大气压等离子体射流在环境领域的应用进展

郝小龙; 石朝阳; 张一波

doi:10.12153/j.issn.1674-991X.20220815

大气压等离子体射流在环境领域的应用进展

doi: 10.12153/j.issn.1674-991X.20220815

江南大学环境与土木工程学院

基金项目: 国家自然科学基金项目（21376108）

详细信息

作者简介:
郝小龙(1978—)，男，副教授，博士，主要从事环境等离子体应用研究，xlhao@jiangnan.edu.cn

中图分类号: X593
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出版历程
- 收稿日期: 2022-08-16
- 网络出版日期: 2023-07-19

Progress in the application of atmospheric pressure plasma jets in environmental field

College of Environmental and Civil Engineering, Jiangnan University

摘要

摘要:
大气压等离子体射流（APPJ）是一种新兴的大气压等离子体放电技术，其在大气压下产生，具有放电温度和激发电压低、放电装置灵活、操作简便安全等优点，能够在大气环境中产生，在生物医学、环境卫生、材料改性等多领域具有广泛的应用前景。概述了近年来国内外APPJ在环境卫生和环境污染治理等环境领域，特别是环境灭菌、环境污染物去除和环境藻类治理等方面的应用；阐述了APPJ的射流装置与处理方式、效果和机理；基于研究现状，探讨了APPJ在环境领域应用存在的问题与解决途径，主要包括其灭菌降解机理、试验规模放大、等离子体射流发生装置设计和等离子体射流电源研发；最后展望了该技术未来在环境领域应用的发展方向和趋势。
- 大气压等离子体射流(APPJ) /
- 环境灭菌消毒 /
- 污染物去除 /
- 湖泊藻类去除 /
- 环境应用
Abstract:
Atmospheric pressure plasma jet (APPJ) is a new type of atmospheric pressure plasma discharge technology. It is generated under atmospheric pressure and has the advantages of low discharge temperature and excitation voltage, flexible discharge device, simple and safe operation. It can be produced in atmospheric environment, and has a wide range of application prospects in biomedicine, environmental health, material modification and other fields. The applications of APPJ in the environmental field such as environmental sanitation and pollution control at home and abroad in recent years were comprehensively summarized, especially the applications of environmental sterilization, environmental pollutant removal and environmental algae treatment, and its jet equipment, treatment styles, effects and mechanisms were elaborated. Based on the research status, the existing problems and solutions in the field of APPJ environment were discussed, including its sterilization and degradation mechanism, scale-up of test, design of plasma jet generator and development of plasma jet power supply. Finally, the future development direction and trend of the application of this technology in the field of environment were prospected.
- atmospheric pressure plasma jet (APPJ) /
- environmental sterilization and disinfection /
- pollutant removal /
- lake algae removal /
- environmental application

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图 1 几种典型的大气压等离子体射流处理液相环境污染物的形式示意

注：①—等离子体射流装置；②—射流羽辉；③—液相界面；④—溶液。A—射流液上形式；B—射流接触形式；C—射流上部浸入形式；D—射流底部浸入形式。

Figure 1. Schematic diagram of several typical styles of environmental pollutant treatment in aqueous phase by APPJ

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表 1 APPJ对水中典型环境污染物去除的应用研究

Table 1. Application of APPJ to the removal of typical environmental pollutants in the water

