Single-Atom Pd₁/Graphene Catalyst Achieved by Atomic Layer Deposition: Remarkable Performance in Selective Hydrogenation of 1,3-Butadiene.
We reported that atomically dispersed Pd on graphene can be fabricated using the atomic layer deposition technique. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine structure spectroscopy both confirmed that isolated Pd single atoms dominantly existed on the graphene support. In selective hydrogenation of 1,3-butadiene, the single-atom Pd1/graphene catalyst showed about 100% butenes selectivity at 95% conversion at a mild reaction condition of about 50 °C, which is likely due to the changes of 1,3-butadiene adsorption mode and enhanced steric effect on the isolated Pd atoms. More importantly, excellent durability against deactivation via either aggregation of metal atoms or carbonaceous deposits during a total 100 h of reaction time on stream was achieved. Therefore, the single-atom catalysts may open up more opportunities to optimize the activity, selectivity, and durability in selective hydrogenation reactions.
Department of Chemical Physics, National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Huan
H
Yan
Department of Chemical Physics, National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Hao
H
Cheng
Department of Chemical Physics, National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Hong
H
Yi
Department of Chemical Physics, National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Yue
Y
Lin
Department of Chemical Physics, National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Tao
T
Yao
Department of Chemical Physics, National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Chunlei
C
Wang
Department of Chemical Physics, National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Junjie
J
Li
Department of Chemical Physics, National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Shiqiang
S
Wei
Department of Chemical Physics, National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, University of Science and Technology of China , Hefei, Anhui 230026, P. R. China.
Junling
J
Lu