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Migration and transformation mechanisms of iron in clayey sediments during compaction: studies using simulation experiments

Mécanismes de migration et de transformation du fer dans les sédiments argileux lors du compactage: études à l’aide d’expériences de simulation

Mecanismos de migración y transformación del hierro en sedimentos arcillosos durante la compactación: estudios utilizando experimentos de simulación

黏土沉积物压实过程中铁的迁移与转化机制：利用模拟实验进行的研究

Mecanismos de migração e transformação do ferro em sedimentos argilosos durante a compactação: estudos utilizando experimentos de simulação

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Abstract

The behavior of iron (Fe) in clayey aquitards has a significant effect on the groundwater environment. However, the release processes and impact of Fe within clayey sediments during compaction remain unknown. Two groups of simulation experiments were carried out to demonstrate the migration and transformation mechanisms of Fe during clayey sediment compaction. Experiment A, which simulated a natural deposition condition, revealed that pressurization changed the reaction environment from oxidative to reductive by isolating oxygen. Oxidation of ferrous ions was followed by reduction dissolution of poorly crystalline Fe (III) and crystalline Fe (III) oxides. Under the microbial utilization of organic matter, the main transformation process of sediment Fe was the dissimilatory reduction of poorly crystalline Fe (III) oxides. The total Fe concentration in pore water was 0.09–11.61 mg/L, with ferrous ions predominating among the Fe species. The lower moisture content (\(\text{<}\)~36%) in the later stage of compaction inhibited the dissimilatory reduction of Fe (III), and the formation of Fe (II) minerals resulted in a decrease in Fe concentration. Experiment B, which simulated an artificial compaction state, revealed that the sediment Fe was primarily released by physical dissolution because of changes in pore structure and solubility. The concentration of total Fe in pore water was 0.02–1.96 mg/L, with a significant increase in response to a rapid increase in pressure. According to the estimates in the Chen Lake wetland (eastern China), the contribution of clay pore water release accounted for 19.9–31.9% of the average Fe concentration in groundwater during natural deposition.

Résumé

Le comportement du fer (Fe) dans les aquitards argileux a un effet significatif sur l’environnement des eaux souterraines. Cependant, les processus de libération et l’impact du Fe dans les sédiments argileux pendant le compactage restent inconnus. Deux groupes d’expériences de simulation ont été réalisés pour démontrer les mécanismes de migration et de transformation du Fe pendant le compactage des sédiments argileux. L’expérience A, qui simulait des conditions de dépôt naturelles, a révélé que la pressurisation modifiait l’environnement réactionnel d’oxydant à réducteur en isolant l’oxygène. L’oxydation des ions ferreux a été suivie par la dissolution réductrice du Fe (III) mal cristallisé et des oxydes de Fe (III) cristallisés. Dans le cadre de l’utilisation microbienne de la matière organique, le principal processus de transformation du Fe des sédiments était la réduction dissimilaire des oxydes de Fe (III) peu cristallins. La concentration totale du Fe dans l’eau interstitielle était de 0.09 à 11.61 mg/L, les ions ferreux prédominant parmi les espèces de Fe. La teneur en humidité plus faible (\(\text{<} \,\)~36%) au cours de la dernière étape du compactage a inhibé la réduction dissimulatrice de Fe (III), et la formation de minéraux de Fe (II) a entraîné une diminution de la concentration de Fe. L’expérience B, qui simulait un état de compactage artificiel, a révélé que le sédiment Fe était principalement libéré par dissolution physique en raison de changements dans la structure porale et de la solubilité. La concentration de Fe total dans l’eau interstitielle était de 0.02 à 1.96 mg/L, avec une augmentation significative en réponse à une augmentation rapide de la pression. Selon les estimations faites pour la zone humide de la Chen (partie orientale de la Chine), la contribution d’eau interstitielle libérée par l’argile représentait 19.9 à 31.9% de la concentration moyenne de Fe des eaux souterraines lors du processus naturel de dépôt.

Resumen

El comportamiento del hierro (Fe) en acuíferos arcillosos tiene un efecto significativo en el entorno de las aguas subterráneas. Sin embargo, los procesos de liberación y el impacto del Fe dentro de los sedimentos arcillosos durante la compactación siguen siendo desconocidos. Se llevaron a cabo dos grupos de experimentos de simulación para demostrar los mecanismos de migración y transformación del Fe durante la compactación de sedimentos arcillosos. El experimento A, que simuló una condición de sedimentación natural, reveló que la presurización cambió el ambiente de reacción de oxidativo a reductivo aislando el oxígeno. La oxidación de iones ferrosos fue seguida por la disolución reductora de Fe (III) poco cristalino y óxidos de Fe (III) cristalinos. Bajo la utilización microbiana de materia orgánica, el principal proceso de transformación del Fe del sedimento fue la reducción disimilatoria de óxidos de Fe (III) pobremente cristalinos. La concentración total de Fe en el agua de poros fue de 0.09–11.61 mg/L, predominando los iones ferrosos entre las especies de Fe. El menor contenido de humedad (< ~36%) en la última etapa de compactación inhibió la reducción disimilatoria del Fe (III), y la formación de minerales de Fe (II) dio lugar a una disminución de la concentración de Fe. El experimento B, que simuló un estado de compactación artificial, reveló que el Fe del sedimento se liberó principalmente por disolución física debido a los cambios en la estructura de los poros y la solubilidad. La concentración de Fe total en el agua de los poros fue de 0.02–1.96 mg/L, con un aumento significativo en respuesta a un rápido incremento de la presión. Según las estimaciones realizadas en el humedal del lago Chen (este de China), la contribución de la liberación de agua de poros de arcilla supuso entre el 19.9 y el 31.9% de la concentración media de Fe en las aguas subterráneas durante la sedimentación natural.

