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Kinetic study of microwave enhanced mercury desorption for the regeneration of spent activated carbon supported mercuric chloride catalysts
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2020-10-27 , DOI: 10.1016/j.cej.2020.127355
Peng Liu , Chao Liu , Ting Hu , Junjie Shi , Libo Zhang , Bingguo Liu , Jinhui Peng

A novel microwave enhanced mercury desorption process was proposed for the regeneration of the spent activated carbon supported mercuric chloride catalysts. The mercury species desorption kinetics were investigated in detail by TG experiments, the overall apparent activation energy of 128.4 kJ/mol, the main reaction activation energy of 95.84 kJ/mol and the adsorption energy of 32.56 kJ/mol were confirmed with the combination of the model-free method and the DMol3 DFT module of Materials Studio package. The thermal desorption of HgCl2 and Hg2Cl2 were mainly between 473 K to 670 K, and the dominant mechanism for the desorption process was determined as second-order-model by the model-fitting method and the Z(α) master-plot method. Furthermore, the microwave enhancement degree of 26.36% was proved by the microwave heating experiment for the mercury desorption within 1500s at 673K, and the mercury content was significantly reduced from 19500 mg/kg to 149 mg/kg, which met the requirement of US land disposal restrictions (<260 mg/kg). Moreover, the preliminary activation of the spent activated carbon after microwave heating was demonstrated from the results of XRD, SEM and nitrogen adsorption analysis. Meanwhile, the HgCl2 solution with the concentration of 40-50g/L could be effectively prepared by the water leaching of the condensate of mercury species, which could be used to regenerate the catalyst by soaking adsorption with activated carbon after microwave heating. Finally, a novel microwave enhanced mercury desorption process was proposed, which can synchronous realize the harmless and recovery of the spent activated carbon supported mercuric chloride catalysts.



中文翻译:

微波增强汞解吸再生废活性炭负载的氯化汞催化剂的动力学研究

提出了一种新型的微波增强汞解吸方法,用于再生用过的活性炭负载的氯化汞催化剂。通过TG实验对汞的解吸动力学进行了详细的研究,结合两种催化剂的确证,表观活化能为128.4 kJ / mol,主反应活化能为95.84 kJ / mol,吸附能为32.56 kJ / mol。无模型方法和Materials Studio软件包的DMol 3 DFT模块。HgCl 2和Hg 2 Cl 2的热脱附主要在473 K至670 K之间,并且通过模型拟合方法和Zα)主图法。此外,通过微波加热实验证明,在673K下1500s内汞的解吸,微波增强度为26.36%,汞含量从19500 mg / kg显着降低至149 mg / kg,符合美国土地的要求。处置限制(<260 mg / kg)。此外,通过XRD,SEM和氮吸附分析的结果证明了微波加热后废活性炭的初步活化。同时,HgCl 2通过水浸出汞物种的冷凝物可以有效地制备浓度为40-50g / L的溶液,该溶液可通过微波加热后用活性炭浸泡吸附来再生催化剂。最后,提出了一种新型的微波增强汞解吸工艺,该工艺可以同步实现废活性炭负载的氯化汞催化剂的无害化和回收。

更新日期:2020-10-30
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