等离子体处理水溶液仿真—从参数获取、模型构建到智能算法

罗三土; 张明岩; 张基珅; 王子丰; 孙博文; 刘定新; 荣命哲

doi:10.7498/aps.74.20251221

摘要
大气压低温等离子体在生物医学、环境保护、纳米制造等领域具有广泛应用, 而这些应用中的核心化过程通常是等离子体与水溶液的相互作用. 等离子体与水溶液的相互作用非常复杂, 既包含种类繁多的气液两相反应, 也包含相互耦合的粒子传质过程, 使得现有的实验技术难以系统地阐释内在机制, 仿真研究至关重要. 近10余年来, 国内外对等离子体与水溶液相互作用的仿真研究取得了重要进展, 基本解决了传质与反应参数缺乏的问题, 从无到有建立了多种类型的仿真模型, 并积极探索基于人工智能的新型仿真方法, 显著提升了对该领域的认知水平. 本文将从参数获取、模型构建到智能算法3个方面综述近年来的仿真研究进展, 以期为国内同行和研究生提供参考.

关键词:
等离子体处理水溶液 /

基础参数 /

仿真模型 /

智能算法
Abstract
Atmospheric-pressure low-temperature plasma has been widely used in various fields such as biomedicine, environmental protection, and nanomanufacturing, and the key physicochemical processes in these applications involve the interactions between plasma and aqueous solutions. However, such plasma-liquid interactions are very complex, involving a wide range of gas-liquid phase reactions as well as coupled mass transfer processes. These intricate mechanisms make it challenging for existing experimental techniques to provide a systematic understanding, thereby highlighting the critical role of simulation studies. Over the past decade, significant progress has been made in the simulation of plasma-solution interactions. Researchers have basically solved the problems of scarce transport and reaction parameter data, established various types of simulation models, and actively explored new simulation methods based on intelligence algorithms. These advances have greatly deepened our understanding of this field. Thus, this paper reviews recent developments in simulation studies of plasma-solution interactions from three perspectives, namely parameter acquisition, model construction, and intelligent algorithms, with the aim of providing useful insights for researchers.

Keywords:
plasma treatment of aqueous solution /

basic parameter /

simulation models /

intelligence algorithm
文章全文

施引文献

图 1 等离子体处理水溶液的物理化学过程示意图

Fig. 1. Schematic of physicochemical processes in plasma treatment of aqueous solution.

下载: 全尺寸图片幻灯片

图 2 等离子体处理水溶液气液相化学反应类别

Fig. 2. Types of gaseous and aqueous chemical reactions involved in the plasma treatment of aqueous solution.

下载: 全尺寸图片幻灯片

图 3 基于DFT计算的空气等离子体处理水溶液体系中N₂O₅相关反应　(a) N₂O₅与NO自由基或O原子反应自由能变化图^[41]; (b) N₂O₅与H₂O₂的气液相反应自由能变化图

Fig. 3. DFT-calculated N₂O₅-related reactions in the system of air plasma treatment for aqueous solution: (a) Free energy diagrams of reactions that N₂O₅ reacts with NO radical or O atom^[41]; (b) gaseous and aqueous reactions of N₂O₅ and H₂O₂.

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图 4 不同亨利系数对液相活性粒子浓度分布影响^[50]

Fig. 4. The effect of different Henry coefficients on the density distribution of aqueous reactive species^[50].

下载: 全尺寸图片幻灯片

图 5 等离子体产生的$ {\text{O}}_{{\text{2aq}}}^{ - } $与Aβ-淀粉样蛋白片段反应的动态演化过程

Fig. 5. The dynamic evolution of the reaction between plasma-generated $ {\text{O}}_{{\text{2aq}}}^{-} $ and Aβ-amyloid peptide fragments.

下载: 全尺寸图片幻灯片

图 6 等离子体活化水中含氮活性粒子的浓度分布^[70]

Fig. 6. The concentration distribution of nitrogen reactive species in plasma-activated water^[70].

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图 7 He掺杂空气等离子体反应网络图^[80]

Fig. 7. The reaction network diagram of He + Air plasma^[80].

下载: 全尺寸图片幻灯片

图 8 整体模型与多维流体模型联合计算流程图

Fig. 8. Flowchart of the joint calculation combining global model and multi-dimensional fluid model.

下载: 全尺寸图片幻灯片

表 1 常见粒子种类的实验检测手段及其局限性^[12,15]

Table 1. Experimental detection methods for commonly-seen reactive species and their limitations^[12,15].

粒子类别	示例粒子	常用检测手段	主要挑战/局限性
长寿命粒子	H₂O₂, O₃, NO, N₂O₅	分光光度法; 光化学荧光探针法	非特异性, 受其他粒子干扰; 需要特定pH条件; 试剂难溶于水
短寿命粒子	¹O₂, O, OH	电子自旋共振谱法; 光化学荧光探针法	非特异性, 受其他粒子干扰; 需要特定pH条件; 捕捉剂昂贵且易被氧化
激发态分子/离子	N₂(v), ONOO^–	发射光谱法; 液相色谱法	灵敏度低; 粒子猝灭快, 难以原位检测; 温度敏感

下载: 导出CSV

表 2 常用等离子体工作气体的LJ参数^[47]

Table 2. LJ parameters of commonly-used plasma working gas^[47].

工作气体	$ \sigma $/Å	ε/K	工作气体	$ \sigma $/Å	ε/K
N₂	3.56	102	CO₂	3.76	244
O₂	3.44	125	He	2.57	10.2
Ar	3.43	122	Air	3.71	78.5

下载: 导出CSV

map

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等离子体处理水溶液仿真—从参数获取、模型构建到智能算法

Simulation of plasma treated aqueous solutions: From basic parameter acquisition and model construction to intelligent algorithms

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等离子体处理水溶液仿真—从参数获取、模型构建到智能算法

Simulation of plasma treated aqueous solutions: From basic parameter acquisition and model construction to intelligent algorithms

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