National Engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology, Beijing University of Technology, Beijing, 100124, PR China.
National Engineering Laboratory for Advanced Municipal Wastewater Treatment and Reuse Technology, Beijing University of Technology, Beijing, 100124, PR China.
Chemosphere. 2021 Nov;283:131257. doi: 10.1016/j.chemosphere.2021.131257. Epub 2021 Jun 18.
The development of new heterogeneous Cu-based solid catalysts for hydroxyl radical (∙OH) generation plays a crucial role in degradation of pollutants at neutral pH circumstance. In this work, a Cu-doped graphitic carbon nitride (g-CN) complex was synthesized in one-step pyrolysis process using copper chloride dihydrate and dicyandiamide as precursors. The results reveal that after Cu doping, the bulk structure of g-CN was destroyed with fragmentary morphology formation. Besides, Cu and Cu were successfully embedded in g-CN sheet. Moreover, amoxicillin (AMX) removal by heterogeneous electro-Fenton process was performed to evaluate the catalytic activity of the Cu-doped g-CN. 99.1% AMX removal efficiency was obtained after 60 min electrolysis under neutral pH condition when the current density was 12 mA cm and the catalyst dosage was 0.3 g L. Both Cu and Cu were stably retained in the Cu-doped g-CN catalyst and AMX removal efficiency reached 91.1%, even after 5 cycles, manifesting the remarkable stability of Cu-doped g-CN. Also, Cu-doped g-CN possessed excellent catalytic activities for AMX removal in various waterbodies. According to the catalytic mechanism analysis, the ∙OH was proved to be the primary reactive species for AMX removal in heterogeneous electro-Fenton process. Based on the identification of sixteen different intermediate products, the possible degradation pathways were proposed. This work provides a simple method to synthesize a Cu-based solid catalyst containing stable Cu and Cu for degradation of pollutants in wastewater.
新型异质 Cu 基固体催化剂的开发对于在中性 pH 条件下污染物的降解起着至关重要的作用。在这项工作中，采用一步热解法，以二水合氯化铜和双氰胺为前驱体，合成了一种 Cu 掺杂石墨相氮化碳（g-CN）复合物。结果表明，Cu 掺杂后，g-CN 的体相结构被破坏，形成了碎片形貌。此外，Cu 和 Cu 成功地嵌入了 g-CN 片层中。此外，通过非均相电芬顿法去除阿莫西林（AMX）来评估 Cu 掺杂 g-CN 的催化活性。在中性 pH 条件下，电流密度为 12 mA·cm 和催化剂用量为 0.3 g·L 时，经过 60 min 电解，AMX 的去除率达到 99.1%。Cu 和 Cu 都稳定地保留在 Cu 掺杂的 g-CN 催化剂中，即使经过 5 次循环，AMX 的去除效率仍达到 91.1%，表明 Cu 掺杂的 g-CN 具有显著的稳定性。此外，Cu 掺杂的 g-CN 在各种水体中对 AMX 的去除具有优异的催化活性。根据催化机理分析，证明了在非均相电芬顿过程中，·OH 是 AMX 去除的主要活性物质。通过鉴定出的十六种不同的中间产物，提出了可能的降解途径。这项工作为合成含有稳定的 Cu 和 Cu 的用于废水处理的 Cu 基固体催化剂提供了一种简单的方法。
