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Pr-Doped CeO2 Catalyst in the Prins Condensation–Hydrolysis Reaction: Are All of the Defect Sites Catalytically Active?
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-02-14 00:00:00 , DOI: 10.1021/acscatal.7b04500 Zhixin Zhang 1 , Yehong Wang 1 , Jianmin Lu 1 , Jian Zhang 1 , Mingrun Li 1 , Xuebin Liu 2 , Feng Wang 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-02-14 00:00:00 , DOI: 10.1021/acscatal.7b04500 Zhixin Zhang 1 , Yehong Wang 1 , Jianmin Lu 1 , Jian Zhang 1 , Mingrun Li 1 , Xuebin Liu 2 , Feng Wang 1
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Defect chemistries of metal-doped CeO2 catalysts have attracted extensive scientific interests in heterogeneous catalysis. Here, we report the structure–activity relationship of CeO2 catalysts doped by Pr. The Pr-doped CeO2 solid solution catalysts were prepared by a coprecipitation method and evaluated in Prins condensation–hydrolysis of isobutene with formalin to 3-methyl-1,3-butanediol. Raman and infrared (IR) spectroscopies were used to characterize the defect sites of the catalysts. Pr creates two kinds of defects in Pr-doped CeO2: oxygen vacancy and lattice distortion (Pr3+O8-type complex, which was confirmed by the Raman and XPS spectra), whose concentrations depend on the Pr doping amount. The relationship between defect properties (type and concentration) and their catalytic consequence is established. The catalytic performance significantly depends on the oxygen vacancy concentration in Pr-doped CeO2 catalysts. This study also shows that a Pr3+O8-type complex has little effect on the catalytic performance, indicating that the Pr3+O8-type complex is a spectator during the reaction. DFT calculations have indicated that the oxygen vacancy induced by the Pr dopant on a CeO2 surface promotes the adsorption of HCHO and inhibits the adsorption of isobutene, suggesting the condensation of HCHO and isobutene occurs via an Eley–Rideal (ER) mechanism.
中文翻译：
Prs缩合水解反应中的Pr掺杂CeO 2催化剂：所有缺陷位都具有催化活性吗？
金属掺杂的CeO 2催化剂的缺陷化学在非均相催化中引起了广泛的科学兴趣。在这里，我们报告了Pr掺杂的CeO 2催化剂的结构-活性关系。通过共沉淀法制备掺Pr的CeO 2固溶体催化剂，并在Prins缩合-异丁烯与福尔马林水解成3-甲基-1,3-丁二醇中进行了评估。拉曼光谱和红外光谱用于表征催化剂的缺陷部位。Pr在掺杂Pr的CeO 2中产生两种缺陷：氧空位和晶格畸变（Pr 3+ O 8-型配合物，通过拉曼光谱和XPS光谱证实），其浓度取决于Pr的掺杂量。建立缺陷性质（类型和浓度）与其催化结果之间的关系。催化性能很大程度上取决于掺Pr的CeO 2催化剂中的氧空位浓度。该研究还表明，Pr 3+ O 8型配合物对催化性能的影响很小，表明Pr 3+ O 8型配合物是反应过程中的旁观者。DFT计算表明，Pe掺杂剂在CeO 2上引起的氧空位 表面促进了HCHO的吸附并抑制了异丁烯的吸附，这表明HCHO和异丁烯的缩合是通过Eley-Rideal（ER）机理发生的。
更新日期：2018-02-14
中文翻译：
Prs缩合水解反应中的Pr掺杂CeO 2催化剂：所有缺陷位都具有催化活性吗？
金属掺杂的CeO 2催化剂的缺陷化学在非均相催化中引起了广泛的科学兴趣。在这里，我们报告了Pr掺杂的CeO 2催化剂的结构-活性关系。通过共沉淀法制备掺Pr的CeO 2固溶体催化剂，并在Prins缩合-异丁烯与福尔马林水解成3-甲基-1,3-丁二醇中进行了评估。拉曼光谱和红外光谱用于表征催化剂的缺陷部位。Pr在掺杂Pr的CeO 2中产生两种缺陷：氧空位和晶格畸变（Pr 3+ O 8-型配合物，通过拉曼光谱和XPS光谱证实），其浓度取决于Pr的掺杂量。建立缺陷性质（类型和浓度）与其催化结果之间的关系。催化性能很大程度上取决于掺Pr的CeO 2催化剂中的氧空位浓度。该研究还表明，Pr 3+ O 8型配合物对催化性能的影响很小，表明Pr 3+ O 8型配合物是反应过程中的旁观者。DFT计算表明，Pe掺杂剂在CeO 2上引起的氧空位 表面促进了HCHO的吸附并抑制了异丁烯的吸附，这表明HCHO和异丁烯的缩合是通过Eley-Rideal（ER）机理发生的。
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