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TiO2-Doped CeO2 Nanorod Catalyst for Direct Conversion of CO2 and CH3OH to Dimethyl Carbonate: Catalytic Performance and Kinetic Study
ACS Omega ( IF 3.7 ) Pub Date : 2018-01-08 00:00:00 , DOI: 10.1021/acsomega.7b01475 Zhongwei Fu 1 , Yunyun Zhong 1 , Yuehong Yu 1 , Lizhen Long 1 , Min Xiao 1 , Dongmei Han 1 , Shuanjin Wang 1 , Yuezhong Meng 1
ACS Omega ( IF 3.7 ) Pub Date : 2018-01-08 00:00:00 , DOI: 10.1021/acsomega.7b01475 Zhongwei Fu 1 , Yunyun Zhong 1 , Yuehong Yu 1 , Lizhen Long 1 , Min Xiao 1 , Dongmei Han 1 , Shuanjin Wang 1 , Yuezhong Meng 1
Affiliation
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A new class of TiO2-doped CeO2 nanorods was synthesized via a modified hydrothermal method, and these nanorods were first used as catalysts for the direct synthesis of dimethyl carbonate (DMC) from CO2 and CH3OH in a fixed-bed reactor. The micromorphologies and physical–chemical properties of nanorods were characterized by transmission electron microscopy, X-ray diffraction, N2 adsorption, inductively coupled plasma atomic emission spectrometry, X-ray photoelectron spectroscopy, and temperature-programmed desorption of ammonia and carbon dioxide (NH3-TPD and CO2-TPD). The effects of the TiO2 doping ratio on the catalytic performances were fully investigated. By doping TiO2, the surface acid–base sites of CeO2 nanorods can be obviously promoted and the catalytic activity can be raised evidently. Ti0.04Ce0.96O2 nanorod catalysts exhibited remarkably high activity with a methanol conversion of 5.38% with DMC selectivity of 83.1%. Furthermore, kinetic and mechanistic investigations based on the initial rate method were conducted. Over the Ti0.04Ce0.96O2 nanorod catalyst, the apparent activation energy of the reaction was 46.3 kJ/mol. The reaction rate law was determined to be of positive first-order to the CO2 concentration and the catalyst loading amount. These results were practically identical with the prediction of the Langmuir–Hinshelwood mechanism in which the steps of CO2 adsorption and activation are considered as rate-determining steps.
中文翻译：
TiO 2掺杂的CeO 2纳米棒催化CO 2和CH 3 OH直接转化为碳酸二甲酯的催化性能和动力学研究
通过改进的水热法合成了一类新型的TiO 2掺杂CeO 2纳米棒，这些纳米棒首先被用作固定床反应器中由CO 2和CH 3 OH直接合成碳酸二甲酯（DMC）的催化剂。通过透射电子显微镜，X射线衍射，N 2吸附，电感耦合等离子体原子发射光谱，X射线光电子能谱以及程序升温程序解吸的氨和二氧化碳（NH）表征了纳米棒的微观形貌和理化性质。3- TPD和CO 2 -TPD）。TiO 2的作用充分研究了掺杂比对催化剂性能的影响。通过掺杂TiO 2，可以明显促进CeO 2纳米棒的表面酸碱位，并可以明显提高催化活性。Ti 0.04 Ce 0.96 O 2纳米棒催化剂表现出显着的高活性，甲醇转化率为5.38％，DMC选择性为83.1％。此外，还进行了基于初始速率法的动力学和力学研究。在Ti 0.04 Ce 0.96 O 2纳米棒催化剂上，反应的表观活化能为46.3 kJ / mol。反应速率定律被确定为对CO呈正一阶2浓度和催化剂的负载量。这些结果实际上与Langmuir–Hinshelwood机理的预测相同，在该机理中，CO 2吸附和活化步骤被视为决定速率的步骤。
更新日期：2018-01-08
中文翻译：
TiO 2掺杂的CeO 2纳米棒催化CO 2和CH 3 OH直接转化为碳酸二甲酯的催化性能和动力学研究
通过改进的水热法合成了一类新型的TiO 2掺杂CeO 2纳米棒，这些纳米棒首先被用作固定床反应器中由CO 2和CH 3 OH直接合成碳酸二甲酯（DMC）的催化剂。通过透射电子显微镜，X射线衍射，N 2吸附，电感耦合等离子体原子发射光谱，X射线光电子能谱以及程序升温程序解吸的氨和二氧化碳（NH）表征了纳米棒的微观形貌和理化性质。3- TPD和CO 2 -TPD）。TiO 2的作用充分研究了掺杂比对催化剂性能的影响。通过掺杂TiO 2，可以明显促进CeO 2纳米棒的表面酸碱位，并可以明显提高催化活性。Ti 0.04 Ce 0.96 O 2纳米棒催化剂表现出显着的高活性，甲醇转化率为5.38％，DMC选择性为83.1％。此外，还进行了基于初始速率法的动力学和力学研究。在Ti 0.04 Ce 0.96 O 2纳米棒催化剂上，反应的表观活化能为46.3 kJ / mol。反应速率定律被确定为对CO呈正一阶2浓度和催化剂的负载量。这些结果实际上与Langmuir–Hinshelwood机理的预测相同，在该机理中，CO 2吸附和活化步骤被视为决定速率的步骤。
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