Journal
NATURE CATALYSIS
Volume 1, Issue 9, Pages 666-672Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41929-018-0125-2
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Funding
- Dow Chemical Company
- National Science Foundation [CBET 1701534]
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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 Bronsted acid site towards hydrocarbon products in the effluent before complete catalyst deactivation (similar to 15% carbon final conversion), can be enhanced with increasing efficacy (similar to 2.8x to >70x) by co-feeding H-2 at increasing partial pressures (400-3,000 kPa) in the influent with methanol compared with cofeeding helium at equivalent pressures. The lifetime improvement in the presence of high-pressure H-2 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 H-2 are rendered without any deleterious effects on C-2-C(4 )olefins selectivity, which remains similar to 85% carbon irrespective of the inlet H-2 pressure. These observations can be rationalized based on the participation of H-2 in hydrogen transfer reactions, and in effect, the interception of pathways that promote the formation of deactivation-inducing polycyclic species.
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