Zhao Gui, Lin Jiayi, Lu Mengying, Li Lina, Xu Pengtao, Liu Xi, Chen Liwei
School of Chemistry and Chemical Engineering, In-situ Center for Physical Sciences, Shanghai Electrochemical Energy Device Research Center (SEED), Shanghai Jiao Tong University, Shanghai, PR China.
Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Shanghai, PR China.
Nat Commun. 2024 Sep 30;15(1):8463. doi: 10.1038/s41467-024-52789-2.
The electrocatalytic valorization of polyethylene terephthalate-derived ethylene glycol to valuable glycolic acid offers considerable economic and environmental benefits. However, conventional methods face scalability issues due to rapid activity decay of noble metal electrocatalysts. We demonstrate that a dynamic potential cycling approach, which alternates the electrode potential between oxidizing and reducing values, significantly mitigates surface deactivation of noble metals during electrochemical oxidation of ethylene glycol. This method enhances catalyst activity by 20 times compared to a constant-potential approach, maintaining this performance for up to 60 h with minimal deactivation. In situ Raman and X-ray absorption spectroscopy show that this effectiveness results from efficient removal of surface oxide during the reaction. The strategy is applicable to polyethylene terephthalate hydrolysates and various noble metals, such as palladium, gold, and platinum, with palladium showing a high conversion rate in recent studies. Our approach offers an efficient and durable method for electrochemical upcycling of biomass-derived compounds.
将聚对苯二甲酸乙二酯衍生的乙二醇电催化转化为有价值的乙醇酸具有可观的经济和环境效益。然而,由于贵金属电催化剂的活性迅速衰减,传统方法面临可扩展性问题。我们证明,一种动态电位循环方法,即在氧化和还原值之间交替电极电位,可显著减轻乙二醇电化学氧化过程中贵金属的表面失活。与恒电位方法相比,该方法将催化剂活性提高了20倍,并在长达60小时内保持这种性能,失活最小。原位拉曼光谱和X射线吸收光谱表明,这种有效性源于反应过程中表面氧化物的有效去除。该策略适用于聚对苯二甲酸乙二酯水解产物和各种贵金属,如钯、金和铂,最近的研究表明钯具有较高的转化率。我们的方法为生物质衍生化合物的电化学升级循环提供了一种高效且持久的方法。