摘要
针对CO_(2)和甲醇绿色合成碳酸二甲酯路线进行热力学计算分析。在反应压力0.1—8.0 MPa和反应温度293.15—473.15 K分别研究反应温度和反应压力对吉布斯自由能Δ_(r)G、平衡常数K和平衡转化率C的影响。在此基础上,以CeO_(2)为催化剂分别固定反应压力8.0 MPa或反应温度413.15 K,在不同反应温度或压力下进行反应,并将实验结果与热力学计算结果进行对比。结果表明:CeO_(2)在反应温度为373.15—473.15 K内表现出良好的催化性能,增大反应压力可以有效降低Δ_(r)G,并提高K和C,促进反应正向进行。此外,热力学计算结果显示,较低温度不同反应压力条件下,增加反应压力对反应平衡常数的增大更显著,且为开发高活性催化材料在较低温下催化CO_(2)和甲醇高效合成碳酸二甲酯提供理论参考。
The green synthesis process of dimethyl carbonate from CO_(2) and methanol was researched with thermodynamic calculation.The effects of reaction temperature and pressure on Gibbs free energy Δ_rG,equilibrium constant K and equilibrium conversion rate C were studied in the range of 0.1-8.0 MPa and 293.15-473.15 K.Furthermore,the effects of temperatures and pressures on the reaction performance were investigated by using CeO_(2) as the catalyst at a fixed reaction pressure of 8.0 MPa or a reaction temperature of 413.15 K,and the obtained results were compared with the results of thermodynamic calculations.The results show that CeO_(2) gives a good performance in the range of 373.15-473.15 K,and the increase of reaction pressure can reduce Δ_(rG) and increase K and C,promoting the reaction in the positive direction.In addition,thermodynamic calculations show that the reaction pressure displays a more significant effect on the equilibrium constant under the condition of lower reaction temperature with different reaction pressure,and provides a theoretical reference for the development of highly active catalytic materials to catalyze the efficient synthesis of dimethyl carbonate from CO_(2) and methanol at lower temperatures.
作者
李建国
贾爱忠
薛伟
赵新强
王延吉
LI Jianguo;JIA Aizhong;XUE Wei;ZHAO Xinqiang;WANG Yanji(School of Chemical Engineering,Hebei University of Technology,Tianjin 300130,China)
出处
《化学工程》
CSCD
北大核心
2024年第1期54-58,共5页
Chemical Engineering(China)
基金
中央引导地方科技发展资金项目(216Z3701G)
河北省自然科学基金资助项目(B2022202034)
天津市自然科学基金资助项目(15JCYBJC2100)。
