Tuning hydrogenation chemistry of Pd-based heterogeneous catalysts by introducing homogeneous-like ligands

Jianghao Zhang, Wenda Hu, Binbin Qian, Houqian Li, Berlin Sudduth, Mark Engelhard, Lian Zhang, Jianzhi Hu, Junming Sun (), Changbin Zhang (), Hong He and Yong Wang ()
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Jianghao Zhang: Washington State University
Wenda Hu: Washington State University
Binbin Qian: Yancheng Teachers University
Houqian Li: Washington State University
Berlin Sudduth: Washington State University
Mark Engelhard: Pacific Northwest National Laboratory
Lian Zhang: Monash University
Jianzhi Hu: Washington State University
Junming Sun: Washington State University
Changbin Zhang: Research Center for Eco-environmental Sciences, Chinese Academy of Sciences
Hong He: Research Center for Eco-environmental Sciences, Chinese Academy of Sciences
Yong Wang: Washington State University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Noble metals have been extensively employed in a variety of hydrotreating catalyst systems for their featured functionality of hydrogen activation but may also bring side reactions such as undesired deep hydrogenation. It is crucial to develop a viable approach to selectively inhibit side reactions while preserving beneficial functionalities. Herein, we present modifying Pd with alkenyl-type ligands that forms homogeneous-like Pd-alkene metallacycle structure on the heterogeneous Pd catalyst to achieve the selective hydrogenolysis and hydrogenation. Particularly, a doped alkenyl-type carbon ligand on Pd-Fe catalyst is demonstrated to donate electrons to Pd, creating an electron-rich environment that elongates the distance and weakens the electronic interaction between Pd and unsaturated C of the reactants/products to control the hydrogenation chemistry. Moreover, high H2 activation capability is maintained over Pd and the activated H is transferred to Fe to facilitate C-O bond cleavage or directly participate in the reaction on Pd. The modified Pd-Fe catalyst displays comparable C-O bond cleavage rate but much higher selectivity (>90%) than the bare Pd-Fe ( 90%) in acetylene hydrogenation. This work sheds light on the controlled synthesis of selective hydrotreating catalysts via mimicking homogeneous analogues.

Date: 2023
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DOI: 10.1038/s41467-023-39478-2

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