Fluorine-free synthesis of all-silica STT zeolite membranes for H2/CH4 separation

Fluorine-free synthesis of all-silica STT zeolite membranes for H2/CH4 separation
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无氟合成用于H2/CH4分离的全硅STT沸石膜

DOI:
10.1016/j.cej.2021.133567
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发表时间:
2021-11
影响因子:
15.1
通讯作者:
Xuehong Gu
Xuehong Gu
中科院分区:
工程技术1区
文献类型:
--
作者:
Tao Zhou;Mengyang Shi;Lingjie Chen;Chao Gong;Ping Zhang;Jixian Xie;Xuerui Wang;Xuehong Gu

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氢气(H2)是最有前途的化石能源零排放的CO2替代品。然而,焦化过程中副产的H2通常作为燃料燃烧。焦炉煤气中的氢气作为清洁能源的回收利用是一个迫切的需求。本文以无氟前驱体为原料制备了全硅STT分子筛膜,用于分离H2/CH 4。在高温下,结晶周期缩短了75%。水热合成2d后,在0.2MPa、298 K下,膜的H2渗透率达到2.8 × 10− 8 mol·m−2·s−1·Pa− 1,H2/CH 4选择性达到49.6。更重要的是,STT分子筛膜是抵抗CO和H2S,这应该被阻止进料到商业聚合物和Pd膜。该膜在含100 ppm H2S的63 H2:28 CH 4:7 CO:2 C2 H6的模拟焦炉煤气中稳定336 h。这将为沸石膜分离氢气的实际应用铺平道路。
Hydrogen (H2) is the most promising alternative to fossil energy for zero-emission of CO2. However, the by-produced H2from coking process was generally burned as fuel. It is highly desired to recycle the H2from coke oven gas as the clean energy resource. Herein all-silica STT zeolite membranes were prepared from the fluorine-free precursor for H2/CH4separation. The crystallization period was shortened by 75% at the elevated temperature. After hydrothermal synthesis of 2 days, the membrane showed H2permeance up to 2.8 × 10−8mol·m−2·s−1·Pa−1and H2/CH4selectivity up to 49.6 at 0.2 MPa and 298 K. More importantly, STT zeolite membrane was resistant to CO and H2S, which should be prevented from feeding to the commercial polymeric and Pd membranes. The membrane was stable up to 336 h in the simulated coke oven gas of 63 H2: 28 CH4: 7 CO: 2 C2H6containing 100 ppm H2S. This would pave the way of zeolite membranes to H2separation in practical applications.
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