School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Soil and Groundwater Pollution Control, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, 518055, People's Republic of China.
State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control, School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, China.
Environ Geochem Health. 2019 Dec;41(6):2491-2503. doi: 10.1007/s10653-019-00301-x. Epub 2019 Apr 29.
Recent studies have reported the potential copper immobilization in aluminates (CuAlO and CuAlO) and ferrites (tetragonal CuFeO and cubic CuFeO) and suggested a reliable method to stabilize metals in reusable ceramic products. In this study, copper immobilization effect was further analyzed in the leaching solutions with pH close to environmental conditions. The results from the chemical equilibrium model Visual MINTEQ illustrated that almost all copper, aluminum, and iron formed complexes with CHCOO ions in the leachates. The dissolution behavior on sample surface was further explicated by time-of-flight secondary ion mass spectrometry (ToF-SIMS). The weight percentage of leached copper was lower than 0.1% even after 22-day leaching, indicating the successful copper stabilization in aluminates and ferrites. The results showed the highest copper concentrations in CuAlO leachates and the smallest leached copper amount from tetragonal CuFeO, respectively. The incongruent dissolution with Al-O or Fe-O bonds still remaining on the solid surface may be beneficial for preventing further leaching of copper. Furthermore, the modeling of reaction kinetics found that copper leaching from the CuAlO and CuAlO obeyed the second-order reaction with correlation coefficients higher than 0.99. Moreover, the shrinking core model was chosen to analyze the leaching mechanisms of both CuFeO ferrites, and the diffusion through product layer model acted as the rate-controlling step in their leaching process.
最近的研究报告指出,铜在铝酸盐(CuAlO 和 CuAlO)和铁酸盐(四方相 CuFeO 和立方相 CuFeO)中可能会被固定,并提出了一种在可重复使用的陶瓷产品中稳定金属的可靠方法。在本研究中,进一步分析了 pH 值接近环境条件的浸出液中铜的固定效果。化学平衡模型 Visual MINTEQ 的结果表明,几乎所有的铜、铝和铁都与浸出液中的 CHCOO 离子形成了配合物。飞行时间二次离子质谱(ToF-SIMS)进一步说明了样品表面的溶解行为。即使在 22 天的浸出后,浸出的铜的重量百分比仍低于 0.1%,表明铜在铝酸盐和铁酸盐中的固定是成功的。结果表明,CuAlO 浸出液中铜的浓度最高,四方相 CuFeO 中浸出的铜量最小。在固液界面上仍存在 Al-O 或 Fe-O 键的非均相溶解,可能有利于阻止铜的进一步浸出。此外,反应动力学模型表明,CuAlO 和 CuAlO 中铜的浸出符合二级反应,相关系数均高于 0.99。此外,还选择了收缩核模型来分析两种 CuFeO 铁酸盐的浸出机理,扩散通过产物层模型是其浸出过程的速率控制步骤。