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Nano Research

Article Title

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

Authors

Xiaohui Huang, Department of Chemical Physics, iChEM, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, China
Yujia Xia, Department of Chemical Physics, iChEM, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, China
Yuanjie Cao, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
Xusheng Zheng, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
Haibin Pan, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
Junfa Zhu, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
Chao Ma, Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China
Hengwei Wang, Department of Chemical Physics, iChEM, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, China
Junjie Li, Department of Chemical Physics, iChEM, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, China
Rui You, Department of Chemical Physics, iChEM, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, China
Shiqiang Wei, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
Weixin Huang, Department of Chemical Physics, iChEM, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, China Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei 230026, China
Junling Lu, Department of Chemical Physics, iChEM, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China, Hefei 230026, China

Keywords

single-atom catalyst, Pd catalyst, atomic layer deposition, acetylene hydrogenation, C3N4, selectivity, coke formation, support effect

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.

Graphical Abstract

Publisher

Tsinghua University Press

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