Synthesis of dimethyl carbonate from CO2 and methanol over CeO2 nanoparticles/Co3O4 nanosheets
Synthesis of dimethyl carbonate from CO2 and methanol over CeO2 nanoparticles/Co3O4 nanosheets
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CeO2 纳米粒子/Co3O4 纳米片上 CO2 和甲醇合成碳酸二甲酯
DOI：
10.1016/j.fuel.2022.124945
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发表时间：
2022-10
期刊：
影响因子：
7.4
通讯作者：
Liu Zhao-Tie
中科院分区：
文献类型：
--
作者：
He Zhen-Hong;Sun Yong-Chang;Wei Yuan-Yuan;Wang Kuan;Wang Weitao;Chen Zhuo;Wang Zhong-Yu;Tian Yue;Liu Zhao-Tie
甲醇与二氧化碳的反应是利用二氧化碳资源和合成碳酸二甲酯（DMC）的理想途径，碳酸二甲酯是重要的燃料和燃料添加剂。本研究开发了Ce/Co摩尔比为3/7 （Ce3-NPs/Co7-NSs）的CeO2nanoparticles （CeO2NPs）负载在Co3O4nanosheets （Co3O4NSs）上的催化剂，可以有效催化该反应。DMC的生成活性和产率分别达到16.8 mmol·gcat-1·h -1和47.2%（以甲醇为基础），超过了目前报道的大多数催化剂，特别是在相对较低的120℃条件下。表征结果表明，Co3O4NSs能提高氧空位量和co2吸附量，但能降低甲醇吸附量。甲醇和co2之间的吸附平衡对反应至关重要，它们的原位红外光谱证实了催化剂可以同时激活co2和甲醇，反应涉及Langmuir-Hinshelwood （LH）机制。本文构建的co3o4纳米片负载ceo_2纳米颗粒催化剂为co3o4纳米片负载ceo_2纳米颗粒催化剂的制备提供了一种高效的co2和甲醇合成DMC催化剂，并为构建其他具有可调节co2和甲醇吸附能力的催化剂提供了重要参考。
The reaction of methanol and CO2is an ideal route for the utilization of CO2resources and the synthesis of dimethyl carbonate (DMC), which is an important fuel and fuel-additive. In this work, we developed a catalyst of CeO2nanoparticles (CeO2NPs) loaded on Co3O4nanosheets (Co3O4NSs) with the Ce/Co molar ratio of 3/7 (Ce3-NPs/Co7-NSs) which could efficiently catalyze the reaction. The formation activity and the yield of DMC reached 16.8 mmol·gcat-1·h−1and 47.2 % (based on methanol), surpassing most reported catalysts, especially at a relatively low temperature of 120 ℃. Characterization results indicated that the Co3O4NSs could enhance the amounts of oxygen vacancies and CO2adsorption but reduce methanol adsorption. The adsorption equilibrium between methanol and CO2is crucial for the titled reaction, and thein-situIR spectra confirmed that the catalyst could simultaneously activate CO2and methanol and the reaction involves a Langmuir-Hinshelwood (LH) mechanism. The present strategy for constructing a catalyst of CeO2nanoparticles loaded on Co3O4nanosheets provides an efficient catalyst for the DMC synthesis from CO2and methanol and offers an important reference in building other catalysts with adjustable adsorption capacities of CO2and methanol.