Evidence map›Paper›PMID 39365853›Full record

ArticleScience advances2024

High pressure-derived nonsymmetrical [Cu

Peter E VanNatta, Cynthia M Archambault, Sicheng Wang, Tengteng Lyu, Jack D'Amelio, Noah J Martell, Scott K Watson, Kunyu Wang, Zhenxian Liu, Matthew T Kieber-Emmons and 1 more

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Article in Science advances, 2024. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.

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1 · What the graph read from it

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2 · The registry

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3 · Its place in the literature

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4 · The record

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5 · Who and what money

Authors and funding

11 authors.

Peter E VanNattaDepartment of Chemistry, University of North Texas, Denton, TX 76205, USA.ORCID 0000-0003-1360-579X
Cynthia M ArchambaultDepartment of Chemistry, University of North Texas, Denton, TX 76205, USA.ORCID 0000-0002-2514-7688
Sicheng WangDepartment of Chemistry, University of North Texas, Denton, TX 76205, USA.ORCID 0000-0002-5224-5697
Tengteng LyuDepartment of Chemistry, University of North Texas, Denton, TX 76205, USA.
Jack D'AmelioDepartment of Chemistry, University of Illinois at Urbana-Champaign, Urbana, IL 61801, USA.
Noah J MartellDepartment of Chemistry, Iowa State University, Ames, IA 50011, USA.ORCID 0000-0002-0158-5501
Scott K WatsonDepartment of Chemistry, University of North Texas, Denton, TX 76205, USA.ORCID 0009-0000-2626-3691
Kunyu WangDepartment of Chemistry, Texas A&M University, College Station, TX 77843, USA.ORCID 0000-0001-8982-0547
Zhenxian LiuDepartment of Physics, University of Illinois Chicago, Chicago, IL 60607, USA.ORCID 0000-0003-2617-7077
Matthew T Kieber-EmmonsDepartment of Chemistry, Cedar Crest College, Allentown, PA 18104, USA.
Hao YanDepartment of Chemistry, University of North Texas, Denton, TX 76205, USA.ORCID 0000-0003-1545-1659

Funding

No grant is acknowledged in the PubMed record.

6 · The paper itself

Abstract

Nonsymmetrical oxygen-bridged binuclear copper centers have been proposed and modeled as intermediates and transition states in several C─H oxidation pathways, leading to the postulation that structural dissymmetry enhances the reactivity of the bridging oxygen. However, experimentally characterizing the structure and reactivity of these transient species is remarkably challenging. Here, we report the high-pressure synthesis of a metastable nonsymmetrical dicopper-μ-oxo compound with exceptional reactivity toward the mono-oxygenation of aliphatic C─H bonds. The nonequivalent coordination environment of copper stabilizes localized mixed valency and greatly enhances the hydrogen atom abstraction activity of the bridging oxygen, enabling room-temperature hydroxylation of methane under pressure. These findings highlight the role of dissymmetry in the reactivity of binuclear copper centers and demonstrate precise control of molecular structures by mechanical means.

Identifiers

PMID39365853
PMCPMC11451512

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