MOF-derived Zr-doped Mn2O3 as a high-performance catalyst for CO2 conversion to ethylene urea
摘要
The conversion of carbon dioxide (CO2) into high-value chemicals is crucial for mitigating greenhouse emissions and achieving sustainable carbon cycles. This study presented a series of Zr-doped MOF-derived Mn2O3 catalysts (xZr-MnBP), synthesized via an aqueous solution process using trimesic acid and polyvinylpyrrolidone as ligands, followed by zirconium incorporation. The catalysts were thoroughly characterized by XRD, TG, TEM, CO2/NH3-TPD, FTIR, and XPS and applied in the synthesis of ethylene urea (EU) from CO2 and ethylenediamine (EDA). Among them, the 10Zr-MnBP catalyst, with 10 wt% Zr doping, demonstrated superior performance with 93% conversion of EDA and 75% selectivity of EU under mild conditions (60 ℃, 1 min). Characterization indicated that optimal Zr doping promoted surface oxygen vacancies, increased Mn3+ species, and balanced acid–base sites, which synergistically enhanced CO2 adsorption and activation. Kinetic studies further confirmed a lower activation energy consistent with the improved activity. Moreover, 10Zr-MnBP demonstrated excellent stability over five reaction cycles with negligible efficiency decay. This work offers an effective Mn-based catalyst for CO2 valorization and provides insights into designing efficient systems for sustainable chemical synthesis.