Quantifying the Contribution of Hot Electrons in Photothermal Catalysis: A Case Study of Ammonia Synthesis over Carbon-supported Ru Catalyst.
Angew Chem Int Ed Engl
; 62(25): e202304452, 2023 Jun 19.
Article
em En
| MEDLINE
| ID: mdl-37083180
Photothermal catalysis is one of the most promising green catalytic technologies, while distinguishing the effects of hot electrons and local heating remains challenging. Herein, we reported that the actual reaction temperature of photothermal ammonia synthesis over carbon-supported Ru catalyst can be measured based on Le Chatelier's principle, enabling the hot-electron contribution to be quantified. By excluding local heating effects, we established that the activation energy via photothermal catalysis was much lower than that of thermocatalysis (54.9 vs. 126.0â
kJ mol-1 ), stemming from hot-electron injection lowering the energy barriers for both N2 dissociation and intermediates hydrogenation. Furthermore, hot-electron injection acted to suppress carbon support methanation, giving the catalyst outstanding operational stability over 1000â
h. This work provides new insights into the hot-electron effects in ammonia synthesis, guiding the design of high-performance photothermal catalysts.
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Texto completo:
1
Base de dados:
MEDLINE
Assunto principal:
Rutênio
/
Carbono
Idioma:
En
Revista:
Angew Chem Int Ed Engl
Ano de publicação:
2023
Tipo de documento:
Article
País de afiliação:
China