Porous graphene-assisted dynamic Pd catalysis for superior hydrogenation

Jie Gao, Chao Jia, Fengbo Yu, Yang Cao, Linyu Zhu, Aodi Li, Liming Sun, Litao Lin, Xuan Wu, Zhelin He, Zhongyue Zhou, James H. Clark, Lina Li, Yong Wang, Xiangdong Zhu*, Shicheng Zhang*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Statically immobilized Pd active sites leads to suboptimal hydrogenation efficacy even under harsh reaction conditions, and dynamic catalysis for individual requirements of H2 dissociation and substrate activation is devoid. Here, we have developed an innovative All-in-one system that employs dynamic Pd catalysis assisted by porous graphene, enabling hydrogenation to be conducted under mild conditions. The conversion of vanillin at 30 °C is 99% and the yield of 2-methoxy-4-methylphenol is >95%, significantly exceeding the reported records. The uniformly distributed N-doping and thin sheets of porous graphene induce Pd single-atom (PdN4) formation, and inhibit rapid agglomeration to nanoparticles (Pd NPs) for assisting dynamic catalysis. High–pressure process analysis and theoretical calculations reveal that excellent activity comes from the synergistic effects of PdN4 and Pd NPs. Importantly, All-in-one system is applicable for complex bio–oil hydrogenation and for a broad spectrum of unsaturated substrates.

Original languageEnglish
Article number124026
Number of pages10
JournalApplied Catalysis B: Environmental
Volume352
Early online date10 Apr 2024
DOIs
Publication statusE-pub ahead of print - 10 Apr 2024

Bibliographical note

Funding Information:
The authors acknowledge the financial support from the National Natural Science Foundation of China (No. 22278085). The authors thank beamline BL14W1 (Shanghai Synchrotron Radiation Facility) for providing the beam time. The authors thank the DFT calculations assisted by Shenzhen HUASUAN Technology Co. Ltd. The authors thank Chunfang Zheng (Shiyanjia Lab, www.shiyanjia.com) for the support of the XRD and XPS test.

Funding Information:
The authors acknowledge the financial support from the National Natural Science Foundation of China (No. 22278085). The authors thank beamline BL14W1 (Shanghai Synchrotron Radiation Facility) for providing the beam time. We thank the DFT calculations assisted by Shenzhen HUASUAN Technology Co., Ltd.

Publisher Copyright:
© 2024 Elsevier B.V.

Keywords

  • Dynamic Pd catalysis
  • Hydrogenation
  • Porous graphene
  • The All-in-one system

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