In situ studies of molecular copper compounds for highly selective purification of ethylene

Peter W. Stephens, Rasika H. V. Dias, Andrey A. Yakovenko
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Abstract

Purification of ethylene from ethylene -ethane mixtures is an important and challenging industrial process, currently performed by highly energy-intensive cryogenic distillation. We have been studying the reversible reaction of C2H4 with various molecular pyrazolate complexes of copper, and fi nd that they are extremely selective for ethylene vs. ethane.1 -4 A typical gas-phase adsorption/desorption reaction, which occurs at 320 K – 343 K at atmospheric pressure, is illustrated in Fig. 1. We have performed in situ powder diffraction measurements of the repeated adsorption and desorption of ethylene from dense powders of several copper pyrazolate complexes at beamline 17 - BM of the Advanced Photon Source.2,3 We have determined previously unknown structures of several of the compounds and monitor the conversion between phases with and without adsorbed ethylene. It is truly remarkable that the subject molecules reversibly pass between trimer and dimer structures in the solid state upon reaction with ethylene.
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原位研究用于高选择性乙烯净化的分子铜化合物
从乙烯-乙烷混合物中提纯乙烯是一项重要而具有挑战性的工业流程,目前采用的是高能耗的低温蒸馏法。我们一直在研究 C2H4 与各种吡唑啉酸铜分子络合物的可逆反应,发现它们对乙烯和乙烷具有极高的选择性。我们在先进光子源的光束线 17 - BM 上对几种吡唑啉铜复合物的致密粉末中乙烯的反复吸附和解吸进行了原位粉末二重衍射测量。令人惊奇的是,这些化合物分子在固态下与乙烯反应时可逆地在三聚体和二聚体结构之间转换。
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