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土壤有机质在石英-水界面吸附与团聚行为的分子动力学模拟(PDF)

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《地球科学与环境学报》[ISSN:1672-6561/CN:61-1423/P]

卷:: 第47卷
期数:: 2025年第06期

页码:: 1057-1069

栏目:: 环境与可持续发展

出版日期:: 2025-12-10

文章信息/Info

Title:: Adsorption and Aggregation of Soil Organic Matter at the Quartz-water Interface: Insights from Molecular Dynamics Simulations

文章编号:: 1672-6561(2025)06-1057-13

作者:: 张弛^1*; 马浩哲¹; 卢玮丽¹; 杜少喜^2; 任蕊²; 周知宇¹; 贾汉忠¹; (1. 西北农林科技大学资源环境学院,陕西杨凌 712100; 2. 陕西省水工环地质调查中心,陕西西安 710068)

Author(s):: ZHANG Chi^1*; MA Hao-zhe¹; LU Wei-li¹; DU Shao-xi^2; REN Rui²; ZHOU Zhi-yu¹; JIA Han-zhong¹; (1. College of Natural Resources and Environment, Northwest A&F University, Yangling 712100, Shaanxi, China; 2. Shaanxi Hydrogeology Engineering Environment Geology Survey Center, Xi'an 710068, Shaanxi, China)

关键词:: 土壤有机质; 矿物-水界面; 分子动力学; 石英; 纳米孔; 吸附; 团聚

Keywords:: soil organic matter; mineral-water interface; molecular dynamics; quartz; nanopore; adsorption; aggregation

分类号:: S153.6

DOI:: 10.19814/j.jese.2025.05028

文献标志码:: A

摘要:: 作为土壤中最丰富的原生矿物,石英界面对有机质的吸附行为是调控土壤有机碳循环与稳定性的关键地球化学过程。采用分子动力学模拟方法,探究不同石英表面((100)-α、(100)-β、(001)和(101))纳米孔中有机质的界面微观结构、团聚迁移行为及其构象动态变化特征等关键分子机制,阐明离子类型对有机质稳定性的调控作用。模拟过程为:基于CLAYFF力场(描述石英)和Amber99SB力场(描述有机质及离子),在Ca²⁺和Mg²⁺浓度为0.06 mol·L^-1环境下开展了时间为300 ns的模拟。结果表明:范德华力虽然有助于有机质在石英界面的吸附和沉积,但是同时受到不稳定的氢键作用和静电排斥效应的影响; 此外,Ca²⁺通过内球配位作用形成致密且稳定的团聚体,以显著抑制有机质的扩散,而Mg²⁺则通过外球配位形成松散团聚结构,导致有机质具有更高的迁移能力。

Abstract:: As the most abundant primary mineral in soil, the interfacial behavior of soil organic matter(SOM)on quartz is a key geochemical process controlling the cycling and stability of soil organic carbon. Molecular dynamics simulations were employed to investigate the key molecular mechanisms, including the interfacial microstructure, aggregation-migration behavior, and conformational dynamics of SOM within nanopores of distinct quartz crystal surfaces((100)-α,(100)-β,(001), and(101)), and to elucidate the regulatory effects of ion types on SOM stability. The simulations were conducted using the CLAYFF force field for quartz and the Amber99SB force field for SOM and ions, with Ca²⁺ and Mg²⁺ concentrations of 0.06 mol·L^-1 and a duration of 300 ns. The results show that although van der Waals interactions contribute to the adsorption and deposition of SOM on quartz surfaces, they are simultaneously affected by unstable hydrogen bonding and electrostatic repulsion effects. Furthermore, Ca²⁺ forms dense and stable aggregates through inner-sphere coordination, significantly inhibiting the diffusion of SOM; whereas Mg²⁺ forms loose aggregate structures through outer-sphere coordination, thereby resulting in higher migration capacity for SOM. This study provides molecular-level insights into the stabilization mechanisms of SOM in quartz nanopores and offers a theoretical basis for regulating the stability of soil carbon pools.

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备注/Memo

备注/Memo:: 收稿日期:2025-05-25; 修回日期:2025-09-02投稿网址:http:∥jese.chd.edu.cn/
基金项目:陕西省公益性地质调查项目(陕地勘金字〔2025〕50号); 国家自然科学基金项目(42107263)
*通信作者:张弛(1990-),男,陕西华阴人,副教授,工学博士,E-mail:chizhang@nwafu.edu.cn。
通信作者:杜少喜(1970-),男,陕西紫阳人,高级工程师,E-mail:603107975@qq.com。

更新日期/Last Update: 2025-12-10

《地球科学与环境学报》[ISSN:1672-6561/CN:61-1423/P]

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