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用于CH₄/N₂选择性分离的自支撑超微孔碳纳米片

Self-Pillared Ultramicroporous Carbon Nanoplates for Selective Separation of CH /N.

作者信息

Xu Shuang, Li Wen-Cui, Wang Cheng-Tong, Tang Lei, Hao Guang-Ping, Lu An-Hui

机构信息

State Key Laboratory of Fine Chemicals, Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2021 Mar 15;60(12):6339-6343. doi: 10.1002/anie.202014231. Epub 2021 Feb 2.

Abstract

There is growing evidence that pillaring up a densely packed ultramicroporous two-dimensional (2D) structure is an effective strategy to reduce their internal diffusion. Reliable pillaring paradigms, however, is rather challenging. Here we report a one-pot multi-component sequential assembly method for the preparation of a new self-pillared 2D polymer and ultramicroporous carbon with integrated surface protrusions. The molecular level pillaring process is surprisingly fast, that is, in 10 min. The thickness of nanoplate edge and the density (roughness), angle as well as height of protrusions can be precisely tuned. Exemplified in coal bed methane purification/separation, this unique pillared 2D carbons exhibit a CH /N selectivity up to 24 at a low CH partial pressure and two orders of magnitude faster CH diffusion kinetics than the commercial carbon molecular sieves. This solution synthesis methodology is generalizable for creation and fine tuning of pillared 2D heterostructures.

摘要

越来越多的证据表明,支撑紧密堆积的超微孔二维(2D)结构是减少其内部扩散的有效策略。然而,可靠的支撑模式颇具挑战性。在此,我们报告了一种一锅多组分顺序组装方法,用于制备具有集成表面突起的新型自支撑二维聚合物和超微孔碳。分子水平的支撑过程出奇地快,即在10分钟内即可完成。纳米板边缘的厚度以及突起的密度(粗糙度)、角度和高度均可精确调节。以煤层气净化/分离为例,这种独特的支撑二维碳在低CH分压下表现出高达24的CH₄/N₂选择性,且CH₄扩散动力学比商业碳分子筛快两个数量级。这种溶液合成方法可推广用于支撑二维异质结构的创建和精细调控。

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