基于紫外线的高级氧化工艺用于抗生素耐药性控制——效率、影响因素及能耗

韩佳芮 ,  李婉鑫 ,  Yun Yang ,  Xuanwei Zhang ,  Siyu Bao ,  张相如 ,  张彤 ,  Kenneth Mei Yee Leung

工程（英文） ›› 2024, Vol. 37 ›› Issue (6) : 28 -43.

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工程（英文） ›› 2024, Vol. 37 ›› Issue (6) : 28 -43. DOI: 10.1016/j.eng.2023.09.021
研究论文

基于紫外线的高级氧化工艺用于抗生素耐药性控制——效率、影响因素及能耗

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UV-Based Advanced Oxidation Processes for Antibiotic Resistance Control: Efficiency, Influencing Factors, and Energy Consumption

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摘要

携带抗生素抗性基因（ARGs）的抗生素抗性细菌（ARB）能够降低或消除抗生素的有效性，从而威胁人类健康。联合国环境规划署将抗生素抗性列为六个值得关注的新兴问题中的首要问题。结合紫外线（UV）照射和化学氧化（主要是氯、过氧化氢和过硫酸盐）的高级氧化工艺（AOPs）作为一种先进的水和污水处理技术，正受到越来越多的关注。由于能够产生多种活性物质，相比单独的紫外线照射或化学氧化，这些组合技术显著提高了ARB灭活和ARG降解的效率。本文基于最近的研究，回顾了UV/氯、UV/过氧化氢和UV/过硫酸盐工艺在控制ARB和ARG方面的性能及其潜在机制，讨论了影响这些工艺效率的因素，包括生物因素、氧化剂剂量、紫外线强度、pH值和水基质特性。此外，本文基于单位数量级能耗对不同UV-AOPs进行了成本效益评估。在污水处理基质中，UV/氯工艺显示出比其UV-AOPs更高的效率和更低的能耗，表明其在污水处理中用于ARB灭活和ARG降解的潜力。对于真实污水处理，需要进一步研究如何权衡UV/氯工艺的能效与有毒卤代副产物的形成，以促进其在控制ARB和ARG方面的优化和应用。

Abstract

Antibiotic resistant bacteria (ARB) with antibiotic resistance genes (ARGs) can reduce or eliminate the effectiveness of antibiotics and thus threaten human health. The United Nations Environment Programme considers antibiotic resistance the first of six emerging issues of concern. Advanced oxidation processes (AOPs) that combine ultraviolet (UV) irradiation and chemical oxidation (primarily chlorine, hydrogen peroxide, and persulfate) have attracted increasing interest as advanced water and wastewater treatment technologies. These integrated technologies have been reported to significantly elevate the efficiencies of ARB inactivation and ARG degradation compared with direct UV irradiation or chemical oxidation alone due to the generation of multiple reactive species. In this study, the performance and underlying mechanisms of UV/chlorine, UV/hydrogen peroxide, and UV/persulfate processes for controlling ARB and ARGs were reviewed based on recent studies. Factors affecting the process-specific efficiency in controlling ARB and ARGs were discussed, including biotic factors, oxidant dose, UV fluence, pH, and water matrix properties. In addition, the cost-effectiveness of the UV-based AOPs was evaluated using the concept of electrical energy per order. The UV/chlorine process exhibited a higher efficiency with lower energy consumption than other UV-based AOPs in the wastewater matrix, indicating its potential for ARB inactivation and ARG degradation in wastewater treatment. Further studies are required to address the trade-off between toxic byproduct formation and the energy efficiency of the UV/chlorine process in real wastewater to facilitate its optimization and application in the control of ARB and ARGs.

