What is it about?
We report how phase engineering of MoS2 significantly improves the selectivity for nitrite reduction to nitrous oxide, a critical process in biological denitrification, using continuous-wave and pulsed electron paramagnetic resonance spectroscopy. We reveal that metallic 1T-MoS2 has a protonation site with a pKa of ∼5.5, where the proton is located ∼3.26 Å from redox-active Mo site. This protonation site is unique to 1T-MoS2 and induces sequential proton−electron transfer which inhibits ammonium formation while promoting nitrous oxide production, as confirmed by the pH-dependent selectivity and deuterium kinetic isotope effect.
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Why is it important?
Molybdenum sulfide (MoS2) is the most widely studied transition-metal dichalcogenide (TMDs) and phase engineering can markedly improve its electrocatalytic activity. However, the selectivity toward desired products remains poorly explored, limiting its application in complex chemical reactions.
Perspectives
This is atomic-scale evidence of phase-dependent selectivity on MoS2, expanding the application of TMDs to selective electrocatalysis.
Dr. Daoping He
Shanghai Jiao Tong University
Read the Original
This page is a summary of: Atomic-scale evidence for highly selective electrocatalytic N−N coupling on metallic MoS
2, Proceedings of the National Academy of Sciences, November 2020, Proceedings of the National Academy of Sciences,
DOI: 10.1073/pnas.2008429117.
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