Separation and Purification Technology ( IF 8.1 ) Pub Date : 2023-12-21 , DOI: 10.1016/j.seppur.2023.126122 Qianzhen Fang , Ni Liu , Yanling Gu , Hailan Yang , Shujing Ye , Zhongzhus Yang , Gaobin Chen , Xiaofei Tan , Xinjiang Hu
Metal-based materials are widely regarded as promising catalysts for activating peroxymonosulfate (PMS) to remove refractory organic contaminants with high efficiency. In our study, Ni-Fe layered double hydroxide (LDH)-biochar (BC) composite-induced PMS-based advanced oxidation process (AOP) was utilized to elucidate the degradation of tetracycline hydrochloride (TCH). In Ni-Fe LDH-BC/PMS system, more than 99% TCH (45 μM) could be removed effectively at low doses of oxidant (PMS, 0.10 mM) and catalyst (Ni-Fe LDH-BC, 0.10 g/L) addition within 80 min. Besides, the Ni-Fe LDH-BC/PMS system showed high resistance to some inorganic anions, and the Ni-Fe LDH-BC composite possessed excellent reusability in the degradation of TCH (>99% in four cyclic experiments). The reaction mechanisms were investigated via electron paramagnetic resonance detection, chemical quenching tests, probe experiments, and electrochemical measurements. These results indicated that the electron-shuttle mechanism played the dominant role in the removal of TCH. It is worth noting that determination of PMS concentration can reflect the reliability of quenching experiments. In the Ni-Fe LDH-BC composite, BC could not only improve the dispersion of Ni-Fe LDH, but also increase the conductivity of Ni-Fe LDH. Overall, a successful modification strategy was proposed in our study to improve the catalytic property of Ni-Fe LDH, and reaction mechanisms of TCH degradation were discussed deeply and comprehensively.
中文翻译:
Ni-Fe层状双氢氧化物-生物炭/过一硫酸盐体系降解四环素的机理探索:非自由基主导的氧化过程
金属基材料被广泛认为是激活过一硫酸盐(PMS)以高效去除难降解有机污染物的有前途的催化剂。在我们的研究中,利用镍铁层状双氢氧化物(LDH)-生物炭(BC)复合物诱导的基于PMS的高级氧化工艺(AOP)来阐明盐酸四环素(TCH)的降解。在Ni-Fe LDH-BC/PMS体系中,低剂量的氧化剂(PMS,0.10 mM)和催化剂(Ni-Fe LDH-BC,0.10 g/L)即可有效去除99%以上的TCH(45 μM)。 80分钟内添加 此外,Ni-Fe LDH-BC/PMS体系对某些无机阴离子表现出较高的耐受性,并且Ni-Fe LDH-BC复合材料在TCH降解中具有优异的可重复使用性(四次循环实验中>99%)。通过电子顺磁共振检测、化学猝灭测试、探针实验和电化学测量研究了反应机理。这些结果表明电子穿梭机制在TCH的去除中起主导作用。值得注意的是,PMS浓度的测定可以反映猝灭实验的可靠性。在Ni-Fe LDH-BC复合材料中,BC不仅可以改善Ni-Fe LDH的分散性,还可以提高Ni-Fe LDH的电导率。总的来说,我们的研究提出了一种成功的修饰策略来提高Ni-Fe LDH的催化性能,并对TCH降解的反应机制进行了深入而全面的讨论。