环境化学2024,Vol.43Issue(12) :4182-4194.DOI:10.7524/j.issn.0254-6108.2023060603

3种合成施氏矿物对Sb(Ⅲ)的吸附动力学机制

Kinetics mechanisms of Sb(Ⅲ)adsorbed by three synthesized Schwertmannites

谢志磊 莘嘉静 李智超 吕昌伟 何江
环境化学2024,Vol.43Issue(12) :4182-4194.DOI:10.7524/j.issn.0254-6108.2023060603

3种合成施氏矿物对Sb(Ⅲ)的吸附动力学机制

Kinetics mechanisms of Sb(Ⅲ)adsorbed by three synthesized Schwertmannites

谢志磊 1莘嘉静 2李智超 2吕昌伟 3何江3
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作者信息

  • 1. 内蒙古自治区环境监测总站,呼和浩特,010011
  • 2. 内蒙古大学生态与环境学院,呼和浩特,010021
  • 3. 内蒙古大学生态与环境学院,呼和浩特,010021;内蒙古大学环境地质研究所,呼和浩特,010021
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摘要

施氏矿物具有结晶度低、比表面积大等特点,对环境中锑的界面行为有显著影响.本文合成了3种施氏矿物(过氧化氢氧化法施氏矿物H-SCH、高锰酸钾氧化法施氏矿物M-SCH和乙醇改性法施氏矿物Y-SCH),以3种施氏矿物对Sb(Ⅲ)的吸附性能研究为主线,开展了吸附动力学实验研究,结合动力学全过程动态表征监测,揭示了不同化学法合成的施氏矿物对Sb(Ⅲ)吸附的差异性机制.结果表明,H-SCH在合成过程中结合了更多的Fe,具有更稳定的骨架结构;M-SCH与Y-SCH拥有比H-SCH更多的结构态SO42-;Y-SCH拥有更大的比表面积以及丰富的表面活性羟基;同时与H-SCH相比,M-SCH和Y-SCH的矿物结晶度均有所下降.吸附动力学过程揭示,3种施氏矿物对Sb(Ⅲ)的吸附均符合准二级动力学、颗粒内扩散模型,均以化学吸附为主,属于非均相扩散过程.XRD等矿物表征分析表明,在3种施氏矿物吸附Sb(Ⅲ)的过程中,Y-SCH未发生矿相转化,具有较好的稳定性;而H-SCH和M-SCH在吸附中后期出现了水铁矿的特征峰,由于水铁矿对Sb(Ⅲ)也具有一定的吸附能力,这在一定程度上促进了这两种矿物对Sb(Ⅲ)的吸附.3种施氏矿物主要通过外表面羟基官能团的络合作用对Sb(Ⅲ)进行吸附,在吸附过程中Sb(Ⅲ)会被Fe(Ⅲ)氧化为Sb(Ⅴ),形成的Sb(OH)6-进一步与施氏矿物表面可交换态SO42-进行离子交换,促进了施氏矿物对锑的吸附,为施氏矿物在含锑废水处理领域的实际应用积累了理论和实验数据基础.

Abstract

Schwertmannites are characterized by low crystallinity and high specific surface area,which significantly impact the interface process of antimony(Sb)in the environment.In this study,three types of Schwertmannites,namely H-SCH(synthesized by H2O2 oxidation method),M-SCH(synthesized by KMnO4 oxidation method),and Y-SCH(H-SCH modified by ethanol),were prepared.The study investigated the kinetics mechanisms of Sb(Ⅲ)adsorption by the three synthesized Schwertmannites through comprehensive monitoring and characterization.The results revealed that H-SCH combined more Fe during the synthesis process,resulting in a more stable framework structure.M-SCH and Y-SCH exhibited higher structural SO42-compared to H-SCH.Particularly,Y-SCH displayed a larger specific surface area and abundant surface-active hydroxyl groups.Both M-SCH and Y-SCH presented decreased trends in mineral crystallinity compared to H-SCH.The adsorption kinetics indicated that the adsorption of Sb(Ⅲ)by the three Schwertmannites followed the models of pseudo-second-order kinetics and particle diffusion,suggesting dominant chemical adsorption and a non-homogeneous diffusion process.XRD analysis revealed relative stability in Y-SCH during the adsorption process of Sb(Ⅲ),with no observed mineral phase transformation.However,the H-SCH and M-SCH groups exhibited characteristic peaks of ferrihydrite during the late stage of adsorption process,enhancing the adsorption of Sb(Ⅲ)due to the high adsorption abilities of ferrihydrite to Sb(Ⅲ).Chelation of surface hydroxyl functional groups was the main mechanism for Sb(Ⅲ)adsorption by the three synthesized Schwertmannites.During the adsorption process,Sb(Ⅲ)was oxidized to Sb(V)by Fe(Ⅲ),and the formed Sb(OH)6-further exchanged with exchangeable SO42-on the surface of Schwertmannites,inherently enhancing the adsorption of Sb(Ⅲ)by Schwertmannites.This work provides a theoretical basis and a comprehensive dataset for the practical application of Schwertmannites in the treatment of wastewater containing Sb.

关键词

施氏矿物//吸附/动力学机制/表征

Key words

Schwertmannite/Sb(Ⅲ)/adsorption/kinetics mechanisms/characterization

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出版年

2024
环境化学
中国科学院生态环境研究中心

环境化学

CSTPCDCSCD北大核心
影响因子:1.049
ISSN:0254-6108
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