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Oxygen Vacancy Promoting Dimethyl Carbonate Synthesis from CO2 and Methanol over Zr-Doped CeO2 Nanorods
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-10-01 00:00:00 , DOI: 10.1021/acscatal.8b00415 Bin Liu 1 , Congming Li 1 , Guoqiang Zhang 1 , Xuesi Yao 2 , Steven S. C. Chuang 2 , Zhong Li 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-10-01 00:00:00 , DOI: 10.1021/acscatal.8b00415 Bin Liu 1 , Congming Li 1 , Guoqiang Zhang 1 , Xuesi Yao 2 , Steven S. C. Chuang 2 , Zhong Li 1
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The synthesis of dimethyl carbonate (DMC) from CO2 and methanol by Zr-doped CeO2 nanorods with different ratios of Zr/Ce has been studied at 6.8 MPa and 140 °C. The catalysts were characterized extensively by TEM, XRD, N2 adsorption, Raman spectroscopy, UV–vis spectroscopy, XPS, CO2-TPD, and in situ FTIR techniques. Doping of Zr atoms into the ceria lattice produced a fluorite-like solid solution, promoting the formation of oxygen vacancy sites. Zr-doped CeO2 nanorods exhibited significantly more oxygen vacancy sites than pure CeO2 nanorods. Zr0.1Ce nanorods which exhibited DMC synthesis activity also possess the highest concentration of oxygen vacancy sites. In situ FTIR studies further revealed that CO2 can adsorb on the oxygen vacancy to form bidentate carbonate and as intermediate to participate in the reaction. This study presents a strategy to design a high-efficiency CeO2-based catalysts by controlling the concentration of the surface oxygen vacancies.
中文翻译：
Zr掺杂CeO 2纳米棒上氧空位促进CO 2和甲醇合成碳酸二甲酯
研究了在6.8 MPa和140°C条件下，用Zr / Ce比例不同的掺Zr的CeO 2纳米棒从CO 2和甲醇合成碳酸二甲酯（DMC）的过程。通过TEM，XRD，N 2吸附，拉曼光谱，UV可见光谱，XPS，CO 2 -TPD和原位FTIR技术对催化剂进行了广泛的表征。将Zr原子掺杂到二氧化铈晶格中会产生萤石状固溶体，从而促进了氧空位的形成。掺Zr的CeO 2纳米棒比纯CeO 2纳米棒具有更多的氧空位。锆0.1表现出DMC合成活性的Ce纳米棒也具有最高浓度的氧空位。原位FTIR研究进一步表明，CO 2可以吸附在氧空位上以形成双齿碳酸盐，并作为中间体参与反应。这项研究提出了一种通过控制表面氧空位浓度来设计高效CeO 2基催化剂的策略。
更新日期：2018-10-01
中文翻译：
Zr掺杂CeO 2纳米棒上氧空位促进CO 2和甲醇合成碳酸二甲酯
研究了在6.8 MPa和140°C条件下，用Zr / Ce比例不同的掺Zr的CeO 2纳米棒从CO 2和甲醇合成碳酸二甲酯（DMC）的过程。通过TEM，XRD，N 2吸附，拉曼光谱，UV可见光谱，XPS，CO 2 -TPD和原位FTIR技术对催化剂进行了广泛的表征。将Zr原子掺杂到二氧化铈晶格中会产生萤石状固溶体，从而促进了氧空位的形成。掺Zr的CeO 2纳米棒比纯CeO 2纳米棒具有更多的氧空位。锆0.1表现出DMC合成活性的Ce纳米棒也具有最高浓度的氧空位。原位FTIR研究进一步表明，CO 2可以吸附在氧空位上以形成双齿碳酸盐，并作为中间体参与反应。这项研究提出了一种通过控制表面氧空位浓度来设计高效CeO 2基催化剂的策略。
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