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MICROPOROUS AND MESOPOROUS MATERIALS · 2021 · IF 5.455

Steam-assisted synthesis of SAPO-34@ZSM-5 core-shell zeolite for enhancing the synergies of n-hexane-Methanol Co-Reaction to light olefins

Qitong Cheng,Benxian Shen,Jichang Liu,Hui Sun,Di Wu,Lei Jiang,Peikun Yan,Xin Pu,Suhui Ou,Jigang Zhao

An alternative and promising route for the production of light olefins which realizes the objective of effective resource usage is the coupling conversion of n -hexane-methanol. The SAPO-34@ZSM-5 core-shell composite has been designed and fabricated by the steam-assisted crystallization (SAC) method for boosting the n -hexane-methanol synergies. SAC avoids the undesired phase transformation/dissolution of SAPO-34 caused by exposure to harsh basic conditions of the ZSM-5 precursor solution. In comparison with the nanosized ZSM-5 or physical mixture, the SAPO-34@ZSM-5 core-shell zeolite demonstrates a 32–38 wt% increase in the light olefin selectivity, a 28–67 wt% increase in the n -hexane conversion, and an 89–143% improvement in the catalyst lifetime under identical reaction conditions. With the aid of GC-MS analysis of carbonaceous deposits in spent catalysts, higher polymethylbenzenes concentration and lower polycyclic aromatic hydrocarbon (PHA) concentration are obtained from the extracted species of spent SAPO-34@ZSM-5 in comparison with that of other samples, which suggests the aromatic-based route to light olefins is enhanced and the carbonaceous deposition is slowed down. The core-shell configuration of the SAPO-34@ZSM-5 composite diminishes the diffusion rate of methanol towards the SAPO-34 core layer and increases the coupling of n -hexane derivatives with methanol in the hydrocarbon pool (HCP) route. The decreased number of acidic sites on the external surface of the SAPO-34 core layer may also be accounted for the inhibited carbon deposition.

研究领域: 化学工程 · 催化 · 材料科学
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