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The Influence of a Changing Local Environment during Photoinduced CO 2 Dissociation
Author(s) -
Vyshnepolsky Michael,
Ding ZhaoBin,
Srivastava Prashant,
Tesarik Patrik,
Mazhar Hussain,
Maestri Matteo,
Morgenstern Karina
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202105468
Subject(s) - dissociation (chemistry) , chemistry , catalysis , molecule , reactivity (psychology) , photochemistry , nanoscopic scale , limiting , reaction rate , photodissociation , chemical physics , nanotechnology , materials science , organic chemistry , medicine , mechanical engineering , alternative medicine , pathology , engineering
Though largely influencing the efficiency of a reaction, the molecular‐scale details of the local environment of the reactants are experimentally inaccessible hindering an in‐depth understanding of a catalyst's reactivity, a prerequisite to maximizing its efficiency. We introduce a method to follow individual molecules and their largely changing environment during a photochemical reaction. The method is illustrated for a rate‐limiting step in a photolytic reaction, the dissociation of CO 2 on two catalytically relevant surfaces, Ag(100) and Cu(111). We reveal with a single‐molecule resolution how the reactant's surroundings evolve with progressing laser illumination and with it their propensity for dissociation. Counteracting processes lead to a volcano‐like reactivity. Our unprecedented local view during a photoinduced reaction opens the avenue for understanding the influence of the products on reaction yields on the nanoscale.