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<p>This study proposes a simple method for tailoring the morphology and activity of cerium oxide (CeO<sub>2</sub>) catalysts in converting carbon dioxide (CO<sub>2</sub>) and methanol to green organic carbonate, dimethyl carbonate (DMC), to utilize and reduce CO<sub>2</sub> emissions. CeO<sub>2</sub> was prepared by urea precipitation at 85, 105, and 125 °C for 2 h, then calcining at 600 °C for 2 h. The phase structure and morphology of CeO<sub>2</sub> correlated with the urea hydrolysis rate. A low degree of supersaturation at 85 °C led to heterogeneous precipitation of cerium oxycarbonate (Ce<sub>2</sub>O(CO<sub>3</sub>)<sub>2</sub>.H<sub>2</sub>O) and CeO<sub>2</sub> with spherical morphology, while a higher degree of supersaturation at 105 °C and 125 °C resulted in homogeneous precipitation of single-phase Ce<sub>2</sub>O(CO<sub>3</sub>)<sub>2</sub>.H<sub>2</sub>O with spindle and elongated octahedral morphology, respectively. The spindle-shaped CeO<sub>2</sub> prepared at 105&#xa0;°C with a predominant surface (111) facet showed the highest catalytic activity, with a DMC yield of 18.81&#xa0;mmol.g<sub>cat</sub><sup>−1</sup>. The enhanced catalytic efficiency of spindle-shaped CeO<sub>2</sub> was due to the high concentration of surface-active defect sites of exposed cerium cations and oxygen vacancies, which optimized the number of acid–base sites in adsorbing and activating CO<sub>2</sub> and methanol to produce DMC.</p> Graphical abstract <p></p>

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Correlation of urea precipitation temperature with phase formation, morphology, and catalytic activity for CO2 conversion of CeO2

  • 期刊论文

  • 发表日期：

    2025年6月11日

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  • Panpailin Seeharaj,
  • Jenjira Duangtanon,
  • Chanakan Sreemueang,
  • Phetchphalin Noppharat,
  • Tachatad Kulthananat,
  • Naratip Vittayakorn,
  • Sira Srinives,
  • Pattaraporn Kim-Lohsoontorn

摘要

This study proposes a simple method for tailoring the morphology and activity of cerium oxide (CeO2) catalysts in converting carbon dioxide (CO2) and methanol to green organic carbonate, dimethyl carbonate (DMC), to utilize and reduce CO2 emissions. CeO2 was prepared by urea precipitation at 85, 105, and 125 °C for 2 h, then calcining at 600 °C for 2 h. The phase structure and morphology of CeO2 correlated with the urea hydrolysis rate. A low degree of supersaturation at 85 °C led to heterogeneous precipitation of cerium oxycarbonate (Ce2O(CO3)2.H2O) and CeO2 with spherical morphology, while a higher degree of supersaturation at 105 °C and 125 °C resulted in homogeneous precipitation of single-phase Ce2O(CO3)2.H2O with spindle and elongated octahedral morphology, respectively. The spindle-shaped CeO2 prepared at 105 °C with a predominant surface (111) facet showed the highest catalytic activity, with a DMC yield of 18.81 mmol.gcat−1. The enhanced catalytic efficiency of spindle-shaped CeO2 was due to the high concentration of surface-active defect sites of exposed cerium cations and oxygen vacancies, which optimized the number of acid–base sites in adsorbing and activating CO2 and methanol to produce DMC.

Graphical abstract