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Remarkable active-site dependent H2O promoting effect in CO oxidation.
Shu Zhao1,2, Fang Chen3, Sibin Duan4
1Department of Chemistry and Key Laboratory of Organic Optoelectronics & Molecular Engineering of the Ministry of Education, Tsinghua University, 100084, Beijing, China.
Nature Communications
|August 25, 2019
Summary
Single-atom catalysts (SACs) show enhanced CO oxidation activity, significantly boosted by water. This water-promoted effect makes gold SACs far more active than traditional nanocatalysts and commercial catalysts.
Area of Science:
- Heterogeneous catalysis
- Materials science
- Surface chemistry
Background:
- Interfacial sites on supported metal catalysts are crucial for performance.
- Single-atom catalysts (SACs) maximize atom-support interfacial sites.
- The catalytic properties of single-atom sites versus nanocatalyst interfacial sites remain unclear.
Purpose of the Study:
- To investigate the active-site dependent catalytic performance of supported gold single atoms and nanoparticles.
- To compare the effect of water on CO oxidation over gold single-atom sites and nanoparticle interfacial sites.
- To elucidate the mechanism behind water's promotion of CO oxidation on gold SACs.
Main Methods:
- Synthesis and characterization of supported gold single atoms and nanoparticles.
- Experimental evaluation of CO oxidation activity over different gold catalysts.
- Theoretical studies (e.g., DFT calculations) to understand reaction mechanisms.
Main Results:
- CO oxidation on gold single-atom sites is dramatically promoted by water.
- The promoting effect of water on gold nanoparticle interfacial sites is significantly weaker.
- Gold SACs exhibit two orders of magnitude higher activity than commercial three-way catalysts due to water's influence.
- Theoretical studies reveal water facilitates a CO + OH reaction channel on SACs.
Conclusions:
- Catalytic performance is dependent on the nature of the active site (single atom vs. nanoparticle).
- Water plays a critical role in enhancing CO oxidation over gold SACs via a unique reaction pathway.
- Gold SACs represent a highly active catalyst for CO oxidation, surpassing conventional catalysts.
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