Chen Yan, Jia Chenghao, Zhou Chenyu, Wu Shiying, Xiang Xuepeng, Zhang Nian, Zhao Shijun, Lin Zhang
Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, School of Environment and Energy, South China University of Technology, Guangzhou, 510006, P.R. China.
School of Metallurgy and Environment, Central South University, Changsha, Hunan, 410083, P.R. China.
Angew Chem Int Ed Engl. 2025 Aug 25:e202513447. doi: 10.1002/anie.202513447.
Electrocatalytic upcycling of waste polyester plastics into valuable organic acids offers a dual solution for mitigating plastic pollution and promoting sustainable carbon cycling. However, practical implementation remains limited by the scarcity of cost-effective and high-performance electrocatalysts. In this work, we investigate MCoO (where M═Mn, Fe, Co, Cu, and Ni) as model catalysts and identify lattice oxygen activity as a critical factor governing the electrochemical upgrading of waste polyethylene terephthalate (PET). NiCoO demonstrates the highest oxygen activity, characterized by the greatest density of O 2p ligand holes and the closest proximity of the O 2p band center to the Fermi level. Such unique character facilitates lattice oxygen participation in surface electro-oxidation reactions, leading to exceptional performance of up to 98.3% formate selectivity and 98.9% Faraday efficiency, among the highest values reported for transition metal catalysts in alcohol electro-oxidation. We further demonstrate the direct electrocatalytic upcycling of real waste PET plastics, estimating a $739 profit per ton of recycled PET and confirming its economic viability. These results provide critical insights for refining the design principles of electrocatalytic systems aimed at recycling diverse waste materials and pollutants.
将废弃聚酯塑料电催化升级转化为有价值的有机酸，为减轻塑料污染和促进可持续碳循环提供了双重解决方案。然而，实际应用仍受限于缺乏经济高效的高性能电催化剂。在这项工作中，我们研究了MCoO（其中M = Mn、Fe、Co、Cu和Ni）作为模型催化剂，并确定晶格氧活性是控制废弃聚对苯二甲酸乙二酯（PET）电化学升级的关键因素。NiCoO表现出最高的氧活性，其特征在于O 2p配体空穴密度最大且O 2p能带中心最接近费米能级。这种独特的特性促进了晶格氧参与表面电氧化反应，在醇类电氧化中，其甲酸盐选择性高达98.3%，法拉第效率高达98.9%，在过渡金属催化剂中达到了已报道的最高值之一。我们进一步展示了真实废弃PET塑料的直接电催化升级，估计每吨回收PET可获利739美元，并证实了其经济可行性。这些结果为完善旨在回收各种废料和污染物的电催化系统设计原则提供了关键见解。
