The effect of pyrolysis temperature on the structure and uranium separation characteristics of kaolin

IF 6.3 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Surfaces and Interfaces Pub Date : 2025-03-07 DOI:10.1016/j.surfin.2025.106177
Maoling Wu , Keding Li , Bowen Zheng , Li Yang , Lin Zhang , Xuan Luo
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Abstract

Kaolin (KL) is regarded as an available adsorbent for U-containing wastewater treatment owing to its rich resources, low price, high chemical stability and excellent ion-exchange ability. While, the U removal performances of KL are constrained by its structure and poor active sites. Thermal activation is an efficient way to improve the U removal capacity of KL through expanding contact aera and providing more available adsorption sites. While, there were few researches about elaborating the relationship between KL structural properties, adsorption performances and pyrolysis temperature. In this study, the structure of KL at different pyrolysis temperatures relationship with its U separation characteristics was investigated at first. According to the results of characterizations, pyrolysis temperature obviously affected the crystal structure, phase composition and microstructure of KL. By comparison, KL pyrolyzed at 500 °C (KL-500) possessed rougher surface and stripped layer structure, thus providing more adsorptive sites to combine with uranyl. The experimental results indicate that KL-500 showed higher U separation rate (90.4 %) and larger U adsorption capacity (530.8 mg/g). Meanwhile, the maximum U removal capacity of KL-500 was larger than most of reported clay-based materials, illustrating the potential of practical application. Besides, KL-500 also performed favorable recoverability with the U adsorption rate of 80.2 % at the fifth cycle, meaning that KL was expected for treating natural wastewater. The fitting results of isotherm and kinetics models verified that the removal process of U on KL-500 was mainly single layer chemical adsorption. The surface charge of KL was negative due to deprotonation at pH 5.0, thus causing strong electrostatic attraction between adsorbents and uranyl. Combining the results of XPS spectra, the immobilization of U on KL-500 was mainly realized through electrostatic interaction and complexation, which was a combination process of physical and chemical adsorption, with chemical adsorption dominating.

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热解温度对高岭土结构和铀分离特性的影响
高岭土因其资源丰富、价格低廉、化学稳定性高、离子交换能力强等优点,被认为是处理含铀废水的有效吸附剂。而KL的脱U性能受其结构和活性位点差的限制。热活化是通过扩大接触面积和提供更多的有效吸附位点来提高KL脱铀能力的有效途径。而对KL结构性质、吸附性能与热解温度之间关系的研究较少。本研究首先考察了不同热解温度下KL的结构与其铀分离特性的关系。表征结果表明,热解温度对KL的晶体结构、相组成和微观结构有明显的影响,相比之下,500℃热解的KL (KL-500)具有更粗糙的表面和剥离层结构,从而为与铀酰结合提供了更多的吸附位点。实验结果表明,KL-500具有较高的U分离率(90.4%)和较大的U吸附量(530.8 mg/g)。同时,KL-500的最大U去除率大于大多数已报道的粘土基材料,说明了其实际应用潜力。此外,KL-500在第5次循环时的U吸附率为80.2%,具有良好的可回收性,可用于处理天然废水。等温线模型和动力学模型的拟合结果验证了KL-500对U的去除过程以单层化学吸附为主。KL在pH 5.0下发生去质子反应,表面电荷为负,吸附剂与铀酰之间产生强烈的静电吸引力。结合XPS光谱结果可知,U在KL-500上的固定主要是通过静电相互作用和络合作用实现的,这是一个物理吸附和化学吸附相结合的过程,以化学吸附为主。
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来源期刊
Surfaces and Interfaces
Surfaces and Interfaces Chemistry-General Chemistry
CiteScore
8.50
自引率
6.50%
发文量
753
审稿时长
35 days
期刊介绍: The aim of the journal is to provide a respectful outlet for ''sound science'' papers in all research areas on surfaces and interfaces. We define sound science papers as papers that describe new and well-executed research, but that do not necessarily provide brand new insights or are merely a description of research results. Surfaces and Interfaces publishes research papers in all fields of surface science which may not always find the right home on first submission to our Elsevier sister journals (Applied Surface, Surface and Coatings Technology, Thin Solid Films)
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