关键词

高级氧化工艺 / 紫外线/氯 / 紫外线/过氧化氢 / 紫外线/过硫酸盐 / 抗生素抗性细菌 / 抗生素抗性基因

Key words

Advanced oxidation processes / Ultraviolet/chlorine / Ultraviolet/hydrogen peroxide / Ultraviolet/persulfate / Antibiotic resistant bacteria / Antibiotic resistance genes

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韩佳芮,李婉鑫,Yun Yang,Xuanwei Zhang,Siyu Bao,张相如,张彤,Kenneth Mei Yee Leung. 基于紫外线的高级氧化工艺用于抗生素耐药性控制——效率、影响因素及能耗[J]. 工程（英文）, 2024, 37(6): 28-43 DOI:10.1016/j.eng.2023.09.021

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1 引言

抗生素被视为药学领域最重要的发明之一，因为它们能有效治疗细菌感染并延长寿命[1]。据估计，全球每年的抗生素消耗量在10万~20万吨之间[2]，且其使用量仍在持续增加。一项针对76个国家的抗生素消耗量调查显示，从2000年至2015年，抗生素消耗量增长了65% [3]。当细菌进化出对抗生素作用的抵抗力时，就会自然产生抗生素耐药性[4]。然而，包括抗生素滥用或过度使用在内的人为因素，极大地促进了抗生素抗性细菌（ARB）和抗生素抗性基因（ARG）的筛选[5‒6]。抗生素耐药性威胁到抗生素在治疗传染病方面的有效性，导致住院时间延长、治疗成本增加以及发病率和死亡率升高[5,7‒8]。据预测，到2050年，每年将有1000万人因抗菌药物耐药性而死亡[9]。世界卫生组织已宣布，抗生素耐药性是21世纪公共卫生面临的最严重威胁之一[9]。

固有耐药性、基因突变、垂直基因转移和水平基因转移被认为是抗生素耐药性产生和传播的主要机制[10‒11]。固有耐药性与阻止抗生素进入细胞膜、在特定抗生素到达目标之前通过外排泵将其排出以及抗生素降解甚至失活等行为有关。突变以多种方式导致抗生素耐药性，包括切换抗生素靶标、增加药物外排和降低靶基因表达[12]。垂直基因转移是指遗传物质从亲本细胞遗传而来，仅在微生物基因可转移至子代细胞时发生[13]。尽管细胞外ARG（e-ARG）的水平通常比细胞内ARG（i-ARG）低2~3个数量级，但e-ARG的传播可通过水平基因转移显著增强[10,14]。水平基因转移可通过基因转移载体、接合、转化和转导发生（图1 [10,15]）。基因转移载体类似病毒，可将宿主细胞的部分DNA转移到受体细胞，或是通过细胞裂解传播到受体细胞的游离微粒[10]。接合是指当细胞间接触时，可移动遗传载体携带的ARG从供体细胞传递到受体细胞[16]。转化过程是指自然可转化的细菌摄取、整合并功能性表达e-ARG。在转导过程中，供体细胞的i-ARG在DNA复制开始时被包装进噬菌体中，噬菌体携带的ARG在受体细胞被噬菌体感染后就会与其基因组结合[17]。抗生素耐药性出现和传播的多种机制凸显了ARB和ARG控制所面临的挑战[15,18]。

据报道，大约50%~90%的人用和兽用抗生素及其代谢物会以活性形式通过尿液和粪便排出体外[19]。来自家庭、养殖场和医院的含抗生素污水不断进入污水处理厂[20]，而传统的污水处理工艺无法有效地去除或灭活大部分抗生素[21‒22]。同时，生物处理单元中使用的活性污泥具有较高的微生物密度和多样性，这有利于水平基因转移[23]。由于污水中抗生素含量相对较高，并且活性污泥中的生物量也相当可观，因此污水处理厂被认为是促进ARB和ARG增殖的热点区域[24‒25]。有研究报道，生物处理后污水中tet基因的相对丰度增加了212%~358% [24]。由于传统污水处理工艺的去除效率不足，大量抗生素、ARB和ARG可能会进入水环境[25‒26]，因而饮用水源中经常会检测到ARB和ARG [24‒29]。最近，为了研究ARG的全球分布，Zhang等[4]从欧洲核苷酸档案库中收集了4572个宏基因组样本，其中1819个样本来自污水和水生环境。研究共鉴定出2561个ARG，它们共同对24类抗生素具有耐药性。只有25个ARG的检出频率高于75%，而大多数ARG的检出频率低于10%。水生环境中ARG的丰度差异显著，每个样本每百万读数中每千碱基的读数范围从小于0.005到296不等。通过综合考虑ARG的检出频率、丰度以及致病潜力等其他因素，确定了具有较高健康风险的ARG，并列于表1 [4]中。

