Periodate Activation by Contact-Electrification for Organic Pollutant Degradation: Performance and Mechanisms
作者:Senpei Lin, Keyi Li, Yue Lai, Shuwei Sun, Shuigang Wen, Xiaoxue Zhang, Zhen Yu, Yong Yuan · 发表于:ACS ES&T Engineering · 年份:2026 · DOI:10.1021/acsestengg.5c01000 · 被引用次数:3 · 研究领域:Advanced oxidation water treatment、Environmental remediation with nanomaterials、Oxidative Organic Chemistry Reactions
Contact-electro-catalysis (CEC) shows significant potential for integration with advanced oxidation processes (AOPs), but the full scope of its synergistic benefits and underlying mechanisms remains insufficiently elucidated. Here, we developed a CEC-AOP system by leveraging CEC to activate periodate (PI) for the degradation of organic contaminants. The resultant CEC-periodate (CEC-PI) system exhibited outstanding oxidation kinetics ( k obs = 0.053 ± 0.0060 min –1 ) and an oxidant activation efficiency of ∼30% for sulfamethoxazole (SMX) degradation. This CEC-PI system exhibited superior performance compared to CEC integration with other common oxidants (e.g., hydrogen peroxide, peracetic acid, peroxymonosulfate, and peroxydisulfate) for SMX removal under identical conditions. Quenching experiments and electron paramagnetic resonance spectroscopy verified that 1 O 2 and O 2 ·– are the primary reactive oxygen species (ROS) responsible for SMX degradation, with O 2 · – potentially serving as a precursor for 1 O 2 generation. Electrochemical analyses confirmed the essential role of contact electrons in activating the oxidant, while density functional theory calculations demonstrated a significant reduction in the electron-transfer energy barrier between the catalyst and the oxidant due to the CEC process. Furthermore, the system demonstrated low energy consumption, maintained over 90% degradation efficiency after five consecutive cycles, and showed effective removal of multiple o...