxRR at a microscopic level is also decoupled using copper (Cu) nanoparticles as a representative electrocatalyst. The concentration of produced NOx in the pNOR system is confirmed as a function of the length for spark discharge as well as the volumetric ratio for N2 and O2 feeding gas. The successive protonation process of NOx and the key N-containing intermediates (e.g., −NH2) of eNOxRR are detected with in situ infrared spectroscopy. Besides, in situ Raman spectroscopy further reveals the dynamic reconstruction process of Cu nanoparticles during the eNOxRR process. The Cu nanoparticle-driven pNOR-eNOxRR system can finally achieve a high NH3 yield rate of ∼40 nmol s–1 cm–2 and Faradaic efficiency of nearly 90%, overperforming the benchmarks reported in the literature. It is anticipated that this work will stimulate the practical development of the pNOR-eNOxRR system for the green electrosynthesis of NH3 directly from air and water under ambient conditions.


3 Biotech
3D Printing in Medicine
3D Research
3D-Printed Materials and Systems
AAPG Bulletin
AAPS PharmSciTech
Abhandlungen aus dem Mathematischen Seminar der Universität Hamburg
ABI Technik (German)
Academic Medicine
Academic Pediatrics
Academic Psychiatry
Academic Questions
Academy of Management Discoveries
Academy of Management Journal
Academy of Management Learning and Education
Academy of Management Perspectives
Academy of Management Proceedings
Academy of Management Review
Select your citation style and then place your mouse over the citation text to select it.


need help?