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Cu-doped g-C3N4 catalyst with stable Cu0 and Cu+ for enhanced amoxicillin degradation by heterogeneous electro-Fenton process at neutral pH
Chemosphere ( IF 8.8 ) Pub Date : 2021-06-18 , DOI: 10.1016/j.chemosphere.2021.131257
Guifang Pan 1 , Zhirong Sun 1
Affiliation  

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-C3N4) 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-C3N4 was destroyed with fragmentary morphology formation. Besides, Cu0 and Cu+ were successfully embedded in g-C3N4 sheet. Moreover, amoxicillin (AMX) removal by heterogeneous electro-Fenton process was performed to evaluate the catalytic activity of the Cu-doped g-C3N4. 99.1% AMX removal efficiency was obtained after 60 min electrolysis under neutral pH condition when the current density was 12 mA cm2 and the catalyst dosage was 0.3 g L−1. Both Cu0 and Cu+ were stably retained in the Cu-doped g-C3N4 catalyst and AMX removal efficiency reached 91.1%, even after 5 cycles, manifesting the remarkable stability of Cu-doped g-C3N4. Also, Cu-doped g-C3N4 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 Cu0 and Cu + for degradation of pollutants in wastewater.



中文翻译:

具有稳定 Cu0 和 Cu+ 的 Cu 掺杂 g-C3N4 催化剂在中性 pH 条件下通过非均相电芬顿法增强阿莫西林降解

用于羟基自由基(∙OH)生成的新型多相铜基固体催化剂的开发在中性 pH 值环境下降解污染物中起着至关重要的作用。在这项工作中,使用氯化铜二水合物和双氰胺作为前驱体,通过一步热解工艺合成了掺杂铜的石墨氮化碳 (gC 3 N 4 ) 配合物。结果表明,Cu掺杂后,gC 3 N 4的块体结构被破坏,形成碎片状形态。此外,Cu 0和Cu +成功嵌入gC 3 N 4床单。此外,通过非均相电芬顿法去除阿莫西林(AMX)以评估Cu掺杂的gC 3 N 4的催化活性。当电流密度为12 mA cm 2和催化剂用量为0.3 g L -1时,在中性pH条件下电解60分钟后获得99.1%的AMX去除率。Cu 0和Cu +均稳定地保留在Cu掺杂的gC 3 N 4催化剂中,即使经过5个循环,AMX去除效率也达到91.1%,表明Cu掺杂的gC 3 N 4具有显着的稳定性。此外,Cu 掺杂 gC 3 N 4对各种水体中的 AMX 去除具有优异的催化活性。根据催化机理分析,证明∙OH是非均相电芬顿过程中去除AMX的主要反应物种。基于对 16 种不同中间产物的鉴定,提出了可能的降解途径。该工作为合成含有稳定Cu 0和Cu  +的Cu基固体催化剂 用于废水中污染物降解提供了一种简单的方法。

更新日期:2021-06-21
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