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Toward biomass-based single-atom catalysts and plastics: Highly active single-atom Co on N-doped carbon for oxidative esterification of primary alcohols

Hua Zhou#, Song Hong#, Hao Zhang#, Yongting Chen#, Huanghui Xua, Xueke Wang, Zheng Jiang*, Shengli Chen*, Yun Liu*

date: 2019-06-04 20:37      hits:

  Supported single-atom catalysts (SACs) have attracted much attention as their advantageous performances in heterogenous catalysis. Here, we report a general synthesis approach to produce SACs on nitrogen-doped carbon (M SAs-N@C, where M=Fe, Co, Ni, Cu) by engineering bioinspired metal-lignin coordination complexes. The Co SAs-N@C catalyst shows extraordinary reactivity for the oxidative esterification of primary alcohols via aldehyde intermediates, achieving a high turnover frequency (TOF, 55.6mol methyl benzoatemol1Coh1) for benzyle alcohol, which is approx. 18 times of Co nanoparticles. Experiments and theoretical calculations reveal that the atomically dispersed Co species in Co SAs-N@C are active sites for this reaction. As a proof-of-concept, we demonstrate an integrated biorefinery that lignin-based catalyst enables the effective transformation of carbohydrate-derived furans into building block of plastics and fragrance. Our technique not only provides a facile, low-cost and scalable method to atomically dispersed catalysts but also opens new avenue toward lignin valorization and biomass economy.

  https://doi.org/10.1016/j.apcatb.2019.117767