Manipulating interstitial carbon atoms in the nickel octahedral site for highly efficient hydrogenation of alkyne

Yiming Niu, Xing Huang, Yongzhao Wang, Ming Xu, Junnan Chen, Shuliang Xu, Marc-Georg Willinger, Wei Zhang (), Min Wei () and Bingsen Zhang ()
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Yiming Niu: Chinese Academy of Sciences
Xing Huang: Fritz Haber Institute of the Max Planck Society
Yongzhao Wang: Chinese Academy of Sciences
Ming Xu: Beijing University of Chemical Technology
Junnan Chen: Chinese Academy of Sciences
Shuliang Xu: Chinese Academy of Sciences
Marc-Georg Willinger: Fritz Haber Institute of the Max Planck Society
Wei Zhang: Jilin University
Min Wei: Beijing University of Chemical Technology
Bingsen Zhang: Chinese Academy of Sciences

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Light elements in the interstitial site of transition metals have strong influence on heterogeneous catalysis via either expression of surface structures or even direct participation into reaction. Interstitial atoms are generally metastable with a strong environmental dependence, setting up giant challenges in controlling of heterogeneous catalysis. Herein, we show that the desired carbon atoms can be manipulated within nickel (Ni) lattice for improving the selectivity in acetylene hydrogenation reaction. The radius of octahedral space of Ni is expanded from 0.517 to 0.524 Å via formation of Ni3Zn, affording the dissociated carbon atoms to readily dissolve and diffuse at mild temperatures. Such incorporated carbon atoms coordinate with the surrounding Ni atoms for generation of Ni3ZnC0.7 and thereof inhibit the formation of subsurface hydrogen structures. Thus, the selectivity and stability are dramatically improved, as it enables suppressing the pathway of ethylene hydrogenation and restraining the accumulation of carbonaceous species on surface.

Date: 2020
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DOI: 10.1038/s41467-020-17188-3

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