Glucose dicarboxylic acid finds widespread applications in medicine and industry, such as cancer treatment, cholesterol reduction, and as a precursor for nylon-66, making it one of the "most valuable biomass-refined products." Recently, a team led by Dr. Zhongshuai Wu from the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, in collaboration with Prof. Jinlong Gong from Tianjin University, Prof. Shizhang Qiao from the University of Adelaide, and Dr. Bo Zhang, an associate researcher at the Dalian Institute of Chemical Physics, has developed a novel glucose electrooxidation reaction catalyzed by a two-dimensional high-entropy D-FeCoNiCu-LDH/NF electrocatalyst. Through the synergistic catalytic mechanism of multiple active sites in the high-entropy material, efficient catalytic conversion of biomass glucose to glucose dicarboxylic acid has been achieved. The findings were published in Energy & Environmental Science.
Traditional methods for glucose dicarboxylic acid production suffer from harsh reaction conditions and low selectivity. Electrocatalytic oxidation technology offers advantages such as mild reaction conditions, no need for additional oxidants, and environmental friendliness. By adjusting parameters such as pH, voltage, and electrocatalyst, the selectivity of glucose dicarboxylic acid can be improved, making it a promising green production process. However, existing electrocatalysts face issues of low activity, susceptibility to deactivation, and poor stability, limiting their further application. Therefore, the key to directed glucose dicarboxylic acid synthesis lies in the development and design of electrocatalysts with high activity, multiple active sites, high stability, and high selectivity. High-entropy materials, with their diverse active sites, hold promise as ideal electrooxidation catalysts for converting biomass resources into high-value chemicals. However, due to the complexity of high-entropy materials, the active centers of their catalytic reactions and the synergistic effects between different elements need further confirmation.
In this study, the research team developed a structurally stable and defect-rich high-entropy layered double hydroxide nanoflake catalyst (D-FeCoNiCu-LDH/NF) grown on nickel foam for catalyzing the multi-electron glucose electrooxidation reaction. This catalyst achieved a current density of 100 mA/cm² with a voltage of only 1.22V vs. RHE, with glucose conversion close to 100% and a glucose dicarboxylic acid yield exceeding 90%. The catalyst utilizes various types of active sites in the high-entropy material to synergistically catalyze the rapid glucose electrooxidation reaction. Based on this, the team coupled the high-value, low-potential anodic glucose electrooxidation reaction with cathodic nitrate reduction reaction to develop a GOR||NO3-RR flow electrolysis cell. When the current densities of this cell reached 10 and 100 mA/cm², the voltages were only 1.07 and 1.32V, respectively.
This work achieves the simultaneous production of glucose dicarboxylic acid and ammonia with low energy consumption, providing a new approach for the energy-saving and environmentally friendly production of high-value chemicals.
[Related Paper: https://doi.org/10.1039/D4EE00221K]
