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Lifetime improvement in methanol-to-olefins catalysis over chabazite materials by high-pressure H 2 co-feeds
Nature Catalysis ( IF 42.8 ) Pub Date : 2018-08-24 , DOI: 10.1038/s41929-018-0125-2
Sukaran S. Arora , Davy L. S. Nieskens , Andrzej Malek , Aditya Bhan

Mitigating catalyst deactivation in the industrially deployed process of methanol-to-olefins conversion over HSAPO-34 is a critical challenge. Here, we demonstrate that lifetime in methanol-to-olefins catalysis over HSAPO-34 at sub-complete methanol conversion, as determined by the cumulative turnover capacity per Brønsted acid site towards hydrocarbon products in the effluent before complete catalyst deactivation (~15% carbon final conversion), can be enhanced with increasing efficacy (~2.8× to >70×) by co-feeding H2 at increasing partial pressures (400–3,000 kPa) in the influent with methanol compared with co-feeding helium at equivalent pressures. The lifetime improvement in the presence of high-pressure H2 co-feeds is observed to be more prominent at complete methanol conversion than at sub-complete conversion. The improvements in catalyst lifetime by co-feeding H2 are rendered without any deleterious effects on C2–C4 olefins selectivity, which remains ~85% carbon irrespective of the inlet H2 pressure. These observations can be rationalized based on the participation of H2 in hydrogen transfer reactions, and in effect, the interception of pathways that promote the formation of deactivation-inducing polycyclic species.



中文翻译:

通过高压H 2共进料,在菱沸石材料上催化甲醇制烯烃的使用寿命得到改善

在通过HSAPO-34进行的甲醇制烯烃转化的工业应用过程中,减轻催化剂失活是一项严峻的挑战。在这里,我们证明了在不完全甲醇转化时,HSAPO-34在甲醇制烯烃催化中的寿命,这取决于每个布朗斯台德酸位点对催化剂完全失活之前废水中烃类产物的累积周转能力(〜15%碳)。与在相同压力下共同进料氦气相比,通过在甲醇中增加分压(400–3,000 kPa)下共同进料H 2可以提高功效(〜2.8倍至> 70倍),从而提高效率。高压H 2存在下的寿命提高观察到在甲醇完全转化时,共进料比在亚完全转化时更重要。通过共同进料H 2可以提高催化剂寿命,而对C 2 -C 4烯烃的选择性没有任何有害影响,无论入口H 2压力如何,C 2 -C 4烯烃的选择性都保持在〜85%左右。这些观察结果可以基于H 2参与氢转移反应而得到合理化,实际上可以基于促进促进失活诱导多环物质形成的途径的截获。

更新日期:2018-08-26
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