UV和化学氧化剂（如氯）通常用于水和污水处理中的消毒，这被认为是控制微生物风险的最后一道也是最坚实的屏障[30]。为了灭活ARG，所需的UV剂量高于标准消毒实践中的剂量[26,31]。然而，有证据表明，紫外线和化学氧化可能会增加饮用水/污水中ARB和ARG的丰度[28,32‒35]。例如，研究发现，饮用水氯化可增加18种ARG亚型中14种的绝对丰度[36]。在一个真实污水处理厂中，发现氯化可使e-ARG的绝对丰度增加高达3.8倍，而使i-ARG的绝对丰度增加高达7.8倍[33]。Yuan等[34]报道，氯化使e-ARG的转化频率增加了2.9~7.2倍，因为氯化会产生细胞碎片，增强了e-ARG的吸附，从而增加其持久性和繁殖潜力。研究发现，紫外线处理可使污水中159种ARG的相对丰度增加6.0倍[32]。此外，ARB可能在经紫外线或化学氧化剂处理的水/污水中再生和重新激活[37‒38]。这种受损细胞的再生可能导致水平基因转移和抗生素耐药性的传播[39]，进一步危及水/污水的微生物安全。这些发现表明，仅通过紫外线照射或化学氧化处理不足以有效灭活ARB和降解ARG。

近年来，由于基于UV的高级氧化工艺（AOP）的活性物质的快速形成可显著促进ARB和ARG的减少，运用UV-AOPs以控制水环境中ARB和ARG相关风险引起了越来越多的关注[40‒48]。之前已有关于UV-AOPs技术在控制ARB和ARG方面的应用和性能的综述[31,49]。本研究对UV-AOPs控制ARB/ARG的最新进展进行了系统文献综述。基于紫外线的AOP主要包括UV/过氧化氢（H2O2）、UV/氯、UV/过硫酸盐、UV/臭氧和UV/催化剂工艺。关于使用UV/臭氧和UV/催化剂工艺处理ARB/ARG的研究报道较少[43,50‒53]，因此本研究重点关注UV/H2O2、UV/氯和UV/过硫酸盐工艺，讨论了三种UV-AOPs在各种环境和操作条件下灭活ARB和降解ARG的效率和机制，以提高对ARB和ARG控制的基本理解，并为UV-AOPs的工程设计提供指导。此外，基于单位数量级能耗（EE/O）的概念，对三种UV-AOPs的成本效益进行了系统评估和比较，这为决策者选择适合实际应用的工艺提供有益的启示。

2 UV-AOPs对ARB的灭活和ARG的降解

2.1 UV-AOPs在ARB灭活和ARG降解中的效率和机制

UV/氯工艺作为一种AOP，因其易于实施且在降解难降解微污染物（包括ARB和ARG）方面具有高效性而备受关注[54‒56]。表2 [44,56‒60]展示了在UV/氯、单独UV和单独氯化处理中ARB失活和ARG减少的数据。UV/氯工艺在灭活不同种类的ARB方面表现出强大的能力，其效率高于单独UV和单独氯化的总效率[49,57]。在使用UV/氯处理ARG时，也发现了ARG降解的协同效应。与单独使用氯（20 mg·L-1）或UV254（9.03 mW·cm-2）相比，40 min的UV/氯处理在磷酸盐缓冲盐水（PBS）中分别使tetM和blaTEM的降解量增加了0.98~3.20 log和1.28~3.36 log [57]。在污水处理厂中，UV254（0.1 mW·cm-2）和氯化（2 mg·L-1）的组合在1.3 min内额外减少了1.4 log ARB，并且在53 min内减少了1.0~1.5 log ARG [60]。此外，UV/氯处理显著抑制了ARB的再生和重新激活。

