A Highly Stable Anion-Functionalized Cage-like Framework for Efficient Separation of MTO Products under Harsh Conditions

IF 8.7 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2025-02-03 DOI:10.1021/acsmaterialslett.4c0238310.1021/acsmaterialslett.4c02383

Zhenyu Ji, Yunzhe Zhou, Yongqin Zhu, Yongyao Liu, Zhengyi Di*, Maochun Hong and Mingyan Wu*,

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引用次数: 0

Abstract

Separation of methanol-to-olefin products to obtain high-purity C₂H₄ and C₃H₆ has been deemed as one sustainable method for providing such indispensable industrial feedstocks. To meet the practical separation conditions, it is of critical significance to develop adsorbents that can separate C₃H₆/C₂H₄ under high-temperature and high-humidity conditions. Herein, we reported an anion-functionalized cage-like MOF (SIFSIX-Cu-TPA) showing a high-stability structure and huge distinction in C₃H₆ and C₂H₄ adsorption. Furthermore, C₃H₆- and C₂H₄-loaded single-crystal structures clearly reveal that more supramolecular interactions are generated between the C₃H₆ molecule and SIFSIX-Cu-TPA. Breakthrough experiments show that SIFSIX-Cu-TPA can efficiently separate C₃H₆/C₂H₄. After one separation cycle, 3.5 mol kg^–1 of high-purity C₂H₄ (>99.95%) and 2.5 mol kg^–1 of polymer-grade C₃H₆ (>99.5%) can be obtained from a C₃H₆/C₂H₄ (50/50) mixture at ₂98 K. More importantly, even at 338 K and 100% relative humidity, polymer-grade C₂H₄ (2.7 mol kg^–1) and C₃H₆ (1.4 mol kg^–1) can also be collected.

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在恶劣条件下高效分离MTO产物的高度稳定阴离子功能化笼状框架

将甲醇分离成烯烃产品以获得高纯度的 C2H4 和 C3H6 已被视为提供此类不可或缺的工业原料的一种可持续方法。为满足实际分离条件，开发能在高温高湿条件下分离 C3H6/C2H4 的吸附剂至关重要。在此，我们报告了一种阴离子官能化笼状 MOF（SIFSIX-Cu-TPA），它具有高稳定性结构，在吸附 C3H6 和 C2H4 方面具有巨大的差异。此外，C3H6 和 C2H4 负载单晶结构清楚地表明，C3H6 分子与 SIFSIX-Cu-TPA 之间产生了更多的超分子相互作用。突破性实验表明，SIFSIX-Cu-TPA 可以高效分离 C3H6/C2H4。更重要的是，即使在 338 K 和 100% 相对湿度条件下，也能收集到聚合物级 C2H4（2.7 mol kg-1）和 C3H6（1.4 mol kg-1）。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.