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Functionally Regulating the Oxygen Defects in High-Entropy Oxide Catalysts for Reverse Water-Gas Shift Conversion
Ke Wang1,2, Rui Zhang1,2, Meng Zhao1,2
1State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China.
Journal of the American Chemical Society
|May 20, 2026
Summary
Functional modulation of oxygen defects, not just quantity, significantly impacts catalyst performance for the reverse water-gas shift (RWGS) reaction. Chromium incorporation optimizes defect ratios in high-entropy oxides, enhancing CO2 conversion.
Area of Science:
- Catalysis
- Materials Science
- Surface Chemistry
Background:
- Oxygen defects are crucial for catalytic processes like the reverse water-gas shift (RWGS) reaction.
- Catalyst performance is traditionally linked to the quantity of oxygen defects.
Purpose of the Study:
- To investigate the functional modulation of oxygen defects beyond mere quantity adjustment.
- To explore the role of chromium (Cr) in tailoring high-entropy oxide (HEO) catalysts for RWGS.
Main Methods:
- Synthesis of spinel@rock salt core@shell high-entropy oxide (HEO) catalysts incorporating chromium.
- Characterization of oxygen defect types and their roles in CO2 adsorption and dissociation.
- Evaluation of catalytic performance for the RWGS reaction at 350 °C.
Main Results:
- A Cr-modified HEO catalyst achieved 28.9% CO2 conversion in the RWGS reaction, nearing thermodynamic equilibrium.
- Two distinct types of oxygen defects were identified, responsible for CO2 adsorption and dissociation.
- Chromium incorporation effectively optimized the ratio of these functional oxygen defects.
Conclusions:
- Functional modulation of oxygen defects is more critical than quantity for RWGS catalysis.
- Cr-engineered HEOs with optimized oxygen defect ratios show enhanced catalytic activity.
- This study provides insights into designing advanced catalysts by controlling defect functionality.
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