Agro-Environmental Protection Institute, Chinese Academy of Agricultural Sciences, No. 31, Fukang Road, Nankai District, Tianjin, 300191, China.
Environ Sci Pollut Res Int. 2018 Dec;25(35):35646-35656. doi: 10.1007/s11356-018-3500-2. Epub 2018 Oct 23.
Dehydrochlorination of lindane is commonly conducted in homogeneous alkaline solutions, possessing a series of problems such as corrosion and poor recyclability. In order to overcome the pervasive problems concerning homogeneous catalysts, heterogeneous catalysts have been increasingly employed in the applications. In this study, nitrogen-doped porous carbons (NPCs) were developed by a simple way in which chitosan and ZnCl were employed as the precursor and activation agent, respectively. NPCs exhibited high surface area (1111-1497 m/g) and large porosity (0.464-0.621 cm/g), resulting in a great adsorption affinity to lindane and the by-products. As solid bases, NPCs displayed an enhanced catalytic activity on lindane dehydrochlorination. This was closely related to the amount of pyridinic nitrogen on the pore surface, which could be tuned by the synthesis temperature. The optimal removal efficiency of lindane was up to 99.9% in presence of A800 (a NPC catalyst) at moderate pH (9.0) and mild temperature (45 °C) after incubation for 24 h. The rate constant for A800 suspension was improved by 2-3 orders of magnitude in comparison with that obtained in homogeneous solution at moderate pH (9.0) and mild temperatures (25-45 °C). The reusability of the material was evaluated by cycling for three times without noticeably reduced catalytic activity. This study provides a novel strategy to achieve partial dechlorination of chlorinated organic pollutants.
林丹的脱氯化氢反应通常在均相碱性溶液中进行,但存在一系列问题,如腐蚀和较差的可回收性。为了克服均相催化剂的普遍问题,多相催化剂已越来越多地应用于该领域。在这项研究中,通过一种简单的方法开发了氮掺杂多孔碳(NPCs),其中壳聚糖和 ZnCl 分别用作前体和活化剂。NPCs 具有高的比表面积(1111-1497 m/g)和大的孔隙率(0.464-0.621 cm/g),对林丹和副产物具有很强的吸附亲和力。作为固体碱,NPCs 在林丹脱氯化氢反应中表现出增强的催化活性。这与孔表面上吡啶氮的含量密切相关,而吡啶氮的含量可以通过合成温度来调节。在温和的 pH 值(9.0)和温度(45°C)下,在孵育 24 小时后,A800(一种 NPC 催化剂)存在下林丹的去除效率高达 99.9%。与在温和 pH 值(9.0)和温和温度(25-45°C)的均相溶液中获得的速率常数相比,A800 悬浮液的速率常数提高了 2-3 个数量级。通过循环使用三次评估了材料的可重复使用性,其催化活性没有明显降低。这项研究为实现氯化有机污染物的部分脱氯提供了一种新策略。