污染物名称	等离子体射流类型	射流装置及处理方式	射流试验效果	射流试验机理
水中代表性糖皮质激素污染物氢化可的松 (HC)	空气源介质阻挡放电射流^[44]	射流水反应器由底部多个微等离子体喷射单元组成，采取空气从底部石英管曝入产生射流的处理方式	HC的去除率随放电功率增大和放电时间延长而增加；在初始浓度为0.138 mmol/L，放电功率为49.7 W，空气流量为4 L/min条件下，处理120 min后去除率达98%；HC的去除率随着空气流量的增大而升高。碱性条件(pH为8.3)不利于HC的降解，弱酸性条件(pH为3.8~5.4)有利于HC降解	放电过程中产生了OH(A-X)、NH(A-X)、N₂(C-B)等活性粒子，其中•OH、¹O₂和•O₂⁻在HC的降解过程中起到重要作用
水中环境残留的典型氟喹诺酮抗生素诺氟沙星（NOR）	无电极高流量Ar大气压微波等离子体射流（MPJ）^[45]	无电极高流量Ar源大气压微波等离子体射流反应器，采取射流石英管底部接触溶液的处理方式	处理6 min时NOR降解率可达98.27%±1.03%；处理15 min时，矿化率(TOC去除率)达到68.67%±3.21%。Escherichia coli毒性测试表明，处理20 min后的NOR溶液无毒	NOR溶液的快降解是由于接触溶液的等离子体射流横切接触面大所致，表明•OH的无选择性氧化在降解NOR时起主要作用，其主要攻击对二氮己环、喹诺酮和苯环

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表 2 APPJ对环境有机染料去除的应用研究

Table 2. Application of atmospheric pressure plasma jets to the removal of environmental organic dyes

污染物名称	等离子体射流类型	射流反应器及处理方式	射流试验效果	射流试验机理
亚甲基蓝（MB）	氩气等离子体射流^[51]	由中空通气的不锈钢棒高压电极和置入圆底三口烧瓶外的不锈钢网状接地电极组成射流装置，采用射流置入液面上方的处理方式（距离为5 mm）	Ar等离子体射流在40 min内得到大于99%的降解率；在处理70 min时，在零级纯空气和N₂气源中的降解率分别为99%和89%；MB降解符合拟一级反应动力学，添加铁离子催化剂产生了芬顿反应，会促进了MB降解和矿化	Ar等离子体射流的降解性能最好，是由于在Ar等离子体射流下形成大量的H₂O₂
	常压非热微波氩气等离子体射流^[52]	等离子体液上射流装置，采用T型管射流装置置入液面上方（1 mm）的射流处理方式	随着MB初始浓度的降低（250×10⁻⁶~5×10⁻⁶），其去除率增大。MB拟一级动力学常数可达到0.177 min⁻¹，较高的Ar流速得到更高的MB降解速率；MB降解速率与Ar激发的活性物种强度和H₂O₂浓度有直接关系，H₂O₂能量产率可以达到2.7 mg/(kW·h)；当容积小于50 mL时，50%MB转化的能量产率为0.033~0.296 g/(kW·h)	Ar激发的活性物种和溶液中H₂O₂在MB降解过程中起到重要作用
	常压氦气等离子体液上射流^[53]	射流反应器由石英管内钨丝做高压电极，缠绕石英管的铝箔为接地极组成，采用射流喷头与液面的距离为5 mm的射流处理方式	最佳7.5 L/min的He流速下，等离子体活性物种OH、He^*、H_α、和OI会出现最大峰值；MB降解效率取决于射流处理时间与He流速	活性物种（OH、He^*、H_α和OI）溶解在MB溶液中，对MB分子分解起到关键作用
	单个或多个丝状介质阻挡放电(DBD)射频射流^[54]	Y型DBD等离子射流反应器，射流从液上置入液面以下的处理方式	以Ar/N₂混合气体作为气源，提高了能效和缩短了处理时间（仅6 min），射流浸入式的处理方式会缩短完全脱色处理时间	随着能量效率的增加，在Ar/N₂等离子体中RNS物种含ROS物种会积累，UV辐射也起到重要的作用
铬黑T （EBT）	氩气源等离子体液上射流^[55]	射流反应器是2个石英管外缠绕的铜条状电极组成的介质阻挡放电射流装置，采用石英射流喷头放置离溶液液面以上为1 cm处的处理方式	在Ar流速为0.5 L/min的Ar-APPJ处理6 min后，EBT脱色率高达约80%	HO·和O₂ ⁻·在EBT溶液的脱色过程中发挥着重要的作用，其射流放电会先破坏偶氮键，再将EBT分子的芳香环断裂为小分子化合物

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