Huang Yuan, Yan Haoting, Zhang Chenyang, Wang Yize, Wei Qinhong, Zhang Renkun
Department of Chemical Engineering, School of Petrochemical Engineering & Environment, Zhejiang Ocean University, Zhoushan 316022, China.
Nanomaterials (Basel). 2021 Oct 20;11(11):2776. doi: 10.3390/nano11112776.
Metal-supported catalyst with high activity and relatively simple preparation method is given priority to industrial production. In this work, this study reported an easily accessible synthesis strategy to prepare Mott-Schottky-type N-doped carbon encapsulated metallic Co (Co@NC) catalyst by high-temperature pyrolysis method in which carbon nitride (g-CN) and dopamine were used as support and nitrogen source. The prepared Co@NC presented a Mott-Schottky effect; that is, a strong electronic interaction of metallic Co and N-doped carbon shell was constructed to lead to the generation of Mott-Schottky contact. The metallic Co, due to high work function as compared to that of N-doped carbon, transferred electrons to the N-doped outer shell, forming a new contact interface. In this interface area, the positive and negative charges were redistributed, and the catalytic hydrogenation mainly occurred in the area of active charges. The Co@NC catalyst showed excellent catalytic activity in the hydrogenation of phenylacetylene to styrene, and the selectivity of styrene reached 82.4%, much higher than those of reference catalysts. The reason for the promoted semi-hydrogenation of phenylacetylene was attributed to the electron transfer of metallic Co, as it was caused by N doping on carbon.
具有高活性且制备方法相对简单的金属负载型催化剂优先用于工业生产。在本工作中，本研究报道了一种易于实现的合成策略，通过高温热解法制备莫特-肖特基型氮掺杂碳包覆金属钴（Co@NC）催化剂，其中氮化碳（g-CN）和多巴胺用作载体和氮源。制备的Co@NC呈现出莫特-肖特基效应；也就是说，构建了金属Co与氮掺杂碳壳之间的强电子相互作用，导致莫特-肖特基接触的产生。与氮掺杂碳相比，金属Co由于功函数高，将电子转移到氮掺杂的外壳，形成新的接触界面。在该界面区域，正电荷和负电荷重新分布，催化氢化主要发生在活性电荷区域。Co@NC催化剂在苯乙炔加氢制苯乙烯反应中表现出优异的催化活性，苯乙烯选择性达到82.4%，远高于参考催化剂。苯乙炔半加氢反应得到促进的原因归因于金属Co的电子转移，这是由碳上的氮掺杂引起的。
