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Title: Dinitrogen Reduction by a Chromium(0) Complex Supported by a 16-membered Phosphorus Macrocycle

An unexpected reaction leading to the synthesis and characterization of two Cr-N2 complexes supported by cyclic phosphorus macrocycles that contain pendant amine bases. Reactivity with acid produced hydrazine and ammonia, illustrating the first example of N2 reduction by a "Chatt-type" chromium dinitrogen complex. Computational analysis examined the initial N2 protonation steps, highlighting the thermodynamically preferred Cr products involved in N2 reduction. This material is based upon work supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences. Pacific Northwest National Laboratory is operated by Battelle for DOE.
Authors:
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Publication Date:
OSTI Identifier:
1091468
Report Number(s):
PNNL-SA-95191
KC0307010
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of the American Chemical Society, 135(31):11493-11496
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
Chromium; N2 reduction; proton relays; ammonia