Fully Aromatic Fluorinated Polyamide Nanofilms with Molecular Gating for Ultrafast Crude Oil Fractionation.

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Jin-Bo Li,Chang Liu,Cheng-Ye Zhu,Jia-Hui Xin,Zhi Wang,Yu-Wei Liu,Chao Zhang,Hong-Qing Liang,Hao-Cheng Yang,Jian Wu,Zhi-Kang Xu
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Abstract

Crude oil is the "black gold" of the world and its fractionation by thermal distillation is a highly energy-consuming process. Polymer membranes are manifesting the potential in revolutionizing crude oil fractionation for developing energy-efficient, low-footprint petrochemical engineering. Nevertheless, conventional polymer membranes suffer from inferior fractionation performance with unsatisfied permeance and selectivity owing to their polar channel chemistry as well as low-connective and vulnerable channel architecture. We report a kind of robust, fully aromatic fluorinated polyamide (FAFPA) nanofilm that features a switchable molecular gating-on/gating-off state to activate and reconstruct sub-nanochannels for the permselectivity of hydrocarbon liquids, enabling ultrafast and stable crude oil fractionation. We demonstrate the gating-on state is launched by the interplay of FAFPA networks and polar-matched trigger molecules bearing α-H such as alcohols and ketones, redefining the sub-nanochannel chemistry and improving the spatial connectivity of sub-nanochannels to accelerate the selective transport of hydrocarbons. The gating-on FAFPA nanofilms show a record-high separation factor of 33 for 1,3,5-triisopropylbenzene with a molecular weight of 204 Da as well as a profound n-hexane permeance, 24-fold higher than that of the gating-off state. Moreover, these gating-on FAFPA nanofilms can stably handle typical black crude oil at an elevated temperature of 80 °C for garnering a 32-fold increased permeance while sustaining nearly constant selectivity toward hydrocarbons.
具有分子门控的全芳香族氟化聚酰胺纳米膜用于原油超快分馏。
原油是世界上的“黑金”,其热蒸馏分馏是一个高能耗的过程。聚合物膜在革新原油分馏、开发节能、低足迹的石化工程方面显示出潜力。然而,传统聚合物膜由于其极性通道化学以及低连接和脆弱的通道结构,导致其分选性能较差,渗透率和选择性不理想。我们报道了一种坚固的、全芳香族氟化聚酰胺(FAFPA)纳米膜,它具有可切换的分子门通/关状态,可以激活和重建亚纳米通道,用于碳氢化合物液体的准选择性,实现超快速和稳定的原油分选。我们证明了FAFPA网络和极性匹配的α-H触发分子(如醇类和酮类)的相互作用启动了门控状态,重新定义了亚纳米通道化学,提高了亚纳米通道的空间连通性,加速了碳氢化合物的选择性运输。门合FAFPA纳米膜对分子量为204 Da的1,3,5-三异丙苯的分离系数高达33,具有比关合状态高24倍的正己烷渗透率。此外,这些FAFPA纳米膜可以在80°C的高温下稳定地处理典型的黑色原油,获得32倍的渗透率,同时保持对碳氢化合物的几乎恒定的选择性。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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