当前位置: X-MOL 学术Chem. Eng. Sci. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Unrefined low-grade pyrolusite for elemental mercury removal from flue gas: Experimental and DFT insights
Chemical Engineering Science ( IF 4.1 ) Pub Date : 2024-01-04 , DOI: 10.1016/j.ces.2023.119689
Qian Yu , Xin Sun , Menglu Sun , Bo Yuan , Xiaomeng Zuo , Dong Fu

Dual characteristics of oxidation capacity and economic advantage endow the unrefined low-grade pyrolusite (LGP) as a potential adsorbent/catalyst. This paper successfully applied it to remove Hg0 from flue gas, by which 98.6% of removal efficiency was obtained without chemical modification or external oxidant. Effects of various flue gas components on the Hg0 removal were investigated, and the synchronous improvement in efficiency and stability by HCl was revealed. Also, its reusability was evaluated and the decrease in removal efficiency after 5th cycles is less than 6%. Product analysis indicated that over 90% of Hg0 was chemisorbed as HgO without HCl, but the presence of HCl reversed the pathway to form HgCl2 that easily escape from the surface, with a proportion of about 95%. By combing experiments, characterizations and theoretical calculations, the mechanism was preliminarily speculated: (i) without HCl, O2 and the main components of LGP (MnOx, Fe2O3, etc.) involved in the catalytic oxidation according to Mars-Maessen mechanism; (ii) HCl tended to dissociate and adsorb on the MnO2 to form the chlorinated surface, and the mercury removal followed both L-H and E-R mechanism, although E-R was dominant; (iii) the formation of HgCl lowered the energy barrier of HgCl2 desorption, thereby expediting the oxidation-removal of Hg0.



中文翻译:

用于从烟气中去除元素汞的未精炼低品位软锰矿:实验和 DFT 见解

氧化能力和经济优势的双重特性赋予未精炼的低品位软锰矿(LGP)作为潜在的吸附剂/催化剂。本文成功地将其应用于烟气中Hg 0的去除,无需化学改性或外加氧化剂,去除率达到98.6%。研究了不同烟气组分对Hg 0去除的影响,揭示了HCl对效率和稳定性的同步提高。此外,对其可重复使用性进行了评估,第 5 次循环后去除效率的下降小于 6%。产物分析表明,在没有HCl的情况下,超过90%的Hg 0以HgO的形式被化学吸附,但HCl的存在逆转了形成HgCl 2的途径,很容易从表面逸出,比例约为95%。通过结合实验、表征和理论计算,初步推测其机理:(i)在没有HCl、O 2和导光板主要成分(MnO x、Fe 2 O 3等)参与催化氧化的情况下,根据Mars-梅森机构;(ii) HCl倾向于解离并吸附在MnO 2上形成氯化表面,并且除汞遵循LH和ER机制,尽管ER占主导地位;(iii)HgCl的形成降低了HgCl 2解吸的能垒,从而加速了Hg 0的氧化去除。

更新日期:2024-01-05
down
wechat
bug