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低酸介质中超声强化臭氧氧化从填埋冶金残渣中浸出钒的机理及动力学研究

Mechanism and kinetics study of vanadium leaching from landfilled metallurgical residues by ultrasonic with ozonation enhancement in a low-acid medium.

作者信息

Li Haoyu, Hu Chunhua, He Xinyi, Wang Jun, Tian Shihong, Zhu Xuejun, Mao Xuehua

机构信息

College of Biological and Chemical Engineering (College of Agricultural Sciences), Panzhihua University, Panzhihua 617000, China.

College of Biological and Chemical Engineering (College of Agricultural Sciences), Panzhihua University, Panzhihua 617000, China.

出版信息

Ultrason Sonochem. 2024 Oct;109:106998. doi: 10.1016/j.ultsonch.2024.106998. Epub 2024 Jul 17.

Abstract

Landfilled metallurgical residues are valuable raw materials for the recovery of strategic vanadium resources. However, efficient separation of vanadium from these residues is challenging due to its strong oxidation resistance and coating within silicate inclusions. To address this issue, this study proposes an enhanced leaching process utilizing the synergistic effect of O-catalyzed ultrasonic field in a low concentration sulfuric acid system. Results show that following a 10-minute O and ultrasonic treatment, the direct leaching rate of vanadium experienced a remarkable 46.7 % increase. Quenching experiments revealed a hierarchical order of active species within the reaction process:⋅OH >⋅O> H, with⋅OH oxidation exhibiting the most pronounced capacity for disrupting the inclusion structure. Electron Paramagnetic Resonance analysis indicated that the highest⋅OH yield arose from the combined application of ultrasound and ozone. Kinetic investigations demonstrated that the vanadium leaching process is governed by interfacial chemical reactions. The activation energy of vanadium oxidation leaching under ultrasonic-O conditions was determined to be 40.41 kJ/mol, representing a 20.19 % reduction compared to ultrasonic conditions alone. Through the integration of analysis, characterization, and comparative evaluations, it was discerned that the synergistic impact of ultrasonic and ozone treatments significantly enhances the breakdown of silicate inclusions by low-concentration HF, particularly in the conversion of SiOSi bonds into SiOH bonds and SiF bonds. In summary, the refined leaching methodology incorporating ozone catalysis in conjunction with ultrasonic treatment provides a new idea for the separation and extraction of refractory residual vanadium.

摘要

填埋的冶金残渣是回收战略性钒资源的宝贵原材料。然而,由于钒具有很强的抗氧化性且包裹在硅酸盐夹杂物中,要从这些残渣中高效分离钒具有挑战性。为解决这一问题,本研究提出了一种在低浓度硫酸体系中利用臭氧催化超声场协同效应的强化浸出工艺。结果表明,经过10分钟的臭氧和超声处理后,钒的直接浸出率显著提高了46.7%。淬灭实验揭示了反应过程中活性物种的层级顺序:·OH >·O> H,其中·OH氧化对破坏夹杂物结构的能力最为显著。电子顺磁共振分析表明,超声和臭氧联合应用产生的·OH产率最高。动力学研究表明,钒的浸出过程受界面化学反应控制。超声-臭氧条件下钒氧化浸出的活化能测定为40.41 kJ/mol,比单独超声条件降低了20.19%。通过综合分析、表征和对比评估发现,超声和臭氧处理的协同作用显著增强了低浓度氢氟酸对硅酸盐夹杂物的破坏作用,特别是在将SiOSi键转化为SiOH键和SiF键方面。总之,结合臭氧催化与超声处理的精制浸出方法为难处理残余钒的分离和提取提供了新思路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a576/11639428/a65f7c562e97/gr1.jpg

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