The Rise of Calcination Temperature Enhances the Performance of Cu Catalysts: Contributions of Support
The Rise of Calcination Temperature Enhances the Performance of Cu Catalysts: Contributions of Support
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DOI：
10.1021/cs501155x
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发表时间：
2014-09
期刊：
影响因子：
12.9
通讯作者：
Yifeng Zhu;Xiao Kong;Dong-bo Cao;J. Cui;Yulei Zhu;Yong-wang Li
中科院分区：
文献类型：
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作者：
Yifeng Zhu;Xiao Kong;Dong-bo Cao;J. Cui;Yulei Zhu;Yong-wang Li
为了开发高性能的负载型金属催化剂，阐明和充分利用不可缺少的载体部分是非常必要的。本文通过对分级焙烧实验、模型催化剂测试和各种催化剂结构表征的综合分析，阐明了载体ZrO2的结构与催化性能的关系。我们证明，铜和四氢氧化锆的组合，使一个高活性，选择性，特别是稳定的催化剂草酸二甲酯加氢乙二醇。为了获得稳定的Cu颗粒，将催化剂在高温下退火（例如，从450至850 °C）。形成了稳定的大Cu颗粒，暴露的Cu位的数量减少。幸运的是，支持ZrO2被激励到四相，补偿，甚至提高活性。乙二醇的收率由原来的26%提高到99%，且反应性能稳定。
To develop the high-performance supported metal catalyst for industrial processes, it is highly desirable to elucidate and fully utilize the indispensable support part. Herein, the relationship between catalytic performance and the structure of support ZrO2 was elucidated by comprehensive analysis of the progressive calcination experiments, tests over model catalysts, and various characterizations of catalyst structures. We demonstrated that combination of Cu and tetragonal ZrO2 makes a highly active, selective, and especially stable catalyst for the hydrogenation of dimethyl oxalate to ethylene glycol. To obtain stable Cu particles, the catalyst was annealed at high temperatures (e.g., from 450 to 850 °C). The stable large Cu particles were formed, and the number of exposed Cu sites decreased. Fortunately, support ZrO2 was motivated into the tetragonal phase, compensating for and even improving the activity. Thus, the yield of ethylene glycol was greatly improved from ∼26 to 99%, and a stable performance...