Au-Cu/Co3O4双金属催化剂上乙烯完全催化氧化性能

doi:10.3866/PKU.WHXB20110719

摘要/Abstract

摘要：

以共沉淀法制得的Co₃O₄为载体, 采用两步法负载Au和Cu制得了一系列Au-Cu/Co₃O₄双金属催化剂, 考察了Au-Cu/Co₃O₄双金属催化剂完全催化氧化乙烯的性能, 并通过X射线衍射(XRD)、高分辨透射电镜(HRTEM)、H₂程序升温还原(H₂-TPR)和O₂程序升温脱附(O₂-TPD)对催化剂进行了表征. 活性测试结果表明: 负载型Au-Cu/Co₃O₄双金属催化剂的催化性能优于单一金属催化剂Au/Co₃O₄, 并且在Au负载量为4% (w, 质量分数)时, 与AuCu/Co₃O₄和Au₃Cu/Co₃O₄催化剂相比, AuCu₃/Co₃O₄催化剂的催化活性较好, 0 ℃时可催化转化15.3%的乙烯为CO₂和H₂O, 120 ℃时100%催化转化乙烯. XRD和HRTEM表明, AuCu₃/Co₃O₄催化剂中有Au-Cu合金相的生成, 而Au₃Cu/Co₃O₄催化剂中Cu主要以氧化物的形式存在. Au和Cu之间产生相互作用, 使活性相金属的粒径降低. H₂-TPR和O₂-TPD分析结果表明, AuCu₃/Co₃O₄催化剂具有较强的低温可还原能力和可提供的大量表面活性吸附氧物种, 促进了乙烯的完全催化氧化.

关键词: 纳米金催化材料, Au-Cu/Co₃O₄, 乙烯, 催化氧化, 金铜合金

Abstract:

A series of Au-Cu/Co₃O₄ catalysts with different mass fractions of Cu were synthesized by a two-step method that consists of depositing gold and copper onto a Co₃O₄ support, which was synthesized by coprecipitation. The effect of copper on the catalytic activity of Au-Cu/Co₃O₄ was evaluated for the complete oxidation of ethylene at different temperatures and the prepared catalysts were characterized by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), H₂ temperature- programmed reduction (H₂-TPR), and O₂ temperature-programmed desorption (O₂-TPD). The results show that Au-Cu/Co₃O₄ bimetal catalysts exhibit higher catalytic activities than the Au/Co₃O₄ catalyst. At a gold loading amount of 4% (w, mass fraction) the AuCu₃/Co₃O₄ catalyst gives higher catalytic activity compared to catalysts AuCu/Co₃O₄ and Au₃Cu/Co₃O₄. Ethylene conversion was 15.3% for AuCu₃/Co₃O₄ even at 0 ℃ whereas at 120 ℃ the full conversion of ethylene was obtained. The results of XRD and HRTEM indicate the formation of an Au-Cu alloy in AuCu₃/Co₃O₄. However, we have found that the majority of Cu is present in the form of Cu2O in Au₃Cu/Co₃O₄. The interaction between Au and Cu on the surface of the catalysts decreases the particle size of the gold and, therefore, it is much easier to activate ethylene. H₂-TPR and O₂-TPD results show that the high reduction ability and the high intensity of surface oxygen active species contribute to the excellent catalytic activity of the AuCu₃/Co₃O₄ catalyst.

Key words: Nano-gold catalyst, Au-Cu/Co₃O₄, Ethylene, Catalytic oxidation, Au-Cu alloy

薛雯娟, 张新艳, 李鹏, 刘昭铁, 郝郑平, 麻春艳, . Au-Cu/Co₃O₄双金属催化剂上乙烯完全催化氧化性能[J]. 物理化学学报, 2011, 27(07): 1730-1736.

XUE Wen-Juan, ZHANG Xin-Yan, LI Peng, LIU Zhao-Tie, HAO Zheng-Ping, MA Chun-Yan. Catalytic Activities for the Complete Oxidation of Ethylene over Au-Cu/Co₃O₄ Catalysts[J]. Acta Phys. -Chim. Sin., 2011, 27(07): 1730-1736.

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB20110719

https://www.whxb.pku.edu.cn/CN/Y2011/V27/I07/1730

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Au-Cu/Co₃O₄双金属催化剂上乙烯完全催化氧化性能

Catalytic Activities for the Complete Oxidation of Ethylene over Au-Cu/Co₃O₄ Catalysts

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