Zn stabilized Pd clusters with enhanced covalent metal-support interaction the formation of Pd-Zn bonds to promote catalytic thermal stability
Pd-Based heterogeneous catalysts have been demonstrated to be efficient in numerous heterogeneous reactions. However, the effect of the support resulting in covalent metal-support interaction (CMSI) has not been researched sufficiently. In this work, a Lewis base is modulated over MgAl-LDH to invest...
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Published in | Nanoscale Vol. 12; no. 27; pp. 14825 - 1483 |
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Main Authors | , , , , , , , |
Format | Journal Article |
Language | English |
Published |
16.07.2020
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Online Access | Get full text |
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Summary: | Pd-Based heterogeneous catalysts have been demonstrated to be efficient in numerous heterogeneous reactions. However, the effect of the support resulting in covalent metal-support interaction (CMSI) has not been researched sufficiently. In this work, a Lewis base is modulated over MgAl-LDH to investigate the support effects and it is further loaded with Pd clusters to research the metal-support interactions. MgAl-LDH with ultra-low Pd loading (0.0779%) shows CO conversion (55.0%) and dimethyl oxalate (DMO) selectivity (93.7%) for CO oxidative coupling to DMO, which was gradually deactivated after evaluation for 20 h. To promote the stability of Pd/MgAl-LDH, Zn
2+
ions were introduced into the MgAl-LDH support to strengthen the CMSI by forming Pd-Zn bonds, which further increased the adsorption energy of the Pd clusters on ZnMgAl-LDH, and this was verified by X-ray absorption fine structure (XAFS) measurements and density functional theory (DFT) calculations. The stability of the Pd/ZnMgAl-LDH catalyst could be maintained for at least 100 h. This work highlights that covalent metal-support interactions can be strengthened by forming new metal-metal bonds, which could be extended to other systems for the stabilization of noble metals over supports.
Zn
2+
-Modified MgAl-LDH with ultra-low Pd cluster loading was synthesized. The higher adsorption energy and strong covalent metal-support interaction
via
forming Pd-Zn bonds over Pd/ZnMgAl-LDH account for the robust catalytic performance. |
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Bibliography: | Electronic supplementary information (ESI) available: Experimental section, characterization details, computational methods and models, and activity evaluation. See DOI Dedicated to celebrate 60 years of the Fujian Institute of Research on the Structure of Matter. 10.1039/d0nr02987d |
ISSN: | 2040-3364 2040-3372 |
DOI: | 10.1039/d0nr02987d |