Department of Chemical Engineering, South Branch, Islamic Azad University, Tehran, Iran.
Chemistry and Petrochemistry Research Center, Standard Research Institute, Karaj, Iran.
Environ Sci Pollut Res Int. 2022 Feb;29(9):13253-13267. doi: 10.1007/s11356-021-16613-4. Epub 2021 Sep 28.
The disposal of polychlorinated biphenyls (PCBs) as persistent organic pollutants from the environment has been normally performed by isolation from soil or water because of their biological activity and toxic potential. In the present investigation, catalytic hydrodehalogenation was used to detoxify PCBs-contaminated transformer oil. All reactions were directed on an oil containing 11.09 wt% of PCBs utilizing palladium supported on multi-walled carbon nanotubes (Pd/MWCNTs). The amount of hexa-chlorine homologues reduced considerably from 5.07% to less than 800 ppm utilizing HDC at the atmosphere of argon. Moreover, the amounts of long half-lives and bioaccumulative congener of PCB 153 decreased considerably from 3.2% to less than 200 ppm. Besides, the quantity of some environmental pollutants like PCB 105 as a mono-ortho-substituted congener decreased considerably. The significant effects of reaction time, reaction temperature, and catalyst concentration on the efficiency were confirmed and modeled through Box-Behnken design. The optimal reaction condition with an efficiency of 96.67% was 70°C, with catalyst loading of 8 wt% and reaction time of 3.23 h. Furthermore, the quantity of turnover frequency of Pd/MWCNTs showed that it has more activity than palladium-carbon active supported in the ambient pressure without utilizing hydrogen gas in transformer oil complex. The study of the kinetic model revealed that the required activation energy (of 12.99 kJ/mol) to remove PCBs from transformer oil utilizing the present catalyst was lower than other catalyzed hydrodechlorination methods.
多氯联苯(PCBs)作为持久性有机污染物,通常因其生物活性和潜在毒性而从环境中分离出来进行处理。在本研究中,采用催化加氢脱卤法对含多氯联苯的变压器油进行脱毒。所有反应均针对一种含有 11.09wt%多氯联苯的油进行,利用多壁碳纳米管负载的钯(Pd/MWCNTs)作为催化剂。在氩气气氛下,利用 HDC 将六氯同系物的含量从 5.07%降低到 800ppm 以下。此外,PCB 153 的长半衰期和生物累积同系物的含量也从 3.2%降低到 200ppm 以下。此外,一些环境污染物如 PCB 105 的含量也大大降低,其为单邻位取代同系物。通过 Box-Behnken 设计确认并建立了反应时间、反应温度和催化剂浓度对效率的显著影响模型。在最优反应条件下,效率为 96.67%,反应温度为 70°C,催化剂负载量为 8wt%,反应时间为 3.23h。此外,Pd/MWCNTs 的转化频率表明,与在环境压力下不使用氢气的钯-碳活性负载催化剂相比,它在变压器油复合物中具有更高的活性。动力学模型研究表明,利用本催化剂从变压器油中去除多氯联苯所需的活化能(12.99kJ/mol)低于其他催化加氢脱氯方法。