摘要

黏土弱透水层中铁（Fe）的行为对地下水环境有着显著影响。然而, 黏土沉积物压实过程中铁的释放过程及其影响尚不清楚。为了展示黏土沉积物压实过程中铁的迁移转化机制, 进行了两组模拟实验。实验A模拟了自然沉积条件, 结果显示压力作用通过隔绝氧气, 将反应环境由氧化转变为还原环境。继而发生了铁离子的氧化, 以及弱结晶铁（Fe (III)）和结晶性铁（Fe (III)）氧化物的还原溶解。在微生物对有机质的利用下，沉积物中铁的主要转化过程是弱结晶铁（Fe (III)）氧化物的异化还原。孔隙水中的总铁浓度为0.09−11.61 mg/L, 其中亚铁是主要的铁形态。在压实后期, 较低的含水率（<36%）抑制了铁 (III) 的异化还原, 结合铁 (II) 矿物的形成导致铁浓度降低。实验B模拟了人为压实条件, 结果发现沉积物中的铁主要是通过孔隙结构和溶解度变化导致的物理溶解而释放。孔隙水中的总铁浓度为0.02−1.96 mg/L, 而且随着压力的快速升高而显著增加。根据对中国东部沉湖湿地的估算, 自然沉积过程中黏土孔隙水释放对地下水中铁的贡献占平均铁浓度的19.9−31.9%。

Resumo

O comportamento do ferro (Fe) em aquitardos argilosos tem um efeito significativo no ambiente das águas subterrâneas. No entanto, os processos de liberação e o impacto do Fe nos sedimentos argilosos durante a compactação permanecem desconhecidos. Dois grupos de experimentos de simulação foram realizados para demonstrar os mecanismos de migração e transformação do Fe durante a compactação de sedimentos argilosos. O experimento A, que simulou uma condição natural de deposição, revelou que a pressurização mudou o ambiente de reação de oxidativo para redutor, isolando o oxigênio. A oxidação de íons ferrosos foi seguida pela dissolução redutora de óxidos de Fe (III) pouco cristalinos e de Fe (III) cristalinos. Sob a utilização microbiana da matéria orgânica, o principal processo de transformação do Fe sedimentar foi a redução dissimilatória de óxidos de Fe (III) pouco cristalinos. A concentração total de Fe na água dos poros foi de 0.09–11.61 mg/L, com íons ferrosos predominando entre as espécies de Fe. O menor teor de umidade (< ~36%) na fase posterior de compactação inibiu a redução dissimilatória de Fe (III), e a formação de minerais de Fe (II) resultou em uma diminuição na concentração de Fe. O experimento B, que simulou um estado de compactação artificial, revelou que o Fe do sedimento foi liberado principalmente por dissolução física devido a mudanças na estrutura dos poros e na solubilidade. A concentração de Fe total na água dos poros foi de 0.02–1.96 mg/L, com um aumento significativo em resposta a um rápido aumento na pressão. De acordo com as estimativas na zona húmida do Lago Chen (leste da China), a contribuição da libertação de água dos poros de argila foi responsável por 19.9–31.9% da concentração média de Fe nas águas subterrâneas durante a deposição natural.

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Acknowledgements

We thank the anonymous reviewers and associate editor for helpful comments that substantially improved the manuscript.

Funding

This study was financially supported by the National Natural Science Foundation of China (Nos. 41630318 and 42007173).

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Authors and Affiliations

  1. China Institute of Geo-Environment Monitoring, Beijing, 100081, China

    Rui Liu & Xinyan Liu

  2. School of Environmental Studies, China University of Geosciences, Wuhan, 430074, China

    Teng Ma

  3. State Environmental Protection Key Laboratory of Source Apportionment and Control of Aquatic Pollution, China University of Geosciences, Wuhan, 430078, China

    Teng Ma

  4. Hebei Key Laboratory of Environment Monitoring and Protection of Geological Resources, Hebei Geological Environment Monitoring Institute, Shijiazhuang, 050021, China

    Yantao Jian & Juan Chen

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  1. Rui Liu
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Liu, R., Ma, T., Liu, X. et al. Migration and transformation mechanisms of iron in clayey sediments during compaction: studies using simulation experiments. Hydrogeol J 32, 1043–1056 (2024). https://doi.org/10.1007/s10040-024-02783-1

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