The formation of methanol from glycerol bio-waste over doped ceria-based catalysts.
The formation of methanol from glycerol bio-waste over doped ceria-based catalysts.
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在掺杂二氧化铈基催化剂上从甘油生物废物形成甲醇。
DOI：
10.1098/rsta.2020.0059
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发表时间：
2020
期刊：
影响因子：
--
通讯作者：
Devlia J
中科院分区：
文献类型：
--
作者：
Devlia J
通过共沉淀制备了一系列二氧化铈基固溶体金属氧化物，并作为甘油裂解（主要是甲醇）的催化剂进行了评估。根据催化剂的还原性研究了催化剂活性和甲醇选择性。制备、煅烧包含Ce-Pr和Ce-Zr的氧化物并与CeO2、Pr6O11和ZrO2进行比较。通过拉曼光谱测量分析和程序升温还原、氧化和还原循环来检查催化剂的储氧能力。正如拉曼光谱所证明的，Pr 的掺入导致了显着的缺陷。该材料作为甘油到甲醇反应的催化剂进行了评估，发现增加缺陷密度或还原性是有益的。 CeO2 上甲醇的时空产率标准化为表面积为 0.052 mmolMeOHm−2h−1，而 CeZrO2 和 CePrO2 上的甲醇时空产率分别为 0.029 和 0.076 mmolMeOHm−2h−1。掺入Pr减少了表面积；然而，对甲醇和乙二醇的碳摩尔选择性仍然相对较高，这表明与二氧化铈相比，反应途径发生了转变。本文是讨论会议问题“科学促进循环经济”的一部分。
A series of ceria-based solid solution metal oxides were prepared by co-precipitation and evaluated as catalysts for glycerol cleavage, principally to methanol. The catalyst activity and selectivity to methanol were investigated with respect to the reducibility of the catalysts. Oxides comprising Ce-Pr and Ce-Zr were prepared, calcined and compared to CeO2, Pr6O11and ZrO2. The oxygen storage capacity of the catalysts was examined with analysis of Raman spectroscopic measurements and a temperature programmed reduction, oxidation and reduction cycle. The incorporation of Pr resulted in significant defects, as evidenced by Raman spectroscopy. The materials were evaluated as catalysts for the glycerol to methanol reaction, and it was found that an increased defect density or reducibility was beneficial. The space–time yield of methanol normalized to surface area over CeO2was found to be 0.052 mmolMeOHm−2h−1, and over CeZrO2and CePrO2, this was to 0.029 and 0.076 mmolMeOHm−2h−1, respectively. The inclusion of Pr reduced the surface area; however, the carbon mole selectivity to methanol and ethylene glycol remained relatively high, suggesting a shift in the reaction pathway compared to that over ceria.This article is part of a discussion meeting issue ‘Science to enable the circular economy'.