低极化率氮吸附点用于N2/CH4分离

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Dr. Feifei Zhang, Zhiwei Zhao, Yating Wang, Xiaomin Li, Xiaowei Bai, Mengyue Lu, Yanjie Wang, Dr. Xiaoqing Wang, Prof. Libo Li, Prof. Jinping Li, Prof. Jiangfeng Yang
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引用次数: 0

摘要

由于其相似的尺寸和物理化学性质,从CH4中选择性吸附N2是一种具有工业前景但具有挑战性的方法。在此,我们报告了一个坚固的金属有机框架(Cu‐MFU‐4l),具有低极化率的开放Cu(I)位点,用于基准的N2/CH4分离。通过X射线吸收光谱(XAS)、原位CO吸附红外光谱和X射线光电子能谱(XPS)证实了框架中开放Cu(I)位点的存在。气体吸附等温线显示,Cu‐MFU‐4l对N2和CH4的吸收率存在显著差异,导致其具有较高的N2/CH4吸收率(1.94)和动力学选择性(2.20),其中N2/CH4吸收率是迄今报道的mof中最高的。突破性实验证实,Cu‐MFU‐4l是迄今为止报道的用于二元N2/CH4分离的最佳多孔吸附剂,具有创纪录的高突破选择性(2.43)和CH4产率(0.47 mmol g−1)。通过一步分离过程,可以从三元甚至六组分CH4混合物中获得高纯度的CH4(99.99%)。原位红外光谱和计算模型研究表明,开放的Cu(I)位点可以更好地区分N2和CH4。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Nitrogen Adsorption Sites with Low Polarizability for Benchmark N2/CH4 Separation

Nitrogen Adsorption Sites with Low Polarizability for Benchmark N2/CH4 Separation

Selective adsorption of N2 from CH4 is an industrially promising but challenging process given their similar sizes and physicochemical properties. Herein, we report a robust metal-organic framework (Cu-MFU-4l) featuring open Cu(I) sites of low polarizability for benchmark N2/CH4 separation. The presence of open Cu(I) sites in the framework was confirmed by X-ray absorption spectroscopy (XAS), in situ CO-adsorbed infrared spectroscopy, and X-ray photoelectron spectroscopy (XPS). Gas sorption isotherms revealed that Cu-MFU-4l exhibited a significant difference between N2 and CH4 uptakes, resulting in a high N2/CH4 uptake ratio (1.94) and kinetic selectivity (2.20), of which the N2/CH4 uptake ratio was the highest among all MOFs reported to date. Breakthrough experiments confirmed Cu-MFU-4l as the best porous adsorbent hitherto reported for binary N2/CH4 separation, based on the record-high breakthrough selectivity (2.43) and CH4 productivity (0.47 mmol g−1). High-purity CH4 (99.99%) could also be obtained from ternary and even six-component CH4 mixtures by a one-step separation process. In situ infrared spectroscopy and computational modeling studies revealed that the open Cu(I) sites could better distinguish N2 and CH4.

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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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