为了降低水环境中与ARB和ARG相关的风险，UV/H2O2工艺也得到了广泛的研究[61‒63]。在30 min的UV254（9.85 mW·cm-2）/H2O2（340 mg·L-1）处理中，污水中的目标ARG（sul1、tetX、tetG和intI1）丰度显著降低了1.55~2.32 log [64]。Michael等[65]也报道，通过90 min的UV254（3.46 mW·cm-2）/H2O2（5 mg·L-1）处理，目标ARG（即sul1、sul2、tetM、blaOXA-A和blaTEM）的丰度大幅降低，降低了2.0~3.7 log。相比之下，通过长达240 min的UV320‒450（17.4 μW·cm-2）/H2O2（20 mg·L-1）处理污水，目标ARG（包括blaTEM、qnrS和tetW）的丰度仅略有降低[66]。如表3 [41,45,62‒69]所示，通过UV/H2O2处理有效灭活ARB和降解ARG需要相对较高的UV通量和化学剂量，但其效率仍高于单独使用H2O2或UV的工艺。UV/H2O2工艺已被证明能显著抑制细菌的光活化和再生[70]。

通过紫外线照射激活过硫酸盐，包括过二硫酸盐（PDS）和过氧单硫酸盐（PMS），在对抗ARB和ARG方面展现出巨大的潜力[45‒47,71]。例如，在去除污水中的blaKPC-3时，UV254（2.3 μW·cm-2）/PDS（238 mg·L-1）过程比UV254（2.3 μW·cm-2）/H2O2（34 mg·L-1）过程更有效，两种过程在1 min内分别实现了80%和67%的blaKPC-3基因降解[45]。处理5 min后，UV254/PDS和UV254/H2O2过程均实现了超过98%的blaKPC-3基因降解。研究发现，UV254（100 μW·cm-2）/PMS（20 mg·L-1）处理在30 min内分别将sul1和intI1水平降低了2.9 log和3.4 log [42]。表4列出了在不同操作条件下使用UV254/PDS和UV254/PMS处理ARB和ARG的效率[42,45‒48,71‒73]。据报道，UV254和过硫酸盐的组合能有效灭活不同类型的ARB [如抗生素耐药性大肠杆菌（E. coli）、肺炎克雷伯氏菌（K. pneumonia）和假单胞菌属HLS-6]，与单独使用紫外线或过硫酸盐处理相比，观察到了协同效应[45‒47]。然而，对于不同的ARG，组合过程相对于单独的UV254或过硫酸盐过程的优越性有所不同。Zhou等[46]观察到，UV254（0.4 μW·cm-2）/PDS（238 mg·L-1）处理实现了比UV254照射（3.28 log）和PDS氧化（1.68 log）更高的总ARG减少水平（3.84 log）。具体而言，UV254/PDS降解了83.4%的大环内酯抗性基因，显著高于UV254照射的减少率（68.5%）和PDS氧化的减少率（35.9%）。相比之下，与单独使用UV照射相比，UV/PDS联合工艺对喹诺酮抗性基因的降解改善不足5% [46]。

据报道，与单独使用紫外线照射或化学氧化相比，基于UV的AOP通常能实现更高的ARB和ARG减少率，这被认为与孢子表面的破坏增强和ARB细胞内物质的明显释放有关[61,72]。基于UV的AOP对细胞膜的完整性造成有效破坏，促进了ARB的失活并抑制其再生。图2 [40,74]展示了基于UV的AOP如何去除ARB和ARG的示意图。尽管紫外线可以破坏细胞壁大分子，但紫外线照射灭活细菌的主要机制是导致DNA双链断裂和染色体畸变，进而通过坏死或凋亡导致细胞死亡[75]。据报道，化学氧化剂主要通过破坏细胞表面和改变膜通透性来灭活细菌[76]，其中氯的消毒效力高于过氧化氢和过硫酸盐[77‒78]。在UV/氯、UV/过氧化氢或UV/过硫酸盐过程中，可以产生多种自由基（图2，详见第2.2节）。产生的自由基具有高度氧化性，可引起明显的细胞表面损伤和细胞通透性增加[74,79]，这可能促进氧化剂和自由基与编码ARG的DNA反应，并通过紫外线照射促进DNA损伤[13]。同时，细胞通透性的增加使得i-ARG能够释放到水环境中并转化为e-ARG。研究表明，与i-ARG相比，e-ARG更容易被降解，因为它们更容易暴露于基于UV的AOP中的紫外线照射、化学氧化剂和自由基[79‒81]。

