Dept. of Chemical and Environmental Engineering, University of Cincinnati (UC), Cincinnati, OH, 45221, USA.
Dept. of Chemical and Environmental Engineering, University of Cincinnati (UC), Cincinnati, OH, 45221, USA.
Chemosphere. 2024 Feb;349:140987. doi: 10.1016/j.chemosphere.2023.140987. Epub 2023 Dec 18.
Polychlorinated biphenyls (PCBs) is a group of persistent organic pollutants that still requires remediation and reduction long after the production is discontinued. Aroclor 1232 is a commercial PCB mixture that has been much less studied. To address this void, this paper presented catalytic hydro-dechlorination (HDC) of Aroclor 1232 using palladium on activated carbon (Pd/AC) at atmospheric pressure. Experimental variables studied including three mild temperatures, 22.5 °C, 50 °C, and 80 °C, and four different co-catalyst loadings. This batch of Aroclor 1232 constituted of more than 83% of mono-, di-, and tri-, chlorinated biphenyls (CB), in addition to biphenyl, tetra- and penta CBs. HDC efficiency increased with temperature, and reached 99.9% within 4 h of reaction at 80 °C. HDC efficiency also increased with co-catalyst loading. HDC efficiencies followed the trend of para > meta > ortho positions among isomers. The increase of temperature and EtN dosage are especially effective in dechlorination at ortho and meta positions. The apparent activation energy of Aroclor 1232 HDC was estimated as 25.57 kJ/mol based on pseudo-first order assumption, indicating that the reaction may be diffusion limited. Given the modest reaction conditions used, the HDC of Aroclor 1232 can potentially be a low-cost process.
多氯联苯 (PCBs) 是一组持久性有机污染物,即使在生产停止后很长时间,仍需要进行修复和减少。Aroclor 1232 是一种商业 PCB 混合物,研究得较少。为了解决这一空白,本文提出了在大气压下使用活性炭负载钯 (Pd/AC) 对 Aroclor 1232 进行催化加氢脱氯 (HDC)。研究了三个温和的温度(22.5°C、50°C 和 80°C)和四个不同的共催化剂负载量等实验变量。这批 Aroclor 1232 由超过 83%的单氯、二氯和三氯联苯 (CB) 以及联苯、四氯和五氯联苯组成。HDC 效率随温度升高而增加,在 80°C 下反应 4 小时内达到 99.9%。HDC 效率也随共催化剂负载量的增加而增加。HDC 效率在异构体中遵循对位>间位>邻位的趋势。温度和 EtN 用量的增加尤其有利于邻位和间位的脱氯。根据准一级假设,Aroclor 1232 HDC 的表观活化能估计为 25.57 kJ/mol,表明该反应可能受扩散限制。鉴于使用的温和反应条件,Aroclor 1232 的 HDC 可能是一种低成本的过程。