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铜和钌掺杂二氧化铈催化剂的低温氧化还原活性及乙醇氨氧化性能

Low-temperature redox activity and alcohol ammoxidation performance on Cu- and Ru-incorporated ceria catalysts.

作者信息

Chen Chaoqi, Ikemoto Satoru, Yokota Gen-Ichi, Higuchi Kimitaka, Muratsugu Satoshi, Tada Mizuki

机构信息

Department of Chemistry, Graduate School of Science, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi 464-8602, Japan.

Institute of Materials and Systems for Sustainability, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Aichi 464-8602, Japan.

出版信息

Phys Chem Chem Phys. 2024 Jul 3;26(26):17979-17990. doi: 10.1039/d4cp01432d.

Abstract

Transition-metal-incorporated cerium oxides with Cu and a small amount of Ru (CuRuCeO) were prepared, and their low-temperature redox performance (<423 K) and catalytic alcohol ammoxidation performance were investigated. Temperature-programmed reduction/oxidation under H/O and X-ray absorption fine structure revealed the reversible redox behavior of the three metals, Cu, Ru, and Ce, in the low-temperature redox processes. The initially reduced Ru species decreased the reduction temperature of Cu oxides and promoted the activation of Ce species. CuRuCeO selectively catalyzed the production of benzonitrile in the ammoxidation of benzyl alcohol. H-treated CuRuCeO showed a slightly larger initial conversion of benzyl alcohol than O-treated CuRuCeO, suggesting that the reduced structure of CuRuCeO was active for the ammoxidation. The integration of both Cu and Ru resulted in the efficient promotion of ammoxidation, in which the Ru species were involved in the conversion of benzyl alcohol and Cu species were required for selective production of benzonitrile.

摘要

制备了含有铜和少量钌的过渡金属掺杂氧化铈(CuRuCeO),并研究了其低温氧化还原性能(<423 K)和催化醇氨氧化性能。在H/O气氛下的程序升温还原/氧化以及X射线吸收精细结构揭示了铜、钌和铈这三种金属在低温氧化还原过程中的可逆氧化还原行为。最初还原的钌物种降低了氧化铜的还原温度,并促进了铈物种的活化。CuRuCeO在苯甲醇氨氧化反应中选择性催化生成苯甲腈。H处理的CuRuCeO比O处理的CuRuCeO表现出略高的苯甲醇初始转化率,这表明CuRuCeO的还原结构对氨氧化反应具有活性。铜和钌的结合有效地促进了氨氧化反应,其中钌物种参与了苯甲醇的转化,而铜物种是选择性生成苯甲腈所必需的。

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