Sun Yongkang, Zeng Junming, Zhang Jie, Yang Jun, Qian Weixin, Yu Feng, Dai Bin, Li Jiangbing
School of Chemistry and Chemical Engineering/Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, Shihezi University, Shihezi 832003, Xinjiang, China.
Engineering Research Center of Large Reactor Engineering, Ministry of Education, East China University of Science and Technology, Shanghai, 200237, China.
ACS Omega. 2020 Oct 14;5(42):27692-27701. doi: 10.1021/acsomega.0c04289. eCollection 2020 Oct 27.
Sustainable development is a worldwide concern. This work mainly focuses on the reuse of the combustion products of calcium carbide and the influence of different kinds of copper on the acetylene carbonylation reaction. A series of catalysts were prepared by heating the precursors under various atmospheres (air, hydrogen, and nitrogen). The X-ray diffraction and the X-ray photoelectron spectroscopy have been analyzed regarding copper species composition and content in catalysts. The result of the Cu-promoted reaction was in good agreement with the conducted density functional theory analysis, and we speculate that Cu promotes the transfer of electrons in the reaction. Transmission electron microscopy and elemental mapping evaluation confirmed the difference in Cu dispersion. Characterization of catalysts using temperature programmed desorption and pyridine Fourier-transform infrared revealed differences in their acidity. Acidity was found to be favorable for acetylene carbonylation. Selectivity and yield of the CuAlZn-LDO(N) catalyst at 225 °C were 73 and 70%, respectively, and the catalyst showed good stability over two consecutive cycles of reuse.
可持续发展是全球关注的问题。这项工作主要集中在电石燃烧产物的再利用以及不同种类的铜对乙炔羰基化反应的影响。通过在各种气氛(空气、氢气和氮气)下加热前驱体制备了一系列催化剂。对催化剂中铜物种的组成和含量进行了X射线衍射和X射线光电子能谱分析。铜促进反应结果与进行的密度泛函理论分析结果吻合良好,我们推测铜促进了反应中电子的转移。透射电子显微镜和元素映射评估证实了铜分散性的差异。使用程序升温脱附和吡啶傅里叶变换红外光谱对催化剂进行表征,揭示了它们酸度的差异。发现酸度有利于乙炔羰基化。CuAlZn-LDO(N)催化剂在225℃下的选择性和产率分别为73%和70%,并且该催化剂在连续两个循环的再利用中表现出良好的稳定性。