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含酸性气体模拟烟气中砷蒸气在γ-氧化铝上的吸附及反应机理

Adsorption and reaction mechanism of arsenic vapors over γ-AlO in the simulated flue gas containing acid gases.

作者信息

Hu Hongyun, Chen Dunkui, Liu Huan, Yang Yuhan, Cai Hexun, Shen Junhao, Yao Hong

机构信息

State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan 430074, China.

State Key Laboratory of Coal Combustion, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan 430074, China; Department of New Energy Science and Engineering, School of Energy and Power Engineering, Huazhong University of Science and Technology, Wuhan 430074, China.

出版信息

Chemosphere. 2017 Aug;180:186-191. doi: 10.1016/j.chemosphere.2017.03.114. Epub 2017 Mar 28.

Abstract

Arsenic emission from fuel combustion and metal smelting flue gas causes serious pollution. Addition of sorbents is a promising way for the arsenic capture from high temperature flue gas. However, it is difficult to remove arsenic from SO/HCl-rich flue gas due to the competitive reaction of the sorbents with arsenic and these acid gases. To solve this problem, arsenic adsorption over γ-AlO was studied in this work to evaluate its adsorption mechanism, resistance to acid gases as well as regeneration behavior. The results show that γ-AlO had good resistance to acid gases and the arsenic adsorption by γ-AlO could be effectively carried out at a wide temperature range between 573 and 1023 K. Nevertheless, adsorption at higher-temperature (like 1173 K) leaded to the decrease of surface area and the rearrangement of crystal structure of γ-AlO, reducing the active sites for arsenic adsorption. The adsorption of arsenic was confirmed to occur at different active sites in γ-AlO by forming various adsorbed species. Increasing temperature facilitated arsenic transformation into more stable chemisorbed As and As which were difficult to remove through thermal treatment regeneration. Fortunately, the regeneration of spent γ-AlO could be well performed using NaOH solution.

摘要

燃料燃烧和金属冶炼烟气中的砷排放会造成严重污染。添加吸附剂是从高温烟气中捕获砷的一种很有前景的方法。然而,由于吸附剂与砷和这些酸性气体之间的竞争反应,很难从富含SO/HCl的烟气中去除砷。为了解决这个问题,本研究对γ-AlO上的砷吸附进行了研究,以评估其吸附机理、对酸性气体的耐受性以及再生行为。结果表明,γ-AlO对酸性气体具有良好的耐受性,γ-AlO对砷的吸附可以在573至1023 K的宽温度范围内有效进行。然而,在较高温度(如1173 K)下吸附会导致γ-AlO的表面积减小和晶体结构重排,减少砷吸附的活性位点。通过形成各种吸附物种,证实砷在γ-AlO的不同活性位点上发生吸附。温度升高促进砷转化为更稳定的化学吸附态As和As,难以通过热处理再生去除。幸运的是,使用NaOH溶液可以很好地实现废γ-AlO的再生。

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