Order–disorder hybrid high-entropy Co–Cu-Fe–Mn–Ce oxides for photothermal CO2 hydrogenation†
Abstract
CO2 is a waste gas but also a crucial C1 resource. Thus, the chemical conversion of CO2 is significant for reducing its concentration in the air and mitigating its negative impacts on the environment. High-entropy oxides (HEOs) have recently attracted significant attention, especially in catalysis. In the present work, we developed high-entropy Co–Cu–Mn–Fe–Ce oxides via a simple sol–gel method combined with a calcination temperature control strategy, and the prepared samples were applied in photothermal catalytic hydrogenation of CO2 to CO. The calcination temperature during the preparation of the catalyst significantly influenced its structure, resulting in different photoelectronic properties, CO2/H2 adsorption properties, and catalytic performances. Among the prepared samples, CoCuMnFeCeOx calcinated at 500 °C, denoted as CoCuMnFeCeOx(500), delivered high performance with a highest activity of 110 mmol gcat−1 h−1 and a selectivity of 99.4%. Thus, the prepared high-entropy oxides have excellent catalytic activity and facilitate the conversion of CO2. In situ DRIFTS and DFT calculations confirmed that the reaction generates a *COOH intermediate in the synthesis of the CO product, and the rate-determining step is related to the formation of *COOH from CO2. The present work provides a promising approach for constructing efficient catalysts for CO2 utilization and sheds light on developing a strategy for enhancing the catalytic efficiency of HEO samples.