Ultrahigh Metal Content Carbon-Based Catalyst for Efficient Hydrogenation of Furfural: The Regulatory Effect of Glycerol.

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.