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Curvature-Induced Electron Spin Catalysis with Carbon Spheres.
Qiao, Zirui; Cao, Huaqiang; Wang, Jiadao; Yang, Haijun; Yao, Wenqing; Wang, Jiaou; Cheetham, Anthony K.
Afiliación
  • Qiao Z; Tsinghua University, Chemistry, CHINA.
  • Cao H; Tsinghua University, Department of Chemistry, Zhongguancun Street, 100084, Beijing, CHINA.
  • Wang J; Tsinghua University, Department of Mechanical Engineering, CHINA.
  • Yang H; Tsinghua University, Chemistry, CHINA.
  • Yao W; Tsinghua University, Chemistry, CHINA.
  • Wang J; Chinese Academy of Sciences, Beijing Synchrotron Radiation Facility, Institute of Highly Energy Physics, CHINA.
  • Cheetham AK; University of California Santa Barbara, Materials Research Laboratory, UNITED STATES OF AMERICA.
Angew Chem Int Ed Engl ; : e202412745, 2024 Sep 01.
Article en En | MEDLINE | ID: mdl-39218803
ABSTRACT
Here, we report curvature-induced electron spin catalysis by using solid carbon spheres as catalysts, which were synthesized using positive curvature molecular hexabromocyclopentadiene as a precursor molecule, following a radical coupling mechanism. The curvature spin of carbon is regarded as an overlapping state of σ- and π-radical, which is identified by the inverse Laplace transform of pulse-electron paramagnetic resonance. The growth mechanism of carbon spheres abiding by Kroto's model, is supported by the density functional theory study of thermodynamics and kinetics calculations. The solid carbon spheres present excellent catalytic behaviour of oxidation coupling of amines to form corresponding imines with the conversion of >99%, selectivity of 98.7%, and yield of 97.7%, which is attributed to the predominantly curvature-induced electron spin catalysis of carbon, supported by the calculation of oxygen adsorption energy. This work proposes a view of curvature-induced spin catalysis of carbon, which opens up a research direction for curvature-induced electron spin catalysis.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania
Texto completo
Añadir a Mi BVS
Imprimir
XML
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania