Journal
JOURNAL OF CATALYSIS
Volume 370, Issue -, Pages 107-117Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2018.12.006
Keywords
Layered double hydroxide; Metal-hydroxide interface; Sandwich structure; Oxygen vacancy; Selective hydrogenation of C=O Bonds
Categories
Funding
- National key Research and Development Program of China [2016YFB0301600]
- National Natural Science Foundation
- Fundamental Research Funds for the Central Universities [BHYC1701B, JD1816]
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In this work, a Pd/MgAl-LDH catalyst was synthesized by the ion-exchange and liquid-reduction process (IE), with impregnation method (IM) as contrast, to study the difference in the interfacial structure induced by the preparation methods and the catalytic behavior for selective hydrogenation of 2-ethylanthraquinone. STEM-EDS measurement reveals that the IE-Pd/MgAl-LDH catalyst possesses an obvious sandwich structure of which Pd nanoparticles uniformly located in the LDH interlayer space, and therefore exhibits more Pd-LDH interface sites due to the high intimacy. More importantly, it was confirmed that the Pd-LDH interface structure was characterized by rich oxygen vacancies (Vo) due to the loss of surface hydroxyl groups on the LDH layer during the ion-exchange process. As expected, the IE-Pd/MgAl-LDH catalyst exhibited a 127% higher H2O2 yield than that of IM-Pd/MgAl-LDH catalyst. High activity was attributed to the facilitated hydrogen activation resulting from significantly enhanced hydrogen spillover over the Pd-LDH interface structure. Preferred selectivity was owing to the special adsorption mode of C=O bond interacted with the Pd-Vo interfacial sites, which leads to the selective activation of C=O bond. This work develops a feasible approach to fabricate the metal-hydroxide interface structure and provides a fundamental understanding on interfacial effect toward selective hydrogenation of C=O bonds. (C) 2018 Elsevier Inc. All rights reserved.
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