Jimenez-Martin Jose M, Orozco-Saumell Ana, Hernando Héctor, Linares María, Mariscal Rafael, López Granados Manuel, García Alicia, Iglesias Jose
Chemical & Environmental Engineering Group, Universidad Rey Juan Carlos, C/ Tulipan s/n, 28933 Madrid, Spain.
Energy and Sustainable Chemistry (EQS) Group, Institute of Catalysis and Petrochemistry, CSIC, C/ Marie Curie 2, Campus de Cantoblanco, 28049 Madrid, Spain.
ACS Sustain Chem Eng. 2022 Jul 11;10(27):8885-8896. doi: 10.1021/acssuschemeng.2c01987. Epub 2022 Jun 28.
Sn-USY materials have been prepared through an optimized post-synthetic catalytic metalation procedure. These zeolites displayed, upon ion exchange with alkaline metals, an outstanding activity in the direct transformation of glucose into methyl lactate, yielding more than 70% of the starting glucose as the target product, and an overall combined retro-aldol condensation product yield above 95% in a short reaction time (<4 h). This outstanding catalytic performance is ascribed to the neutralization of Brønsted acid sites, the consequent depression of side reactions, and a higher population of tin open sites in the ion-exchanged Sn-USY zeolites. Reusability tests evidenced some loss of catalytic activity, partially caused by the closing of tin sites, although the use of small amounts of water in the reaction media demonstrated that this deactivation mechanism can be, at least, partially alleviated.
通过优化的合成后催化金属化程序制备了Sn-USY材料。这些沸石在与碱金属进行离子交换后,在将葡萄糖直接转化为乳酸甲酯的反应中表现出出色的活性,以目标产物形式生成的起始葡萄糖超过70%,并且在短反应时间(<4小时)内总的逆羟醛缩合产物产率高于95%。这种出色的催化性能归因于布朗斯特酸位点的中和、随之而来的副反应抑制以及离子交换后的Sn-USY沸石中更多的锡开放位点。可重复使用性测试证明了催化活性有所损失,部分原因是锡位点的封闭,尽管在反应介质中使用少量水表明这种失活机制至少可以部分缓解。