Wu Haoran, Song Jinliang, Liu Huizhen, Xie Zhenbing, Xie Chao, Hu Yue, Huang Xin, Hua Manli, Han Buxing
Beijing National Laboratory for Molecular Science , CAS Key Laboratory of Colloid and Interface and Thermodynamics , CAS Research/Education Center for Excellence in Molecular Sciences , Institute of Chemistry , Chinese Academy of Sciences , Beijing 100190 , China . Email:
School of Chemistry and Chemical Engineering , University of Chinese Academy of Sciences , Beijing 100049 , China.
Chem Sci. 2019 Mar 25;10(17):4692-4698. doi: 10.1039/c9sc00322c. eCollection 2019 May 7.
Development of efficient strategies for biomass valorization is a highly attractive topic. Herein, we conducted the first work on electrocatalytic oxidation of renewable furfural to produce the key bioactive intermediate 5-hydroxy-2(5)-furanone (HFO). It was demonstrated that using HO as the oxygen source and metal chalcogenides (CuS, ZnS, PbS, ) as electrocatalysts, the reaction could proceed efficiently, and the CuS nanosheets prepared in this work showed the best performance and provided high HFO selectivity (83.6%) and high conversion (70.2%) of furfural. In addition, the CuS electrocatalyst showed long-term stability. Mechanism investigation showed that furfural was oxidized to HFO multistep reactions, including C-C cleavage, subsequent ring opening and oxidation, and intramolecular isomerization.
开发高效的生物质增值策略是一个极具吸引力的课题。在此，我们首次开展了将可再生糠醛电催化氧化以制备关键生物活性中间体5-羟基-2(5)-呋喃酮（HFO）的工作。结果表明，以HO作为氧源，金属硫族化物（CuS、ZnS、PbS等）作为电催化剂，该反应能够高效进行，并且本工作制备的CuS纳米片表现出最佳性能，糠醛的HFO选择性高（83.6%）、转化率高（70.2%）。此外，CuS电催化剂表现出长期稳定性。机理研究表明，糠醛通过多步反应被氧化为HFO，包括C-C键断裂、随后的开环和氧化以及分子内异构化。
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