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One-pot synthesis of nitrogen-enriched carbon spheres for hexavalent chromium removal from aqueous solution

机译：一锅合成富氮碳球以从水溶液中去除六价铬

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Nitrogen-enriched carbon spheres (NECS) were obtained after ZnCl2 activation of high-nitrogen-content polymer spheres prepared by one-pot hydrothermal synthesis using m-phenylenediamine and hexamethylenetetramine as raw materials. The NECS were characterized by SEM, BET, FT-IR, and XPS. It was found that the NECS possessed homogeneously spherical morphology with diameters of about 0.6-1.2 mm and a high specific surface area (1237 m(2) g(-1)). Elemental analysis indicated that the nitrogen content of NECS was up to 10.21 wt%. When the hexavalent chromium (Cr(VI)) in acidic solution was used to evaluate the adsorption performance, the maximum Cr(VI) removal capacity was as high as 279 mg g(-1) at pH 2.0. The pseudo-second-order and Freundlich model fitted the Cr(VI) adsorption behavior well. Based on zeta potential and XPS analysis, the Cr(VI) removal mechanism was proposed to be electrostatic adsorption of Cr(VI) anions on the NECS surface at low pH, followed by a reduction reaction of Cr(VI) to Cr(III) via the nitrogen functionality of carbon spheres and possible coordination reaction of the resulting Cr(III) with the lone pair electrons of nitrogen. The NECS adsorbent was shown to maintain over 90% Cr(VI) removal efficiency after six cycles. Finally, the Cr(VI) removal efficiency of NECS reached 99.9% with a dosage of 12 g L-1 for real acidic electroplating wastewater (initial concentration 936.68 mg g(-1) and pH 1.5), clearly showing the promise of this novel adsorbent for treating Cr-containing wastewater.
机译：在以间苯二胺和六亚甲基四胺为原料的一锅式水热合成中，通过ZnCl2活化高氮含量的聚合物球体后，获得了富氮碳球（NECS）。 NECS的特征在于SEM，BET，FT-IR和XPS。发现NECS具有直径约0.6-1.2 mm的均质球形形态和高比表面积（1237 m（2）g（-1））。元素分析表明，NECS的氮含量高达10.21wt％。当使用酸性溶液中的六价铬（Cr（VI））评估吸附性能时，在pH 2.0时最大的Cr（VI）去除能力高达279 mg g（-1）。拟二阶和Freundlich模型很好地拟合了Cr（VI）的吸附行为。基于ζ电势和XPS分析，提出Cr（VI）去除机理是在低pH值下NECS表面静电吸附Cr（VI）阴离子，然后将Cr（VI）还原为Cr（III）。通过碳球的氮官能团以及所得的Cr（III）与氮的孤对电子的配位反应。在六个循环后，NECS吸附剂可保持90％以上的Cr（VI）去除效率。最后，以12 g L-1的剂量处理真正的酸性电镀废水（初始浓度为936.68 mg g（-1）且pH为1.5）时，NECS的Cr（VI）去除率达到99.9％，清楚地表明了该新型产品的前景用于处理含铬废水的吸附剂。

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