Revealing the Active Species for Aerobic Alcohol Oxidation by Using Uniform Supported Palladium Catalysts

Pingyu Xin; Jia Li; Yu Xiong; Xi Wu; Juncai Dong; Wenxing Chen; Yu Wang; Lin Gu; Jun Luo; Hongpan Rong; Chen Chen; Qing Peng; Dingsheng Wang; Yadong Li

doi:10.1002/anie.201801103

Revealing the Active Species for Aerobic Alcohol Oxidation by Using Uniform Supported Palladium Catalysts

Pingyu Xin, Jia Li, Yu Xiong, Xi Wu, Juncai Dong, Wenxing Chen, Yu Wang, Lin Gu, Jun Luo, Hongpan Rong, Chen Chen, Qing Peng, Dingsheng Wang^*, Yadong Li

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

109 Citations (Scopus)

Abstract

The active species in supported metal catalysts are elusive to identify, and large quantities of inert species can cause significant waste. Herein, using a stoichiometrically precise synthetic method, we prepare atomically dispersed palladium–cerium oxide (Pd₁/CeO₂) and hexapalladium cluster–cerium oxide (Pd₆/CeO₂), as confirmed by spherical-aberration-corrected transmission electron microscopy and X-ray absorption fine structure spectroscopy. For aerobic alcohol oxidation, Pd₁/CeO₂ shows extremely high catalytic activity with a TOF of 6739 h⁻¹ and satisfactory selectivity (almost 100 % for benzaldehyde), while Pd₆/CeO₂ is inactive, indicating that the true active species are single Pd atoms. Theoretical simulations reveal that the bulkier Pd₆ clusters hinder the interactions between hydroxy groups and the CeO₂ surface, thus suppressing synergy of Pd-Ce perimeter.

Original language	English
Pages (from-to)	4642-4646
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	57
Issue number	17
DOIs	https://doi.org/10.1002/anie.201801103
Publication status	Published - 16 Apr 2018
Externally published	Yes

Keywords

aerobic oxidation
benzyl alcohol
palladium clusters
single atom catalysts
supported catalysts

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10.1002/anie.201801103

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title = "Revealing the Active Species for Aerobic Alcohol Oxidation by Using Uniform Supported Palladium Catalysts",

abstract = "The active species in supported metal catalysts are elusive to identify, and large quantities of inert species can cause significant waste. Herein, using a stoichiometrically precise synthetic method, we prepare atomically dispersed palladium–cerium oxide (Pd1/CeO2) and hexapalladium cluster–cerium oxide (Pd6/CeO2), as confirmed by spherical-aberration-corrected transmission electron microscopy and X-ray absorption fine structure spectroscopy. For aerobic alcohol oxidation, Pd1/CeO2 shows extremely high catalytic activity with a TOF of 6739 h−1 and satisfactory selectivity (almost 100 % for benzaldehyde), while Pd6/CeO2 is inactive, indicating that the true active species are single Pd atoms. Theoretical simulations reveal that the bulkier Pd6 clusters hinder the interactions between hydroxy groups and the CeO2 surface, thus suppressing synergy of Pd-Ce perimeter.",

keywords = "aerobic oxidation, benzyl alcohol, palladium clusters, single atom catalysts, supported catalysts",

author = "Pingyu Xin and Jia Li and Yu Xiong and Xi Wu and Juncai Dong and Wenxing Chen and Yu Wang and Lin Gu and Jun Luo and Hongpan Rong and Chen Chen and Qing Peng and Dingsheng Wang and Yadong Li",

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year = "2018",

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doi = "10.1002/anie.201801103",

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T1 - Revealing the Active Species for Aerobic Alcohol Oxidation by Using Uniform Supported Palladium Catalysts

AU - Xin, Pingyu

AU - Li, Jia

AU - Xiong, Yu

AU - Wu, Xi

AU - Dong, Juncai

AU - Chen, Wenxing

AU - Wang, Yu

AU - Gu, Lin

AU - Luo, Jun

AU - Rong, Hongpan

AU - Chen, Chen

AU - Peng, Qing

AU - Wang, Dingsheng

AU - Li, Yadong

PY - 2018/4/16

Y1 - 2018/4/16

N2 - The active species in supported metal catalysts are elusive to identify, and large quantities of inert species can cause significant waste. Herein, using a stoichiometrically precise synthetic method, we prepare atomically dispersed palladium–cerium oxide (Pd1/CeO2) and hexapalladium cluster–cerium oxide (Pd6/CeO2), as confirmed by spherical-aberration-corrected transmission electron microscopy and X-ray absorption fine structure spectroscopy. For aerobic alcohol oxidation, Pd1/CeO2 shows extremely high catalytic activity with a TOF of 6739 h−1 and satisfactory selectivity (almost 100 % for benzaldehyde), while Pd6/CeO2 is inactive, indicating that the true active species are single Pd atoms. Theoretical simulations reveal that the bulkier Pd6 clusters hinder the interactions between hydroxy groups and the CeO2 surface, thus suppressing synergy of Pd-Ce perimeter.

AB - The active species in supported metal catalysts are elusive to identify, and large quantities of inert species can cause significant waste. Herein, using a stoichiometrically precise synthetic method, we prepare atomically dispersed palladium–cerium oxide (Pd1/CeO2) and hexapalladium cluster–cerium oxide (Pd6/CeO2), as confirmed by spherical-aberration-corrected transmission electron microscopy and X-ray absorption fine structure spectroscopy. For aerobic alcohol oxidation, Pd1/CeO2 shows extremely high catalytic activity with a TOF of 6739 h−1 and satisfactory selectivity (almost 100 % for benzaldehyde), while Pd6/CeO2 is inactive, indicating that the true active species are single Pd atoms. Theoretical simulations reveal that the bulkier Pd6 clusters hinder the interactions between hydroxy groups and the CeO2 surface, thus suppressing synergy of Pd-Ce perimeter.

KW - aerobic oxidation

KW - benzyl alcohol

KW - palladium clusters

KW - single atom catalysts

KW - supported catalysts

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DO - 10.1002/anie.201801103

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JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 17

ER -

Revealing the Active Species for Aerobic Alcohol Oxidation by Using Uniform Supported Palladium Catalysts

Abstract

Keywords

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