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Operando Mobile Catalysis for Reverse Water Gas Shift Reaction.
Haojie Liang1,2,3, Bin Zhang1,2, Mei Hong1,2
1State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, 030001, Taiyuan, China.
Angewandte Chemie (International Ed. in English)
|January 25, 2024
Summary
Introducing operando mobile catalysis, where mobile platinum (Pt) single atoms on ceria (CeO2) enhance catalytic efficiency. This approach converts inert intermediates, significantly boosting performance in the reverse water gas shift reaction.
Area of Science:
- Heterogeneous catalysis
- Surface chemistry
- Materials science
Background:
- Metal atoms on supports are active sites in heterogeneous catalysts.
- Traditionally, active sites and adsorbed intermediates are considered static, limiting reactivity.
- Intermediates distant from active sites often remain untransformed.
Purpose of the Study:
- To introduce and demonstrate operando mobile catalysis for enhanced catalytic efficiency.
- To enable the transformation of inert intermediates on catalyst supports.
- To improve the collision probability between active sites and reactants/intermediates.
Main Methods:
- Utilizing ligand-coordinated platinum (Pt) single atoms on ceria (CeO2).
- Inducing the transformation of isolated MeCpPt- species into mobile MeCpPt(H)CO complexes during reaction.
- Investigating the reverse water gas shift (RWGS) reaction under operando conditions.
Main Results:
- Achieved a turnover frequency (TOF) of 6358 mol CO2 mol_Pt^-1 h^-1.
- Obtained 99% CO selectivity at 300°C for the RWGS reaction.
- Demonstrated the conversion of inert carbonate intermediates on the CeO2 support.
Conclusions:
- Operando mobile catalysis significantly enhances catalytic efficiency by increasing reactant-site proximity.
- This strategy successfully converts inert carbonate intermediates, overcoming a key limitation in heterogeneous catalysis.
- Mobile Pt single atoms on CeO2 offer a promising platform for designing highly efficient catalysts for various applications.
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