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Small-sized cuprous oxide species on silica boost acrolein formation via selective oxidation of propylene
Chinese Journal of Catalysis ( IF 15.7 ) Pub Date : 2021-02-01 , DOI: 10.1016/s1872-2067(20)63636-1
Ling-Ling Guo , Jing Yu , Wei-Wei Wang , Jia-Xu Liu , Hong-Chen Guo , Chao Ma , Chun-Jiang Jia , Jun-Xiang Chen , Rui Si

Abstract Oxide-supported copper-containing materials have attracted considerable research attention as promising candidates for acrolein formation. Nevertheless, the elucidation of the structure-performance relationships for these systems remains a scientific challenge. In this work, copper oxide clusters deposited on a high-surface-area silica support were synthesized via a deposition-precipitation approach and exhibited remarkable catalytic reactivity (up to 25.5% conversion and 66.8% selectivity) in the propylene-selective oxidation of acrolein at 300 °C. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy combined with X-ray absorption fine structure measurements of the catalyst before and after the reaction confirmed the transformation of the small-sized copper oxide (CuO) clusters into cuprous oxide (Cu2O) clusters. With the aid of in situ X-ray diffraction and in situ dual beam Fourier transform infrared spectroscopy (DB-FTIR), the allyl intermediate (CH2=CHCH2*) was clearly observed, along with the as-formed Cu2O species. The intermediate can react with oxygen atoms from neighboring Cu2O species to form acrolein during the catalytic process, and the small-sized Cu2O clusters play a crucial role in the generation of acrolein via the selective oxidation of propylene.

中文翻译:

二氧化硅上的小尺寸氧化亚铜物质通过丙烯的选择性氧化促进丙烯醛的形成

摘要 氧化物负载的含铜材料作为丙烯醛形成的有希望的候选材料已经引起了相当多的研究关注。然而,阐明这些系统的结构-性能关系仍然是一个科学挑战。在这项工作中,沉积在高表面积二氧化硅载体上的氧化铜簇是通过沉积-沉淀方法合成的,并且在丙烯醛的丙烯选择性氧化中表现出显着的催化反应性(高达 25.5% 的转化率和 66.8% 的选择性)。 300℃。像差校正的高角度环形暗场扫描透射电子显微镜结合反应前后催化剂的 X 射线吸收精细结构测量证实了小尺寸氧化铜 (CuO) 簇向氧化亚铜 (Cu2O) 的转化) 簇。借助原位 X 射线衍射和原位双光束傅里叶变换红外光谱 (DB-FTIR),可以清楚地观察到烯丙基中间体 (CH2=CHCH2*) 以及形成的 Cu2O 物种。在催化过程中,中间体可以与来自相邻 Cu2O 物种的氧原子反应形成丙烯醛,而小尺寸的 Cu2O 簇在通过丙烯的选择性氧化生成丙烯醛中起着至关重要的作用。借助原位 X 射线衍射和原位双光束傅里叶变换红外光谱 (DB-FTIR),可以清楚地观察到烯丙基中间体 (CH2=CHCH2*) 以及形成的 Cu2O 物种。在催化过程中,中间体可以与来自相邻 Cu2O 物种的氧原子反应形成丙烯醛,而小尺寸的 Cu2O 簇在通过丙烯的选择性氧化生成丙烯醛中起着至关重要的作用。借助原位 X 射线衍射和原位双光束傅里叶变换红外光谱 (DB-FTIR),可以清楚地观察到烯丙基中间体 (CH2=CHCH2*) 以及形成的 Cu2O 物种。在催化过程中,中间体可以与来自相邻 Cu2O 物种的氧原子反应形成丙烯醛,而小尺寸的 Cu2O 簇在通过丙烯的选择性氧化生成丙烯醛中起着至关重要的作用。
更新日期:2021-02-01
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