Subsurface Carbon as a Selectivity Promotor to Enhance Catalytic Performance in Acetylene Semihydrogenation,ACS Catalysis

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Subsurface Carbon as a Selectivity Promotor to Enhance Catalytic Performance in Acetylene Semihydrogenation
ACS Catalysis ( IF 11.3 ) Pub Date : 2021-08-03 , DOI: 10.1021/acscatal.1c02099
Yu Wang ₁ , Boyang Liu ₁ , Xiaocheng Lan ₁ , Tiefeng Wang ₁

Affiliation

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 PdC_x has been proven to be an effective selectivity promoter in acetylene semihydrogenation. Herein, we theoretically calculated the reaction trajectory on Ni₃ZnC_0.7 and designed a metal–organic framework-layered hydroxide salt-derived synthesis strategy for the Ni₃ZnC_0.7/C catalyst. The formation of the flake-like Ni₃ZnC_0.7 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 Ni₃ZnC_0.7/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.

中文翻译：

亚表面碳作为选择性促进剂以提高乙炔半氢化中的催化性能

对于负载型金属催化剂，亚表面位点可以通过电子效应和几何效应显着影响表面位点的吸附和反应行为。PdC _x中的亚表面碳已被证明是乙炔半氢化中有效的选择性促进剂。在此，我们从理论上计算了 Ni ₃ ZnC _0.7上的反应轨迹，并为 Ni ₃ ZnC _0.7 /C 催化剂设计了金属-有机骨架层状氢氧化物盐衍生合成策略。片状Ni ₃ ZnC _{0.7 的形成}通过原位 X 射线衍射 (XRD) 监测相，并通过 XRD、透射电子显微镜和选区电子衍射表征证实。在乙炔半加氢反应中，Ni ₃ ZnC _0.7 /C 催化剂即使在 100% 乙炔转化率下也具有 85% 的乙烯选择性，这支持了密度泛函理论计算的结论。绿油选择性控制在2%以下。所有结果表明，在亚表面位点引入碳原子显着提高了乙炔半氢化中的乙烯选择性。

更新日期：2021-08-20

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