Li Jianfei, Lan Huachun, Liu Huijuan, Zhang Gong, An Xiaoqiang, Liu Ruiping, Qu Jiuhui
State Key Laboratory of Drinking Water Science and Technology , Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences , Beijing 100085 , China.
University of Chinese Academy of Sciences , Beijing 100039 , China.
ACS Appl Mater Interfaces. 2019 May 1;11(17):15709-15717. doi: 10.1021/acsami.9b03409. Epub 2019 Apr 17.
As a robust reducing system in industrial wastewater treatment, iron/carbon (Fe/C) microelectrolysis suffers from surface passivation and low utilization efficiency. Herein, we introduced FeC into the Fe/C system to develop a core-shell Fe/FeC/C nanorod with a multifunctional interface (FeC/C) providing reduction, catalysis, adsorption, and corrosion resistance. The results proved that the fabricated Fe/FeC/C possesses 5.6 times higher reduction capacity (220 mg/g) for Cr(VI) reduction but a relatively lower Fe leakage (2.7 mg/L) than Fe/C. On the basis of the results of electrochemical characterization (Tafel polarization curves and electrochemical impedance spectroscopy), the corrosion-resistant FeC/C shell can significantly prevent surface passivation of the Fe core, whereas FeC efficiently catalyzes electron transfer from the inner Fe to the external carbon surface. Moreover, the reductive species involved in Cr(VI) removal were identified as hydrogen atoms, adsorbed Fe(II) ions, and electrons tunneling from Fe. STEM, XPS, and Mössbauer spectroscopies were further adopted to characterize the interface reaction of Fe/FeC/C during the Cr(VI) removal process. Finally, the reaction mechanism for Cr(VI) reduction over Fe/FeC/C was proposed, and the distribution of active sites was inferred.
作为工业废水处理中一种强大的还原系统,铁/碳(Fe/C)微电解存在表面钝化和利用效率低的问题。在此,我们将FeC引入Fe/C系统,以开发一种具有多功能界面(FeC/C)的核壳型Fe/FeC/C纳米棒,该界面具有还原、催化、吸附和耐腐蚀性能。结果表明,制备的Fe/FeC/C对Cr(VI)还原的还原容量(220 mg/g)比Fe/C高5.6倍,但铁泄漏量(2.7 mg/L)相对较低。基于电化学表征(塔菲尔极化曲线和电化学阻抗谱)的结果,耐腐蚀的FeC/C壳层可以显著防止Fe核的表面钝化,而FeC则有效地催化电子从内部Fe转移到外部碳表面。此外,确定了参与去除Cr(VI)的还原物种为氢原子、吸附的Fe(II)离子和从Fe隧穿的电子。进一步采用扫描透射电子显微镜(STEM)、X射线光电子能谱(XPS)和穆斯堡尔谱来表征Fe/FeC/C在Cr(VI)去除过程中的界面反应。最后,提出了Fe/FeC/C上Cr(VI)还原的反应机理,并推断了活性位点的分布。