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 CO2 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.
The Influence of a Changing Local Environment during Photoinduced CO2 Dissociation
Maestri M.;
2021-01-01
Abstract
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 CO2 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.File | Dimensione | Formato | |
---|---|---|---|
Angew Chem Int Ed - 2021 - Vyshnepolsky - The Influence of a Changing Local Environment during Photoinduced CO2.pdf
accesso aperto
:
Publisher’s version
Dimensione
1.45 MB
Formato
Adobe PDF
|
1.45 MB | Adobe PDF | Visualizza/Apri |
I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.