酸盐溶解在甲甲中的激活能量:MLFF加速的DFT研究vdW和水化外效应
Mohammadreza Izadifar1, Neven Ukrainczyk1, Klara Schönfeld1
1Institute of Construction and Building Materials, Technical University of Darmstadt Franziska-Braun-Str. 3 Darmstadt 64287 Germany mr.izadifar@icloud.com izadifar@wib.tu-darmstadt.de.
Nanoscale advances
|June 5, 2025
概括
这项研究表明,氧化 (KOH) 与氧化 (NaOH) 相比,一般降低了在甲 (MK) 中酸溶解的激活能量. 减少的水化进一步降低了这种能量,影响了混凝土和地质聚合物材料的发展.
科学领域:
- 材料科学 材料科学 材料科学
- 计算化学计算化学
- 地质化学 地质化学
背景情况:
- 甲 (MK) 粘土是可持续混凝土和地质聚合物生产的重要补充水泥材料 (SCM).
- 了解MK溶解机制对于优化其波佐兰反应性和减少建筑材料的碳足迹至关重要.
- 之前的研究集中在酸盐溶解上;这项研究解决了关于酸物种行为的关键知识差距.
研究的目的:
- 在热激活的甲高 (MK) 中计算研究酸盐物种的溶解机制.
- 为微观前向溶解速率的原子运动蒙特卡洛 (kMC) 升级提供必要的数据.
- 阐明不同激活剂 (NaOH,KOH,水) 和水化结构对酸盐溶解的影响.
主要方法:
- 利用计算化学,特别是密度函数理论 (DFT) 和机器学习力场 (MLFF).
- 在远离平衡条件下的酸盐水解中使用改进的二次数法 (IDM) 计算原子活化能 (ΔEa).
- 分析了范德瓦尔斯 (vdW) 相互作用的效应以及围绕着阳离子 (Na+,K+) 和氧化离子 (OH-) 的各种水化外几何形状.
主要成果:
- 与氧化 (NaOH) 相比,氧化 (KOH) 一般导致酸盐溶解的活性能 (ΔEa) 较低,特别是当包括范德瓦尔斯相互作用时.
- 补水的存在和配置显著影响了激活能量.
- 在KOH和NaOH周围减少的水合导致酸物种溶解的ΔEa降低.
结论:
- 激活剂的选择 (KOH与NaOH) 和阴离子水化程度显然会影响甲甲醇溶解的速度限制步骤.
- 这些发现为改进预测基于MK材料的长期性能和反应性的计算模型提供了关键的见解.
- 该研究通过更好地了解SCM的基本化学成分,有助于开发更可持续的建筑材料.
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