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Enhanced hydrodechlorination of p-chloronitrobenzene by a GAC-Fe-Cu ternary micro-electrolysis system: Synergistic effects and removal mechanism
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2019-12-10 , DOI: 10.1016/j.seppur.2019.116391
Zhihua Xu , Zhenhua Sun , Yuwei Zhou , Daofang Zhang , Yuquan Gao , Yuanxing Huang , Weifang Chen

A ternary micro-electrolysis system composed of a granular activated carbon (GAC) supported Fe0 and Cu0 nanocomposite (GAC-Fe-Cu) was synthesized for the removal of p-chloronitrobenzene (p-CNB). GAC-Fe-Cu exhibited excellent reusability and stability based on the stably anchored nanoparticles and the inner tailored Fe0 with persistent activity. A two-stage reaction revealed the simultaneous adsorption and degradation in the process of p-CNB removal, and the iron corrosion reaction mainly dominated the latter. A stepwise reduction of p-CNB was observed, where the main intermediates, such as p-chloroaniline (p-CAN) and aniline (AN), were formed in sequence. Furthermore, the mechanism of p-CNB removal could be explained by the synergistic effects of GAC-Fe-Cu. p-CNB could be rapidly adsorbed onto the surface of the system for in situ reduction. The conductive GAC cathode pre-accepted the released electrons from the Fe0 anode, and transferred them to the Cu0 cathode. Then, the electron-rich Cu0 cathode could intensively release electrons to form the “point discharge” phenomenon, which possessed strong reducing power to dramatically increase the hydrodechlorination rate of p-CAN. Additionally, the -C-OH and -COOH on the GAC surface could absorb p-CAN through electrostatic interactions with the amine group (-NH2), facilitating the selectivity of p-CAN dechlorination.



中文翻译:

GAC-Fe-Cu三元微电解系统增强对氯硝基苯的加氢脱氯作用:协同作用和去除机理

合成了由颗粒状活性炭(GAC)负载的Fe 0和Cu 0纳米复合材料(GAC-Fe-Cu)组成的三元微电解系统,用于去除对氯硝基苯(p-CNB)。GAC-Fe-Cu基于稳定的纳米颗粒和内部定制的Fe 0表现出优异的可重复使用性和稳定性持续的活动。两步反应表明,在去除p-CNB的过程中同时发生吸附和降解,而铁腐蚀反应则主要是后者。观察到p-CNB的逐步减少,其中依次形成了主要中间体,例如对氯苯胺(p-CAN)和苯胺(AN)。此外,可以通过GAC-Fe-Cu的协同作用来解释p-CNB的去除机理。p-CNB可以迅速吸附到系统表面进行原位还原。导电的GAC阴极预先接受从Fe 0阳极释放的电子,并将其转移到Cu 0阴极。然后,富电子的Cu 0阴极可以强烈释放电子以形成“点放电”现象,该现象具有很强的还原能力,可以大大提高p-CAN的加氢脱氯速率。此外,GAC表面的-C-OH和-COOH可以通过与胺基(-NH 2)的静电相互作用吸收p-CAN ,从而促进p-CAN脱氯的选择性。

更新日期:2019-12-11
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