Microfluidic Flow through Polyaniline Supported by Lamellar-Structured Graphene for Mass-Transfer-Enhanced Electrocatalytic Reduction of Hexavalent Chromium

聚苯胺 材料科学 六价铬 电极 石墨烯 传质 化学工程 分析化学(期刊) 电化学 动力学 化学 纳米技术 复合材料 物理化学 色谱法 冶金 物理 工程类 聚合 聚合物 量子力学
作者
Qinghua Ji,Dawei Yu,Gong Zhang,Huachun Lan,Huijuan Liu,Jiuhui Qu
出处
期刊:Environmental Science & Technology [American Chemical Society]
卷期号:49 (22): 13534-13541 被引量:104
标识
DOI:10.1021/acs.est.5b03314
摘要

Owing to its high efficiency and environmental compatibility, electroreduction holds great promise for the detoxification of aqueous Cr(VI). However, the typical electroreduction system often shows poor mass transfer, which results in slow reduction kinetics and hence higher energy consumption. Here, we demonstrate a flow-through electrode of polyaniline supported on lamellar-structured graphene (LGS–PANI) for electrocatalytic reduction of Cr(VI). The reaction kinetics of the LGS–PANI flow-through electrodes are 6.4 times (at acidic condition) and 17.3 times (at neutral condition) faster than traditional immersed parallel-plate electrodes. Computational fluid dynamics simulation suggests that the flow-through mode greatly enhances the mass transfer and that the nanoscale convection induced by the PANI nanodots increases the nanoscale mass transport in the interfacial region of the electrode/solution. In situ Raman spectroscopy shows that the PANI–Cr(VI) redox reactions are dominated by the leucoemeraldine/emeraldine transition at 1.5 V cell voltage, which also remarkably contributes to the fast reaction kinetics. Using single-pass flow-through mode, the LGS–PANI electrode reaches an average reduction efficiency of 99.8% with residual Cr(VI) concentration of 22.3 ppb (initial [Cr(VI)] = 10 ppm, flux = 20 L h–1 m–2). A long-term stability test shows that the LGS–PANI maintains stable performance over 40 days of operation and achieves >98% reduction efficiency, with average current efficiency of as high as 99.1% (initial [Cr(VI)] = 10 ppm, flux = 50 L h–1 m–2).
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