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Single-Atom 3d Transition Metals on SnO2 as Model Cell for Conversion Mechanism: Revealing Thermodynamic Catalytic Effects on Enhanced Na Storage of Heterostructures.
Xie, Minggang; Zhang, Zhe; Cheng, Zheng; He, Jinghan; Shen, Zhili; Zeng, Jianrong; Chen, Xiao-Bo; Li, Chunguang; Shi, Zhan; Feng, Shouhua.
Afiliación
  • Xie M; State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130015, P. R. China.
  • Zhang Z; State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130015, P. R. China.
  • Cheng Z; State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130015, P. R. China.
  • He J; State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130015, P. R. China.
  • Shen Z; State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, 130015, P. R. China.
  • Zeng J; Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, P. R. China.
  • Chen XB; Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, P. R. China.
  • Li C; School of Engineering, RMIT University, Carlton, VIC 3053, Australia.
  • Shi Z; State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130015, P. R. China.
  • Feng S; State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130015, P. R. China.
Angew Chem Int Ed Engl ; : e202410734, 2024 Jul 03.
Article en En | MEDLINE | ID: mdl-38958047
ABSTRACT
Since the discovery in 2000, conversion-type materials have emerged as a promising negative-electrode candidate for next-generation batteries with high capacity and tunable voltage, limited by low reversibility and severe voltage hysteresis. Heterogeneous construction stands out as a cost-effective and efficient approach to reducing reaction barriers and enhancing energy density. However, the second term introduced by conventional heterostructure inevitably complicates the electrochemical analysis and poses great challenges to harvesting systematic insights and theoretical guidance. A model cell is designed and established herein for the conversion reactions between Na and TMSA-SnO2, where TMSA-SnO2 represents single atom modification of eight different 3d transition elements (V, Cr, Mn, Fe, Co, Ni, Cu or Zn). Such a model unit fundamentally eliminates the interference from the second phase and thus enables independent exploration of activation manifestations of the heterogeneous architecture. For the first time, a thermodynamically dependent catalytic effect is proposed and verified through statistical data analysis. The mechanism behind the unveiled catalytic effect is further elucidated by which the active d orbitals of transition metals weaken the surface covalent bonds and lower the reaction barriers. This research provides both theoretical insights and practical demonstrations of the advanced heterogeneous electrodes.
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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 Pais de publicación: Alemania

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2024 Tipo del documento: Article Pais de publicación: Alemania