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; Jianguo Wang

doi:10.1038/s41467-023-36378-3

Tripodal Pd metallenes mediated by Nb₂C MXenes for boosting alkynes semihydrogenation

Nat Commun. 2023 Feb 7;14(1):661. doi: 10.1038/s41467-023-36378-3.

Authors

Zhongzhe Wei^#¹, Zijiang Zhao^#¹, Chenglong Qiu¹, Songtao Huang¹, Zihao Yao², Mingxuan Wang¹, Yi Chen¹, Yue Lin³, Xing Zhong¹, Xiaonian Li⁴, Jianguo Wang⁵

Affiliations

¹ Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032, PR China.
² Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032, PR China. yaozihao@zjut.edu.cn.
³ Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China.
⁴ Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032, PR China. xnli@zjut.edu.cn.
⁵ Institute of Industrial Catalysis, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032, PR China. jgw@zjut.edu.cn.

^# Contributed equally.

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.

Abstract

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