Iron-Doped MoO3 Nanosheets for Boosting Nitrogen Fixation to Ammonia at Ambient Conditions
- 8 February 2021
- journal article
- research article
- Published by American Chemical Society (ACS) in ACS Applied Materials & Interfaces
- Vol. 13 (6), 7142-7151
- https://doi.org/10.1021/acsami.0c19644
Abstract
Nitrogen can be electrochemically reduced to produce ammonia, which supplies an energy-saving and environmental-benign route at room temperature, but high-efficiency catalysts are sought to reduce the reaction barrier. Here, iron-doped alpha-MoO3 nanosheets are thus designed and proposed as potential catalysts for fixing N-2 to NH3. The alpha-MoO3 band structure is intentionally modulated by the iron doping, which narrows the band gap of alpha-MoO3 and turns the semiconductor into a metal-like catalyst. Oxygen vacancies, generated by substituting Mo6+ for Fe3+ anions, are beneficial for nitrogen adsorption at the active sites. In 0.1 M Na2SO4, the Fe-doped MoO3 catalyst reached a high faradaic efficiency of 13.3% and an excellent NH3 yield rate of 28.52 mu g h(-1) mg(cat)(-1) at -0.7 V versus reversible hydrogen electrode, superior to most of the other metal-based catalysts. Theoretical calculations confirmed that the N2 reduction reaction at the Fe-MoO3 surface followed the distal reaction path.Keywords
Funding Information
- National Natural Science Foundation of China (51702039)
This publication has 45 references indexed in Scilit:
- Ammonia Electrosynthesis with High Selectivity under Ambient Conditions via a Li+ Incorporation StrategyJournal of the American Chemical Society, 2017
- Challenges in reduction of dinitrogen by proton and electron transferChemical Society Reviews, 2014
- Mechanistic aspects of dinitrogen cleavage and hydrogenation to produce ammonia in catalysis and organometallic chemistry: relevance of metal hydride bonds and dihydrogenChemical Society Reviews, 2013
- Fe2(MoO4)3 as an Effective Photo-Fenton-like Catalyst for the Degradation of Anionic and Cationic Dyes in a Wide pH RangeIndustrial & Engineering Chemistry Research, 2013
- Nitrogen Cycle ElectrocatalysisChemical Reviews, 2009
- Indirect, Reversible High-Density Hydrogen Storage in Compact Metal Ammine SaltsJournal of the American Chemical Society, 2008
- Ammonia Synthesis from First-Principles CalculationsScience, 2005
- Catalytic reduction of molecular nitrogen in solutionsRussian Chemical Bulletin, 2003
- Catalytic Synthesis of Ammonia—A “Never‐Ending Story”?Angewandte Chemie, 2003
- Ionization Potential, Electron Affinity, Electronegativity, Hardness, and Electron Excitation Energy: Molecular Properties from Density Functional Theory Orbital EnergiesThe Journal of Physical Chemistry A, 2003