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Title: Design and reactivity of pentapyridyl metal complexes for ammonia oxidation

Abstract

Oxidation of NH3 to N2 by pentapyridyl metal complexes via hydrogen atom abstraction was investigated computationally. Quantum chemical analysis reveals insights on orbital symmetry requirements for efficient NH3 oxidation. The most promising complex, [(PY5)Mo(NH3)]2+, was studied experimentally. It shows conversion of NH3 to N2 upon treatment with 2,4,6-tri-tertbutylphenoxyl radical.

Authors:
 [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1]
  1. BATTELLE (PACIFIC NW LAB)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Molecular Electrocatalysis (CME); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1526032
Report Number(s):
PNNL-SA-141391
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Chemical Communications
Additional Journal Information:
Journal Volume: 55; Journal Issue: 35
Country of Publication:
United States
Language:
English

Citation Formats

Johnson, Samantha JI, Heins, Spencer P., Klug, Christina, Wiedner, Eric S., Bullock, Ronald M., and Raugei, Simone. Design and reactivity of pentapyridyl metal complexes for ammonia oxidation. United States: N. p., 2019. Web. doi:10.1039/C9CC01249D.
Johnson, Samantha JI, Heins, Spencer P., Klug, Christina, Wiedner, Eric S., Bullock, Ronald M., & Raugei, Simone. Design and reactivity of pentapyridyl metal complexes for ammonia oxidation. United States. doi:10.1039/C9CC01249D.
Johnson, Samantha JI, Heins, Spencer P., Klug, Christina, Wiedner, Eric S., Bullock, Ronald M., and Raugei, Simone. Tue . "Design and reactivity of pentapyridyl metal complexes for ammonia oxidation". United States. doi:10.1039/C9CC01249D.
@article{osti_1526032,
title = {Design and reactivity of pentapyridyl metal complexes for ammonia oxidation},
author = {Johnson, Samantha JI and Heins, Spencer P. and Klug, Christina and Wiedner, Eric S. and Bullock, Ronald M. and Raugei, Simone},
abstractNote = {Oxidation of NH3 to N2 by pentapyridyl metal complexes via hydrogen atom abstraction was investigated computationally. Quantum chemical analysis reveals insights on orbital symmetry requirements for efficient NH3 oxidation. The most promising complex, [(PY5)Mo(NH3)]2+, was studied experimentally. It shows conversion of NH3 to N2 upon treatment with 2,4,6-tri-tertbutylphenoxyl radical.},
doi = {10.1039/C9CC01249D},
journal = {Chemical Communications},
number = 35,
volume = 55,
place = {United States},
year = {2019},
month = {5}
}

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