Directed transforming of coke to active intermediates in methanol-to-olefins catalyst to boost light olefins selectivity.
Directed transforming of coke to active intermediates in methanol-to-olefins catalyst to boost light olefins selectivity.
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DOI：
10.1038/s41467-020-20193-1
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发表时间：
2021-01-04
影响因子：
16.6
通讯作者：
Liu Z
中科院分区：
文献类型：
--
作者：
Zhou J;Gao M;Zhang J;Liu W;Zhang T;Li H;Xu Z;Ye M;Liu Z
甲醇制烯烃（MTO）是从非油原料（煤、天然气、生物质、CO2等）生产乙烯和丙烯的最重要的催化工艺，由于焦炭沉积导致的催化剂快速失活而阻碍。恢复催化剂活性的常规做法，即通过空气燃烧或蒸汽气化除去焦炭，可避免地消除有利于轻质烯烃形成的活性烃池物质（HCP）。密度泛函理论计算和结构照明显微镜显示，萘阳离子，活性HCP提高乙烯的生产，是在SAPO-34沸石在高温下高度稳定。在这里，我们展示了一种通过蒸汽裂解将焦炭直接转化为SAPO-34沸石中的萘物种的策略。流化床反应器-再生器中试实验表明，在类似工业的连续操作下，MTO反应中实现了85%的出乎意料的高轻质烯烃选择性，其中88%的有价值的CO和H2以及可忽略的CO2作为再生副产物。这一策略显著提高了MTO工艺的经济性和可持续性。由于焦炭沉积导致的催化剂快速失活阻碍了甲醇制烯烃。在这里，作者展示了一种直接将焦炭转化为活性中间体的方法，以同时恢复催化剂活性并提高轻质烯烃选择性。
Methanol-to-olefins (MTO), the most important catalytic process producing ethylene and propylene from non-oil feedstocks (coal, natural gas, biomass, CO2, etc.), is hindered by rapid catalyst deactivation due to coke deposition. Common practice to recover catalyst activity, i.e. removing coke via air combustion or steam gasification, unavoidably eliminates the active hydrocarbon pool species (HCPs) favoring light olefins formation. Density functional theory calculations and structured illumination microscopy reveal that naphthalenic cations, active HCPs enhancing ethylene production, are highly stable within SAPO-34 zeolites at high temperature. Here, we demonstrate a strategy of directly transforming coke to naphthalenic species in SAPO-34 zeolites via steam cracking. Fluidized bed reactor-regenerator pilot experiments show that an unexpectedly high light olefins selectivity of 85% is achieved in MTO reaction with 88% valuable CO and H2 and negligible CO2 as byproducts from regeneration under industrial-alike continuous operations. This strategy significantly boosts the economics and sustainability of MTO process. Methanol-to-olefins is hindered by rapid catalyst deactivation due to coke deposition. Here the authors demonstrate an approach of directly transforming coke to active intermediates to simultaneously recover catalyst activity and boost light olefins selectivity.
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