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Cu-Doped CoZn@NC promotes catalytic activity of furfural hydrogenation at low temperature: Regulation of copper
Molecular Catalysis ( IF 4.6 ) Pub Date : 2024-03-29 , DOI: 10.1016/j.mcat.2024.114084
Siyi Pu , Lu Sun , Chunyan Yang , Jie Chu , Ying Wang , Chungang Min , Xiaoqin Zou , Changfu Zhuang

The low-cost Cu-based catalysts have excellent selectivity in biomass hydrogenation, but it is challenging to improve their catalytic activity at low temperature. Herein, the trimetallic CuCoZn@NC (where = 0.1, 0.3, 0.5 mmol is the molar mass of Cu) were prepared by in suit pyrolysis using trimesic acid with stronger coordination ability. When it was applied to the furfural (FF) selective hydrogenation process, the catalytic yield of the optimal CuCoZn@NC reached >99 % under mild condition of 90 °C, which was 29 times superior to that of the CoZn@NC without Cu doping. The results demonstrate that the doping of Cu reduces the activation energy of CuCoZn@NC and increases the catalytic activity at low temperature relative to CoZn@NC. The characterizations and density functional theory (DFT) calculations show that the incorporation of suitable Cu content enhances the interaction between Cu and Co. The amount of surface-active Co and the electron density are significantly enhanced, which effectively stimulates the dissociation of hydrogen. Moreover, the Lewis acid content is significantly increased to facilitate the adsorption and activation of FF. Meanwhile, the impact of Cu content variation on the performance of the multi-metal catalyst is discussed. This work is promising to establish a foundation for the accurate design of polymetallic catalysts through adjusting the Cu content to regulate the reaction activity and selectivity.

中文翻译:

Cu掺杂CoZn@NC促进低温糠醛加氢催化活性:铜的调控

低成本的铜基催化剂在生物质加氢中具有优异的选择性,但提高其低温催化活性具有挑战性。本文利用具有较强配位能力的均苯三酸,通过适当热解制备了三金属CuCoZn@NC(其中= 0.1、0.3、0.5 mmol为Cu的摩尔质量)。当应用于糠醛(FF)选择性加氢过程时,最优的CuCoZn@NC在90℃温和条件下催化产率达到>99%,是未掺杂Cu的CoZn@NC的29倍。结果表明,相对于 CoZn@NC,Cu 的掺杂降低了 CuCoZn@NC 的活化能,并提高了低温催化活性。表征和密度泛函理论(DFT)计算表明,合适的Cu含量的加入增强了Cu和Co之间的相互作用。表面活性Co的量和电子密度显着增强,有效地刺激了氢的解离。而且路易斯酸含量显着增加,有利于FF的吸附和活化。同时,讨论了Cu含量变化对多金属催化剂性能的影响。这项工作有望通过调节铜含量来调节反应活性和选择性,为多金属催化剂的精确设计奠定基础。
更新日期:2024-03-29
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