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Research Article

Enhancing both selectivity and coking-resistance of a single-atom Pd1/C3N4 catalyst for acetylene hydrogenation

Xiaohui Huang1,§, Yujia Xia1,§, Yuanjie Cao2, Xusheng Zheng2, Haibin Pan2, Junfa Zhu2, Chao Ma3, Hengwei Wang1, Junjie Li1, Rui You1, Shiqiang Wei2, Weixin Huang1,3, Junling Lu1( )
Department of Chemical Physics, iChEMCAS Key Laboratory of Materials for Energy ConversionUniversity of Science and Technology of ChinaHefei230026China
National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei230029China
Hefei National Laboratory for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefei230026China

§ These authors contributed equally to this work.

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Graphical Abstract

Abstract

Selective hydrogenation is an important industrial catalytic process in chemical upgrading, where Pd-based catalysts are widely used because of their high hydrogenation activities. However, poor selectivity and short catalyst lifetime because of heavy coke formation have been major concerns. In this work, atomically dispersed Pd atoms were successfully synthesized on graphitic carbon nitride (g-C3N4) using atomic layer deposition. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) confirmed the dominant presence of isolated Pd atoms without Pd nanoparticle (NP) formation. During selective hydrogenation of acetylene in excess ethylene, the g-C3N4-supported Pd NP catalysts had strikingly higher ethylene selectivities than the conventional Pd/Al2O3 and Pd/SiO2 catalysts. In-situ X-ray photoemission spectroscopy revealed that the considerable charge transfer from the Pd NPs to g-C3N4 likely plays an important role in the catalytic performance enhancement. More impressively, the single-atom Pd1/C3N4 catalyst exhibited both higher ethylene selectivity and higher coking resistance. Our work demonstrates that the single-atom Pd catalyst is a promising candidate for improving both selectivity and coking-resistance in hydrogenation reactions.

Keywords

single-atom catalystPd catalystatomic layer depositionacetylene hydrogenationC3N4selectivitycoke formationsupport effect

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Nano Research
Volume 10 Issue 4,
April 2017
Pages 1302-1312
DOI: 10.1007/s12274-016-1416-z
Cite this article:
Huang X, Xia Y, Cao Y, et al. Enhancing both selectivity and coking-resistance of a single-atom Pd1/C3N4 catalyst for acetylene hydrogenation. Nano Research, 2017, 10(4): 1302-1312. https://doi.org/10.1007/s12274-016-1416-z
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Received: 11 November 2016
Revised: 09 December 2016
Accepted: 12 December 2016
Published: 20 February 2017
© Tsinghua University Press and Springer-Verlag Berlin Heidelberg 2016
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