Porous graphene-assisted dynamic Pd catalysis for superior hydrogenation

TY - JOUR

T1 - Porous graphene-assisted dynamic Pd catalysis for superior hydrogenation

AU - Gao, Jie

AU - Jia, Chao

AU - Yu, Fengbo

AU - Cao, Yang

AU - Zhu, Linyu

AU - Li, Aodi

AU - Sun, Liming

AU - Lin, Litao

AU - Wu, Xuan

AU - He, Zhelin

AU - Zhou, Zhongyue

AU - Clark, James H.

AU - Li, Lina

AU - Wang, Yong

AU - Zhu, Xiangdong

AU - Zhang, Shicheng

N1 - 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.

PY - 2024/9/5

Y1 - 2024/9/5

N2 - 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.

AB - 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.

KW - Dynamic Pd catalysis

KW - Hydrogenation

KW - Porous graphene

KW - The All-in-one system

UR - http://www.scopus.com/inward/record.url?scp=85189864094&partnerID=8YFLogxK

U2 - 10.1016/j.apcatb.2024.124026

DO - 10.1016/j.apcatb.2024.124026

M3 - Article

AN - SCOPUS:85189864094

SN - 0926-3373

VL - 352

JO - Applied Catalysis B: Environmental

JF - Applied Catalysis B: Environmental

M1 - 124026

ER -