Guangdong Provincial Engineering Technology Research Center for Urban Water Cycle and Water Environment Safety, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, PR China; State Environmental Protection Key Laboratory of Microorganism Application and Risk Control, School of Environment, Tsinghua University, Beijing, 100084, PR China.
Shenzhen Zhenheli Ecology & Environment Co., Ltd., Shenzhen, 518052, China.
Chemosphere. 2022 Sep;303(Pt 3):135254. doi: 10.1016/j.chemosphere.2022.135254. Epub 2022 Jun 8.
It is still a huge challenge to prepare cheap and effective composite materials for removing hexavalent chromium (Cr(VI)) in sewage treatment. In this study, a noval co-polymerization of polypyrrole/polyaniline on ferrate modified biochar (Ppy/PANI/FBC) was fabricated via ferrate-promoted pyrolysis and in-situ oxidative polymerization of pyrrole and aniline molecules to effectively remove Cr(VI) from polluted water. The Ppy/PANI/FBC quickly decreased Cr(VI) concentration from 38.92 to 3.92 mg/L within 400 min, with an efficient removal efficiency (89.92%), which was significantly higher than that of FBC (4.75%), Ppy/FBC (72.30%), and PANI/FBC (42.43%). These results are mainly caused by its conjugated connection and well-dispersion of Ppy and PANI on the surface of a carbon-based material. Meanwhile, the experimental results were in line with the pseudo-second-order kinetic and Freundlich models. The Ppy/PANI/FBC is featured by a high capacity of Cr(VI) adsorption (up to 203.71 mg/g). In addition, it could be adopted for efficiently removing Cr(VI) over a wide pH range (4-9) because of the positively charged nitrogen (-NH- and = N-). The sorption mechanisms of Cr(VI) were identified, including electrostatic interaction with surface protonated nitrogen (N), ion exchange between the doped Cl ions and Cr(VI), chemical decrease of the Cr(VI) to Cr(III) by the iron valence cycle and efficient electron transfer of Ppy/PANI/FBC, as well as surface complexation by amine and oxygen-containing groups. More importantly, 97.98% Cr(VI) was efficiently removed in 20 min by coupling a photocatalytic reaction, also providing a novel idea for the practical use of adsorbents in wastewater treatment.
制备廉价且高效的复合材料以去除污水处理中六价铬(Cr(VI))仍然是一个巨大的挑战。在本研究中,通过高铁酸盐促进的热解和吡咯和苯胺分子的原位氧化聚合,制备了聚吡咯/聚苯胺在高铁酸盐改性生物炭(Ppy/PANI/FBC)上的新型共聚体,以有效地从受污染的水中去除 Cr(VI)。Ppy/PANI/FBC 在 400 分钟内将 Cr(VI)浓度从 38.92 快速降低至 3.92mg/L,去除效率(89.92%)非常高,明显高于 FBC(4.75%)、Ppy/FBC(72.30%)和 PANI/FBC(42.43%)。这些结果主要归因于其共轭连接和 Ppy 和 PANI 在碳基材料表面的良好分散。同时,实验结果与准二级动力学和 Freundlich 模型一致。Ppy/PANI/FBC 的 Cr(VI)吸附容量高(高达 203.71mg/g)。此外,由于带正电荷的氮(-NH-和=N-),它可以在较宽的 pH 范围内(4-9)高效去除 Cr(VI)。Cr(VI)的吸附机制包括与表面质子化氮(N)的静电相互作用、掺杂 Cl 离子与 Cr(VI)之间的离子交换、高铁价循环将 Cr(VI)还原为 Cr(III)以及 Ppy/PANI/FBC 的高效电子转移,以及胺和含氧基团的表面络合。更重要的是,通过耦合光催化反应,在 20 分钟内高效去除了 97.98%的 Cr(VI),为吸附剂在废水处理中的实际应用提供了新的思路。