Accelerated Dinitrogen Electroreduction to Ammonia via Interfacial Polarization Triggered by Single-Atom Protrusions

By Jie Li, Shang Chen, Fengjiao Quan, Guangming Zhan, Falong Jia, Zhihui Ai, Lizhi Zhang. Chem, 2020

239 citations recorded by the source corpus.

Summary Electrocatalytic N2 reduction reaction (NRR) offers a promising low-energy, sustainable ammonia-synthesizing alternative to Haber-Bosch reaction. One roadblock lying in access to high-performance ammonia electrosynthesis emanates from the unsatisfied ability of electrocatalysts to wreck N≡N bond. Here, we report that interfacial polarization is an efficient scenario to enhance N≡N fracture to boost electrocatalytic ammonia synthesis. As a proof-of-concept demonstration, protrusion-shaped Fe single-atom catalysts immobilized onto MoS2 nanosheets engender electric fields to polarize N2. The resultant interfacial polarization fields between Fe-MoS2 and N2 drive the injection of more electrons into N2 antibonding orbitals in a fast manner, leading to a superior ammonia-evolving rate (36.1 ± 3.6 mmol g−1 h−1 or 97.5 ± 6 μg h−1 cm−2) at low applied potential. Similar phenomena are applicable in Co-MoS2, Cu-MoS2, Rh-MoS2, or Ru-MoS2, suggesting the potential universality of our interfacial polarization concept in upgrading wide-scope catalysis.

Subfields: Catalysis, Computer Networks and Communications, Renewable Energy, Sustainability and the Environment

View Paper: https://www.semanticscholar.org/paper/a2144f193657ba8bd20757b479ee7077e79e3c66