2.2 活性物质的形成及其作用

如式（1）~（6）所示，在UV/氯工艺中会产生多种活性氧化剂，包括羟基自由基（∙OH）和活性氯物种（RCS），如Cl∙、 C l 2 · -和ClO∙（图2）[31]。通过使用硝基苯（NB）等自由基清除剂清除∙OH，研究了不同自由基在处理ARB和ARG中的贡献（在UV/氯工艺中，∙OH的反应速率常数k ∙OH-NB = 3.9 × 109 L·mol-1·s-1）。添加硝基苯后，ARG的对数减少量几乎没有变化，表明在UV/氯工艺中∙OH对ARG降解的贡献微乎其微。在之前的研究[41,82]中也得到了类似的结果，表明∙OH对ARG降解的贡献较小是因为∙OH容易被细胞表面成分和细胞内基质消耗。然而，在以苯甲酸作为∙OH和RCS清除剂的样本中，tetM和blaTEM丰度的减少量与仅使用硝基苯作为∙OH清除剂时相当[57]，表明在UV/氯工艺中，∙OH而非RCS是tetM和blaTEM降解的主要因素。文献中关于各种自由基在ARG降解中的作用存在不一致，这可能是由于细菌菌株和实验条件（如紫外线和氯剂量）的不同造成的。

HOCl/OCl- + h ν → HO∙/O∙- + Cl∙
C l ·   +   C l -   ⇌   C l 2 · -   ( k + 1   =   6.5 × 10 9   L · m o l - 1 · s - 1 ,   k - 1   =   1.1 × 10 5   s - 1 )
H O C l   +   H O ·   →   C l O · + H 2 O   ( k   =   2.0 × 10 9   L · m o l - 1 · s - 1 )
O C l -   +   H O ·   →   C l O · + O H -   ( k   =   8.8 × 10 9   L · m o l - 1 · s - 1 )
H O C 1   +   C l ·   →   C l O · + H + + C l -   ( k   =   3.0 × 10 9   L · m o l - 1 · s - 1 )
O C 1 -   +   C l ·   →   C l O · + C l -   ( k   =   8.2 × 10 9   L · m o l - 1 · s - 1 )

在UV/H2O2过程中，∙OH是通过H2O2的光解产生的，而高浓度的H2O2可能充当∙OH的清除剂，如式（7）~（10）所示[67,83]。由于∙OH的高反应活性和非选择性，它会通过与细胞表面成分的反应迅速消耗，导致其对i-ARG的影响微乎其微[41,63]。然而，Meng等[48]观察到，与单独使用UV处理相比，UV/H2O2过程对i-ARG的降解作用要大得多。这可能是因为随着处理时间的增加，∙OH可以改变细菌膜的通透性，使UV照射和H2O2能够渗透到细胞中，随后与细胞内ARG编码的DNA发生相互作用。此外，据报道，细菌的细胞质可以与H2O2反应形成∙OH，这会降低酶活性，减弱代谢，并对DNA和RNA造成诱变性的结构损伤[45,84]。

H 2 O 2   +   h ν   →   2 H O ·
H 2 O 2   +   H O ·   →   H O 2 · + H 2 O ( k   =   2.7 × 10 7   L · m o l - 1 · s - 1 )
H O ·   +   H O 2 ·   →   O 2 + H 2 O ( k   =   6.6 × 10 9   L · m o l - 1 · s - 1 )
H O ·   +   H O ·   →   H 2 O 2 ( k   =   5.5 × 10 9   L · m o l - 1 · s - 1 )

