Deactivation Mechanism and Regeneration of the CuCl/Activated Carbon Catalyst for Gas–Solid Acetylene Dimerization

乙炔 催化作用 化学 机制(生物学) 再生(生物学) 活性炭 碳纤维 材料科学 光化学 化学工程 有机化学 细胞生物学 复合材料 复合数 吸附 生物 工程类 哲学 认识论
作者
Qi Song,Linye Liu,Qinqin Wang,Bin Dai
出处
期刊:ACS omega [American Chemical Society]
卷期号:7 (47): 43265-43272 被引量:5
标识
DOI:10.1021/acsomega.2c05974
摘要

Acetylene dimerization is necessary to the coal chemical industry for producing monovinylacetylene, while the deactivation mechanism and regeneration of catalysts have not been studied in detail, which is crucial to the design of high-efficiency catalysts for acetylene dimerization. Herein, the deactivation mechanism and regeneration methods of CuCl/activated carbon catalysts in gas–solid acetylene dimerization were studied in detail. The catalysts with different reaction times were analyzed by temperature-programmed desorption of ammonia (NH3-TPD), Fourier transform infrared (FT-IR), thermogravimetry (TG), pyridine-FTIR, and X-ray photoelectron spectroscopy (XPS) analyses. NH3-TPD results demonstrated that as the time went on, the strong acid in the samples was enhanced, while the weak acid was weakened. Similarly, pyridine-FTIR results indicated that both Brönsted and Lewis acids in the samples were decreased. TG and XPS results showed that the reasons for deactivation for acetylene dimerization in the gas–solid reaction were significantly affected by coke deposition and the change of Cu valence. The more the content of Cu+, the higher the acetylene conversion rate, implying that Cu+ may be the active center of the acetylene dimerization reaction. Thus, removing carbon deposition through calcining and increasing the content of Cu+ was an effective way of regenerating the catalyst. This work strengthened the understanding of the deactivation behavior and provides a practicable regeneration method for the catalyst in gas–solid acetylene dimerization.
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