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Hot‐Electron‐Induced Photothermal Catalysis for Energy‐Dependent Molecular Oxygen Activation
Author(s) -
Zhang Wei,
Chen Yu,
Zhang Gong,
Tan Xiao,
Ji Qinghua,
Wang Zhaowu,
Liu Huijuan,
Qu Jiuhui
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202012306
Subject(s) - electron , photothermal therapy , photochemistry , chemistry , catalysis , chemical physics , oxygen , activation energy , homo/lumo , electron transport chain , electron donor , atomic physics , nanotechnology , materials science , molecule , physics , organic chemistry , biochemistry , quantum mechanics
Hot electrons activate reactants and reduce the activation energy barrier ( E a ) of a reaction through electron donation. However, a comprehensive understanding of the intrinsic driving force of this electron‐donating effect is lacking, let alone the precise manipulation of electron donation processes. Herein, the essential and promotional role of hot electron energy on the electron‐donating effect was elucidated using molecular oxygen activation (MOA) as a model reaction. Through providing an available electron source to the conventional photo‐thermal conversion system, the high energy carried by hot electrons was liberated and greatly enhanced the electron donation towards the LUMO (π*) orbit of O 2 . The energy was also transferred to O 2 and elevated the potential energy surface (PES) of MOA, which was reflected by the enhanced formation of superoxide oxygen anions. As predicted, the E a of MOA decreased by 45.1 % and exhibited a substantial light dependence, demonstrating that MOA became energy‐efficient due to improved exploitation and conversion of photon energies.