UV/PDS和UV/PMS工艺是新型AOP，主要产生∙OH和SO 4 · -（图2）。在近中性pH条件下，涉及的主要化学反应如式（11）~（15）所示[85‒86]。在脱氧水（Φ = 1.4）和氧饱和水（Φ = 1.8）中，PDS在254 nm紫外光解产生的自由基量子产率（Φ）显著高于PMS（Φ = 1.04）和H2O2（Φ = 1.0）[87]。与∙OH相比，SO 4 · -具有更高的选择性、更长的半衰期（SO 4 · -为30~40 μs，∙OH为20 ns）和更高的氧化还原电位（SO 4 · -为2.5~3.1 V，∙OH为2.8 V）[88]。此外，SO 4 · -可以攻击鸟嘌呤杂环的π位，导致DNA修饰[42]。因此，据报道，在UV/PDS和UV/PMS工艺中，SO 4 · -是导致ARB失活和ARG降解的主要活性物种[45]。然而，UV/PDS或UV/PMS产生的不同自由基在细菌失活和基因降解中的作用可能受到细菌菌株和基因类型的影响。例如，当用UV/PDS处理海洋农业污水中的四环素抗性基因时，SO 4 · -和∙OH主要分别负责tetA和tetW的降解，且这两种自由基均对tetM的降解有显著贡献[89]。

S 2 O 8 2 - + h ν → 2 S O 4 • -  
H S O 5 - + h v → S O 4 • - + H O •
S O 4 • - + S O 4 • - → S 2 O 8 2 - k = 4 × 10 8   L · m o l - 1 · s - 1
S O 4 • - + H 2 O → S O 4 2 - + H O • + H +   k < 60   L · m o l - 1 · s - 1
S O 4 • - + H O • → H S O 5 -   k = 1 × 10 10   L · m o l - 1 · s - 1

3 影响UV-AOPs效率的因素

3.1 生物因素

胞外聚合物（EPS）是微生物来源的有机聚合物，包括多糖、蛋白质、胞外DNA和脂质[90]。作为生物膜的基本组成部分，EPS可以增强细菌对环境胁迫的抵抗力。EPS充当保护微生物免受外部损伤（如液体剪切力、抗生素和紫外线照射）的屏障[48,91]。对于基于UV的AOP，应首先降解致密的EPS层（例如，通过高活性自由基氧化EPS中的多糖和蛋白质），然后紫外线照射、化学氧化剂和自由基可以与细菌细胞相互作用。因此，基于UV的AOP对ARB和ARG的处理效率受到EPS基质的显著影响。处理效率还与细菌类型有关，因为不同的细菌对紫外线、氧化剂和自由基的外部干扰或破坏具有不同的抵抗力。Jia等[92]观察到，氯化可有效降低饮用水中的嗜甲基菌、甲基杆菌、沼杆菌和多核杆菌的水平，而氯化可增加饮用水中的假单胞菌、食酸菌、鞘氨醇单胞菌、邻单胞菌和波河杆菌的相对丰度。随着紫外线通量的增加，微生物群落中革兰氏阳性ARB的相对丰度增加[93]。这归因于革兰氏阳性ARB的肽聚糖层较厚，可抑制紫外线穿透[93]。此外，革兰氏阳性ARB的总基因组大小较小，可以降低其对紫外线照射的敏感性，因为它们具有较少的潜在嘧啶二聚体，而这些二聚体是DNA中紫外线照射的主要目标[94]。ARB的初始水平也可能影响处理性能。ARB的初始浓度较低可能与较高的灭活效率相关[42]，因为细菌细胞质可释放高浓度的有机物，在基于UV的AOP处理过程中消耗自由基。对于ARG的破坏，ARG的特性和结构是至关重要的影响因素。据报道，紫外线和氧化剂在降解不同类型基因方面的效率与目标位点、鸟嘌呤含量以及潜在二聚体的数量有关[42,95]。例如，紫外线诱导的ARG降解与相邻胸腺嘧啶位点的数量成正比，因为紫外线照射主要通过胸腺嘧啶二聚化导致DNA损伤[94]。

