English
 
User Manual Privacy Policy Disclaimer Contact us
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

The Mechanism of Interfacial CO2 Activation on Al Doped Cu/ZnO

MPS-Authors
/persons/resource/persons84554

Heenemann,  Maria
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons126976

Millet,  Marie-Mathilde
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21557

Girgsdies,  Frank
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22071

Schlögl,  Robert
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;
Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

/persons/resource/persons135780

Jones,  Travis
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons104933

Frei,  Elias
Inorganic Chemistry, Fritz Haber Institute, Max Planck Society;

External Ressource
No external resources are shared
Fulltext (public)

acscatal.0c00574.pdf
(Publisher version), 2MB

Supplementary Material (public)
There is no public supplementary material available
Citation

Heenemann, M., Millet, M.-M., Girgsdies, F., Eichelbaum, M., Risse, T., Schlögl, R., et al. (2020). The Mechanism of Interfacial CO2 Activation on Al Doped Cu/ZnO. ACS Catalysis, 10, 5672-5680. doi:10.1021/acscatal.0c00574.


Cite as: http://hdl.handle.net/21.11116/0000-0006-581B-A
Abstract
We report on a combined quantitative charge carrier and catalytic activity analysis of Cu/ZnO model catalysts. The promoting effect of Al3+ on the ZnO support for CO2 activation via the reverse water-gas-shift reaction has been investigated. To the best of our knowledge, this is the first time that contact-free and operando microwave Hall Effect technique is applied to measure charge carriers in Cu/ZnO based model catalysts under reverse water-gas shift reaction conditions. This method allows us to monitor the electrical conductivity, charge carrier mobility, and absolute number of charge carriers. An increase in charge carrier concentration with increasing Al3+ content and its direct correlation with the catalytic activity for CO formation is found. We conclude that the increased availability of charge carriers plays a key role in CO2 activation and CO formation, which finds additional support in a concurrent decrease of the apparent activation energy and increase in the reaction order of CO2. In combination with comprehensive DFT calculations, the impact of the interfacial charge transfer, coupled to oxygen defect sites in ZnO and CO2 adsorption properties, is elucidated and highlighted. In conclusion, the results from this operando investigation combined with DFT calculations demonstrate the importance of charge transfer processes as decisive descriptors for understanding and explaining catalytic properties.