期刊
ACS CATALYSIS
卷 11, 期 16, 页码 10257-10266出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c02099
关键词
subsurface carbon; Ni3ZnC0.7; acetylene semihydrogenation; selectivity; density functional theory (DFT)
资金
- National Natural Science Foundation of China [21676155]
- China Postdoctoral Science Foundation [2020 T130344]
- Shuimu Tsinghua Scholar Program
- Tsinghua National Laboratory for Information Science and Technology
In this study, a novel Ni3ZnC0.7/C catalyst was designed and synthesized to enhance the ethylene selectivity in acetylene semihydrogenation. The results demonstrated that incorporating carbon atoms in subsurface sites significantly improved the selectivity of ethylene while controlling the selectivity of green oil.
For supported metal catalysts, subsurface sites can significantly influence the adsorption and reaction behaviors on surface sites via the electronic effect and geometric effect. Subsurface carbon in PdCx has been proven to be an effective selectivity promoter in acetylene semihydrogenation. Herein, we theoretically calculated the reaction trajectory on Ni3ZnC0.7 and designed a metal-organic framework-layered hydroxide saltderived synthesis strategy for the Ni3ZnC0.7/C catalyst. The formation of the flake-like Ni3ZnC0.7 phase was monitored by in situ X-ray diffraction (XRD) and confirmed by XRD, transmission electron microscopy, and selected area electron diffraction characterizations. In acetylene semihydrogenation, the Ni3ZnC0.7/C catalyst had 85% ethylene selectivity even at 100% acetylene conversion, supporting the conclusions from density functional theory calculations. The green oil selectivity was controlled below 2%. All results indicated that incorporating carbon atoms in the subsurface sites significantly enhanced the ethylene selectivity in acetylene semihydrogenation.
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