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发表于 2019-5-12 19:47:36
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化学学院张振杰研究员ANGEWANDTE,通讯作者:张振杰、Banglin Chen、Libo Li
Angew. Chem. Int. Ed., DOI:10.1002/anie.201904312, First published: 06 May 2019
https://onlinelibrary.wiley.com/doi/10.1002/anie.201904312
Robust Microporous Metal-Organic Frameworks for Highly Efficient and Simultaneous Removal of Propyne and Propadiene
from Propylene
Yun-Lei Peng,# [a] Chaohui He,# [c] Tony Pham,[g] Ting Wang,[a] Pengfei Li,[e] Rajamani Krishna,Katherine
A. Forrest,[g ] Adam Hogan,[g] Shanelle Suepaul,[g] Brian Space,[g] Ming Fang,[e] Yao Chen,[f] Michael J. Zaworotko,[h] Jinping Li,[c] Libo Li,* [b ], [c] Zhenjie Zhang,* [a], [d], [f] Peng Cheng,[a], [d]Banglin Chen* [b ]
[a] Y.-L. Peng, T. Wang, Prof. P. Cheng, Prof. Z. Zhang
College of Chemistry, Nankai University, Tianjin, 300071, P. R. China E-mail: zhangzhenjie nankai.edu.cn
[b ] Prof. L. Li, Prof. B. Chen
Department of Chemistry, University of Texas at San Antonio, One UTSA Circle, San Antonio, Texas 78249-0698, United States E-mail: banglin.chen utsa.edu
[c] C. He, Prof. J. Li, Prof. L. Li
College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan, 030024, Shanxi, P. R. China E-mail: lilibo908 hotmail.com,
[d] Prof. P. Cheng, Prof. Z. Zhang
Key Laboratory of Advanced Energy Materials Chemistry (MOE), Nankai University, Tianjin 300071, P. R. China
[e] P. Li, M. Fang
Department of Chemistry, Hebei Normal University of Science & Technology, Qinhuangdao, 066004, Hebei, China
[f] Prof. Y. Chen, Prof. Z. Zhang
State Key Laboratory of Medicinal Chemical Biology, Nankai University, Tianjin 300071, P. R. China.
[g] T. Pham, K. A. Forrest, A. Hogan, S. Suepaul, Prof. B. Space
Department of Chemistry, University of South Florida, 4202 East Fowler A venue, CHE205, Tampa, Florida 33620-5250, United States.
[h] Prof. M. J. Zaworotko
Department of Chemical Sciences, Bernal Institute, University of Limerick, Limerick V94T9PX, Republic of Ireland.
Prof. R. Krishna
Van't Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, The Netherlands.
[#] These authors contributed equally to this work.
Abstract
Simultaneous removal of trace amount of propyne and propadiene from propylene is an important but challenging industrial process. In this study, we reported a class of microporous metal‐organic frameworks (NKMOF‐1‐M) with exceptional water stability and remarkably high uptakes for both propyne and propadiene at low pressures. Attributed to the strong bind affinity to propyne and propadiene over propylene, NKMOF‐1‐M created new benchmark selectivities for ternary propyne/propadiene/propylene (0.5/0.5/99.0) mixture, and set as a unique MOF platform to achieve both the highest selectivity and productivity of polymer‐grade propylene (99.996%) at ambient temperature, verified by both simulated and experimental breakthrough results. Moreover, we demonstrated a rare example to visualize propyne and propadiene molecules in the single‐crystal structure of NKMOF‐1‐M through a convenient approach under ambient condition, which helped to precisely understand the binding sites and affinity of propyne and propadiene. These results provide important guidance on using ultramicroporous MOFs as physisorbent materials to resolve industrial challenges related to ternary propyne/propadiene/propylene mixture separation.
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