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Catalytic Nitrous Oxide Degradation with Group 15 Clusters

Abstract:
Nitrous oxide (N2O) is sometimes referred to as the forgotten greenhouse gas, but ignoring it would be a mistake. N2O has a greenhouse warming potential 300× that of CO2, and anthropogenic emissions are increasing. Yet, compared to CO2, homogeneous catalysts that mediate its reduction are scarce. We present a range of cluster catalysts based on abundant and inexpensive p-block elements that mediate the conversion of N2O to environmentally benign N2. The catalysts studied offer many critical advantages, and systems can be tuned for performance, recyclability, selectivity, air stability, and commercial availability. Pnictogen clusters present themselves as a general platform in N2O reduction chemistry, and control reactions confirm that these clusters offer access to reactivity that simple monopnictogen molecules do not. Mechanistic investigations reveal that the low-valent clusters can access a –1/+1 redox couple, which goes beyond classical main group redox couples and will unlock a vault of hitherto unknown chemical space.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1021/jacs.5c09618

Authors


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Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry
Role:
Author
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry
Role:
Author
More by this author
Role:
Author
ORCID:
0000-0003-0293-5742
More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Chemistry
Role:
Author
ORCID:
0000-0002-6833-5574


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Funder identifier:
https://ror.org/00k4n6c32
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Funder identifier:
https://ror.org/027m9bs27
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Funder identifier:
https://ror.org/052gg0110
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Funder identifier:
https://ror.org/001aqnf71


Publisher:
American Chemical Society
Journal:
Journal of the American Chemical Society More from this journal
Volume:
147
Issue:
33
Pages:
30317-30325
Publication date:
2025-08-06
Acceptance date:
2025-07-28
DOI:
EISSN:
1520-5126
ISSN:
0002-7863


Language:
English
Source identifiers:
3219404
Deposit date:
2025-08-21
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