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Atomic-scale evidence for highly selective electrocatalytic N-N coupling on metallic MoS2
- Title
- Atomic-scale evidence for highly selective electrocatalytic N-N coupling on metallic MoS2
- Authors
- He, Daoping; Ooka, Hideshi; Kim, Yujeong; Li, Yamei; Jin, Fangming; Kim, Sun Hee; Nakamura, Ryuhei
- Ewha Authors
- 김선희
- SCOPUS Author ID
- 김선희
- Issue Date
- 2020
- Journal Title
- PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
- ISSN
- 0027-8424
- Citation
- PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA vol. 117, no. 50, pp. 31631 - 31638
- Keywords
- denitrification; ENDOR spectroscopy; molybdenum sulfide; phase transitions; electrochemistry
- Publisher
- NATL ACAD SCIENCES
- Indexed
- SCIE; SCOPUS
- Document Type
- Article
- Abstract
- 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. Here 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 pK(a) of similar to 5.5, where the proton is located similar to 3.26 angstrom 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. This is atomic-scale evidence of phase-dependent selectivity on MoS2, expanding the application of TMDs to selective electrocatalysis.
- DOI
- 10.1073/pnas.2008429117
- Appears in Collections:
- 자연과학대학 > 화학·나노과학전공 > Journal papers
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