Tripodal Pd metallenes mediated by Nb2C MXenes for boosting alkynes semihydrogenation

Zhongzhe Wei, Zijiang Zhao, Chenglong Qiu, Songtao Huang, Zihao Yao (), Mingxuan Wang, Yi Chen, Yue Lin, Xing Zhong, Xiaonian Li () and Jianguo Wang ()
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Zhongzhe Wei: Zhejiang University of Technology
Zijiang Zhao: Zhejiang University of Technology
Chenglong Qiu: Zhejiang University of Technology
Songtao Huang: Zhejiang University of Technology
Zihao Yao: Zhejiang University of Technology
Mingxuan Wang: Zhejiang University of Technology
Yi Chen: Zhejiang University of Technology
Yue Lin: University of Science and Technology of China
Xing Zhong: Zhejiang University of Technology
Xiaonian Li: Zhejiang University of Technology
Jianguo Wang: Zhejiang University of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract 2D metallene nanomaterials have spurred considerable attention in heterogeneous catalysis by virtue of sufficient unsaturated metal atoms, high specific surface area and surface strain. Nevertheless, the strong metallic bonding in nanoparticles aggravates the difficulty in the controllable regulation of the geometry of metallenes. Here we propose an efficient galvanic replacement strategy to construct Pd metallenes loaded on Nb2C MXenes at room temperature, which is triggered by strong metal-support interaction based on MD simulations. The Pd metallenes feature a chair structure of six-membered ring with the coordination number of Pd as low as 3. Coverage-dependent kinetic analysis based on first-principles calculations reveals that the tripodal Pd metallenes promote the diffusion of alkene and inhibit its overhydrogenation. As a consequence, Pd/Nb2C delivers an outstanding turnover frequency of 10372 h−1 and a high selectivity of 96% at 25 oC in the semihydrogenation of alkynes without compromising the stability. This strategy is general and scalable considering the plentiful members of the MXene family, which can set a foundation for the design of novel supported-metallene catalysts for demanding transformations.

Date: 2023
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DOI: 10.1038/s41467-023-36378-3

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