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

LUO Santu; ZHANG Mingyan; ZHANG Jishen; WANG Zifeng; SUN Bowen; LIU Dingxin; RONG Mingzhe

doi:10.7498/aps.74.20251221

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
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图 1 等离子体处理水溶液的物理化学过程示意图

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

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图 2 等离子体处理水溶液气液相化学反应类别

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

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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

Figure 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]

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

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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

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

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图 6 等离子体活化水中含氮活性粒子的浓度分布^[70]

Figure 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]

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

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图 8 整体模型与多维流体模型联合计算流程图

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

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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

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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

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