Probing the origin of the enhanced catalytic performance of sp(3)@sp(2) 
nanocarbon supported Pd catalyst for CO oxidation

Zhang, Liyun; Ding, Yuxiao; Koh, Yoobin Esther; Mun, Bongjin Simon; Wu, Kuang-Hsu; Niu, Yiming; Shi, Wen; Zhang, Bingsen

doi:10.1016/j.carbon.2019.09.075

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Probing the origin of the enhanced catalytic performance of sp(3)@sp(2) nanocarbon supported Pd catalyst for CO oxidation

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Ding, Yuxiao
Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society;

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Zhang, L., Ding, Y., Koh, Y. E., Mun, B. S., Wu, K.-H., Niu, Y., et al. (2020). Probing the origin of the enhanced catalytic performance of sp(3)@sp(2) nanocarbon supported Pd catalyst for CO oxidation. Carbon, 156, 463-469. doi:10.1016/j.carbon.2019.09.075.

Cite as: https://hdl.handle.net/21.11116/0000-0007-D523-1

Abstract

Tuning the fine structure of carbon support is crucial for modifying the metal-support interface (MSI) in order to harvest a high-performance catalysis. Herein, a core-shell sp(3)@sp(2) nanocarbon (nano-diamond@graphene, ND@G) and a pure sp(2) carbon derivative (onion-like carbon, OLC) were applied to support Pd nanoparticles. We found that Pd/ND@G displayed a superior catalytic activity for CO oxidation reaction with a TOF of 2.9 times higher than that of Pd/OLC at 46 degrees C. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and ambient pressure Xray photoelectron spectroscopy (AP-XPS) revealed that, different with the Pd/OLC system, a unique interface microstructure was formed in Pd/ND@G, which not only provides a high exposure of active sites, but also enhances the Pd surface reactivity toward oxygen species, thus leading to a superior catalytic activity of Pd/ND@G. Moreover, the temperature-programmed surface reaction (TPSR) results showed that CO oxidation on Pd/ND@G undergoes an unusual termolecular Eley-Rideal (TER) mechanism, which has a lower energy barrier as compared to the traditional Langmuir-Hinshelwood (LH) and ER mechanism. (C) 2019 Elsevier Ltd. All rights reserved.