Yan Han, Yang Chun, Shao Wei-Peng, Cai Li-Hua, Wang Wei-Wei, Jin Zhao, Jia Chun-Jiang
Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, 250100, Jinan, China.
Nat Commun. 2019 Aug 2;10(1):3470. doi: 10.1038/s41467-019-11407-2.
As the water-gas shift (WGS) reaction serves as a crucial industrial process, strategies for developing robust WGS catalysts are highly desiderated. Here we report the construction of stabilized bulk-nano interfaces to fabricate highly efficient copper-ceria catalyst for the WGS reaction. With an in-situ structural transformation, small CeO nanoparticles (2-3 nm) are stabilized on bulk Cu to form abundant CeO-Cu interfaces, which maintain well-dispersed under reaction conditions. This inverse CeO/Cu catalyst shows excellent WGS performances, of which the activity is 5 times higher than other reported Cu catalysts. Long-term stability is also very solid under harsh conditions. Mechanistic study illustrates that for the inverse CeO/Cu catalyst, superb capability of HO dissociation and CO oxidation facilitates WGS process via the combination of associative and redox mechanisms. This work paves a way to fabricate robust catalysts by combining the advantages of bulk and nano-sized catalysts. Catalysts with such inverse configurations show great potential in practical WGS applications.
由于水煤气变换（WGS）反应是一个关键的工业过程，因此迫切需要开发性能强大的WGS催化剂的策略。在此，我们报告了构建稳定的体相-纳米界面以制备用于WGS反应的高效铜-二氧化铈催化剂。通过原位结构转变，小尺寸的CeO纳米颗粒（2-3纳米）稳定在体相Cu上，形成大量的CeO-Cu界面，这些界面在反应条件下保持良好的分散状态。这种反相CeO/Cu催化剂表现出优异的WGS性能，其活性比其他报道的Cu催化剂高5倍。在苛刻条件下，长期稳定性也非常出色。机理研究表明，对于反相CeO/Cu催化剂，卓越的HO解离和CO氧化能力通过缔合和氧化还原机制的结合促进了WGS过程。这项工作为通过结合体相和纳米尺寸催化剂的优点来制备性能强大的催化剂铺平了道路。具有这种反相构型的催化剂在实际WGS应用中显示出巨大潜力。
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