Ultrahigh Metal Content Carbon-Based Catalyst for Efficient Hydrogenation of Furfural: The Regulatory Effect of
Zhouxiao Zhai1, Jie Chu1, Lu Sun1
1Key Laboratory of Forest Resources Conservation and Utilization in the Southwest Mountains of China Ministry of Education, School of Chemical Engineering, Southwest Forestry University, Kunming 650051, P. R. China.
Abstract:
The development of high-content non-noble metal nanocatalysts is important for multiphase catalysis applications. However, it is a challenge to solve the agglomeration in the preparation of high-content metal catalysts. In this paper, a carbon-based catalyst (Co@CN-G-600) with 71.28 wt % cobalt metal content was prepared using a new strategy of gas-phase carbon coating assisted by glycerol. The core of this strategy is to maintain the spacing of metallic cobalt by continuous replenishment of dissociated ligands during pyrolysis over gas-phase glycerol. This approach is also applicable to other non-noble metals. When Co@CN-G-600 was further used as a catalyst for the selective hydrogenation of furfural (FF) to prepare furfuryl alcohol (FOL), the yield of FOL was >99.9% under mild conditions of 80 °C, compared to only 8.23% catalytic yield at up to 130 °C for Co@CN-600 without glycerol. The excellent catalytic performance mainly lies in the fact that the introduction of glycerol modulates the size effect, electronic effect, and acidic site intensity of the high-content Co catalyst, which promotes the activation of FF and hydrogen. Meanwhile, the optimized specific surface area and pore structure by glycerol improve the accessibility of high-density active sites and promote more efficient mass transfer. In addition, the introduction of glycerol produced a graphitic carbon layer encapsulation structure relative to Co@CN-600, which substantially improved the cycling stability of the catalyst. This study resolves the paradox of high content and high dispersion of non-noble metal catalysts in the synthesis process and provides a general pathway and example for the preparation of stable high-content metal catalysts.
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