Mechanistic insights into the chlorination volatilization of oxidized heavy metals via novel staggered chlorination roasting

Chenglong Lu, Xuan Yu, Guohao Yang, Qianqian Guo, Long Jiao, Jinxiang Lin, Kai Deng, Yanjun Hu
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Abstract

Improper handling of heavy metal-containing solid waste poses significant environmental risks. However, developing an effective heavy metal elimination method is still a challenge. Our study introduces a novel method of staggered chlorination roasting. The volatilization and removal effects of two chlorinating agents, NH₄Cl and CaCl₂, on typical key heavy metals, Zn and Cu, were investigated. Compared with the use of a single chlorinating agent, this method, which uses NH₄Cl for low-temperature decomposition and CaCl₂ for high-temperature reactions, significantly extends the chlorination reaction time, overtly enhancing the chlorination volatilization effect. This study elucidated the influence of the chlorinating agent content, temperature, and time on the elimination of heavy metal oxides. The results demonstrated that when the two chlorinating agents were added at a ratio of 2:3, roasting at 1100 °C for 60 min resulted in the highest volatilization rates of Zn (99.9%) and Cu (98.7%). Thermodynamic equilibrium and equilibrium phase composition calculations were conducted to explore the effects of the chlorinating agents and mineral components (SiO₂, Al₂O₃, Fe₂O₃, and CaO) on chlorination roasting. In the staggered chlorination mode, the chlorine-containing gases generated effectively mitigate the influence of mineral components, thereby suppressing interactions between oxidized heavy metals and mineral constituents. This suppression enhances the chlorination and volatilization of heavy metals. This study proposes a novel staggered chlorination roasting method based on composite chlorinating agents, offering a new approach for the collaborative and efficient removal of multiple heavy metals from solid waste.

Graphical abstract

新型交错氯化焙烧对氧化重金属氯化挥发机理的研究
含重金属固体废物处理不当会造成严重的环境风险。然而,开发一种有效的重金属消除方法仍然是一个挑战。本研究介绍了一种新的交错氯化焙烧方法。研究了nh_4 Cl和cac2两种氯化剂对典型关键重金属Zn和Cu的挥发去除效果。与单一氯化剂相比,该方法采用硫酸铵进行低温分解,氯化钙进行高温反应,明显延长了氯化反应时间,明显增强了氯化挥发效果。研究了氯化剂用量、氯化温度和氯化时间对重金属氧化物去除率的影响。结果表明,当两种氯化剂以2:3的比例添加时,在1100℃下焙烧60 min, Zn和Cu的挥发率最高,分别为99.9%和98.7%。通过热力学平衡和平衡相组成计算,探讨了氯化剂和矿物组分(SiO₂、Al₂O₃、Fe₂O₃和CaO)对氯化焙烧的影响。在交错氯化模式下,产生的含氯气体有效地减轻了矿物组分的影响,从而抑制了氧化重金属与矿物组分的相互作用。这种抑制作用增强了重金属的氯化作用和挥发性。本研究提出了一种基于复合氯化剂的交错氯化焙烧新方法,为协同高效去除固体废物中多种重金属提供了新途径。图形抽象
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