Electrocatalytic cleavage of a lignin β-O-4 model compound and coupling with nitrogen-containing aromatics using Prussian blue analogue-derived nickel–cobalt spinel  

作　　者：Yi Qi Xueying Chen Bowen Liu Xuliang Lin Xueqing Qiu Yanlin Qin 

机构地区：[1]Guangdong Provincial Key Laboratory of Plant Resources Biorefinery,School of Chemical Engineering and Light Industry,Guangdong University of Technology,Guangzhou 510006,Guangdong,China [2]Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center,Jieyang 515200,Guangdong,China [3]Guangdong Basic Research Center of Excellence for Ecological Security and Green Development,Guangdong University of Technology,Guangzhou 510006,Guangdong,China

出　　处：《Journal of Energy Chemistry》2025年第1期628-636,共9页能源化学(英文版)

基　　金：National Natural Science Foundation of China (U23A6005 and 22078069);Project funded by China Postdoctoral Science Foundation (GZB20230172 and 2023M740748)。

摘　　要：Electrochemical conversion of lignin for the production of high-value heterocyclic aromatic compounds has great potential.We demonstrate the targeted synthesis and cation modulation of NiCo_(2)O_(4)spinel nanoboxes,synthesized via cation exchange and calcination oxidation.These catalysts exhibit excellent efficacy in the electrocatalytic conversion of lignin model compounds,specifically 2-phenoxy-1-phenylethanol,into nitrogen-containing aromatics,achieving high conversion rates and selectivities.These catalysts were synthesized via a cation exchange and calcination oxidation process,using Prussian blue nanocubes as precursors.The porous architecture and polymetallic composition of the NiCo_(2)O_(4)spinel demonstrated superior performance in electrocatalytic oxidative coupling,achieving a 99.2 wt%conversion rate of the 2-phenoxy-1-phenylethanol with selectivities of 37.5 wt%for quinoline derivatives and 31.5 wt%for phenol.Key innovations include the development of a sustainable one-pot synthesis method for quinoline derivatives,the elucidation of a multistage reaction pathway involving CAO bond cleavage,hydroxyaldol condensation,and CAN bond formation,and a deeper mechanistic understanding derived from DFT simulations.This work establishes a new strategy for lignin valorization,offering a sustainable route to produce high-value nitrogen-containing aromatics from renewable biomass under mild conditions,without the need for additional reagents.

关 键 词：SPINEL Biomass valorization Electrocatalysis Lignin oxidation Coupling 

分 类 号：O62[理学—有机化学]