State Key Laboratory of Chemo/Biosensing and Chemometrics, Hunan University, Changsha 410082, PR China.
Brook Byers Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, 828 West Peachtree Street, Atlanta, GA 30332, United States.
J Hazard Mater. 2018 Sep 15;358:294-301. doi: 10.1016/j.jhazmat.2018.06.064. Epub 2018 Jul 3.
Although noble metal electrocatalysts are highly efficient in the dehalogenation of halogenated antibiotics, the prohibitive cost hinders their practical applications. In this study, a cobalt-phosphorous/oxide (CoP/O) composite prepared via a one-step electrodeposition was for the first time applied in electroreductive dechlorination of halogenated antibiotics (HA), including chloramphenicol (CAP), florfenicol (FLO) and thiamphenicol (TAP). CoP/O had a higher FLO dechlorination efficiency (91%) than Pd/C (69.3%) (t = 60 min, C = 20 mg L, applied voltage of -1.2 V vs. saturated calomel electrode (SCE)). Furthermore, the dechlorination efficiencies of CoP/O for CAP and TAP reached to 98.7 and 74.2%, respectively. The electron spin resonance and in situ Raman characterizations confirmed that atomic H* was produced via the CoP and the formation of CoCl bonds occurred on the CoO in CoP/O. The CoCl bond formation could trap HA molecules onto CoP/O and weaken the CCl bond strength. The synergistic effect of H* attack and CoCl bond was responsible for the high dechlorination efficiency. This study offers new insights into the interface mechanism of electroreductive dehalogenation process, and shows a great potential for the remediation of halogenated antibiotics contaminated wastewater.
虽然贵金属电催化剂在卤代抗生素的脱卤反应中具有很高的效率,但高昂的成本阻碍了它们的实际应用。在这项研究中,首次将通过一步电沉积制备的钴-磷/氧化物(CoP/O)复合材料应用于卤代抗生素(HA)的电还原脱卤反应中,包括氯霉素(CAP)、氟苯尼考(FLO)和甲砜霉素(TAP)。CoP/O 对 FLO 的脱氯效率(91%)高于 Pd/C(69.3%)(t=60min,C=20mg/L,施加电压为-1.2V 相对于饱和甘汞电极(SCE))。此外,CoP/O 对 CAP 和 TAP 的脱氯效率分别达到 98.7%和 74.2%。电子顺磁共振和原位拉曼特性证实,原子 H是通过 CoP 产生的,而 CoP/O 中形成了 CoCl 键。CoCl 键的形成可以将 HA 分子捕获到 CoP/O 上,并削弱 CCl 键的强度。H攻击和 CoCl 键的协同作用是高脱氯效率的原因。本研究为电还原脱卤过程的界面机制提供了新的见解,并展示了在处理卤代抗生素污染废水方面的巨大潜力。