3.2 氧化剂剂量和紫外线通量

与ARB相比，通过氧化剂或紫外线照射去除ARG通常需要比传统工艺更高的UV和氧化剂剂量。然而，ARG的降解并不总是与氧化剂剂量成正比，因为氧化剂过量可能会引起自由基的自清除效应以及与目标ARG竞争光子的内滤效应[38,42]。最佳氧化剂剂量可能因不同的目标基因而异[44]。例如，在UV/氯工艺中，随着氯剂量增加至5 mg·L-1，sul1基因的降解率增加，而当氯剂量更高时，并未观察到进一步的增强效果[42]，相应地，去除intI1基因的最佳氯剂量为20 mg·L-1 [44]。Zhang等[54]还报道，在UV/氯工艺中，随着氯剂量从15 mg·L-1增加到25 mg·L-1，ARG降解的协同作用显著增强，而持续增加氯剂量对ARG减少的影响不显著。在UV/H2O2工艺中，当H2O2剂量为340 mg·L-1时，几种常见的ARG（如sul1、intI1、tetX和tetG）的减少量达到最大[64]；进一步增加H2O2剂量会导致目标ARG的降解效率降低，这归因于较高浓度的H2O2可猝灭·OH。同样，在UV/PMS工艺中，降解intI1基因的最佳PMS剂量为20 mg·L-1，而sul1基因的降解量随PMS剂量的增加而逐渐增加，直至PMS剂量达到30 mg·L-1 [42]。

对于基于UV的AOP，较高的UV通量通常会导致较高的ARB失活和ARG去除，并且基于通量的速率常数因不同的ARB和ARG而异[60,62‒63]。特别地，我们发现intI1的降解效率随着UV/PMS过程中UV通量的增加而波动[42]，这可能是由于其对直接UV光解的敏感性较低。除了UV通量外，ARB的失活效率还可能受到UV波长的影响[49,96]。与254 nm UV相比，265 nm UV可实现更高的细菌失活率[97]。为了灭活空肠弯曲杆菌，280 nm和300 nm UV的组合被证明具有最佳性能[98]。在对UV-AOPs的研究中，最常用的是低压紫外灯（LPUV），这主要是因为约82%的LPUV辐射在254 nm处释放（接近核酸在260 nm处的最大UV吸收）[99]。中压紫外灯（MPUV）利用汞蒸气，其UV辐射光谱在200~300 nm之间。MPUV灯比LPUV灯（功率密度和使用寿命分别为0.5~10 W·cm-1和8000~10 000 h）需要更高的电输入（功率密度为50~250 W·cm-1），且使用寿命较短（4000~8000 h）。但MPUV灯的特点是尺寸紧凑，应用广泛[100]。UV发光二极管（LED）是一种新兴的UV光源。尽管UV-LED的电光效率相对较低（通常低于10%），但其不含汞、波长可变且寿命长，使其成为传统UV灯的有吸引力的替代品[40,55,101]。有必要进一步研究使用不同紫外线源的UV-AOPs对ARB和ARG的控制。

3.3 pH值

水生环境的pH值可能会有很大差异。尽管之前的研究表明，pH值对UV直接光解导致的ARB的失活和ARG的降解影响不大[41,102]，但pH值在活性物种的形成和转化中起着至关重要的作用，因此会显著影响UV-AOPs工艺的效率。一般来说，酸性条件有利于UV-AOPs对ARB和ARG的控制。

UV/氯工艺通常在酸性环境中表现更佳[44,103]，这主要是因为HOCl和OCl-（pK a = 7.5）的物种分布。在酸性条件下，氯的主要物种是HOCl，它比OCl-具有更高的自由基生成量子产率和更低的自由基清除能力[104]。此外，由于HOCl具有更强的氧化能力，因此在降解ARG方面比OCl-更有效[101]。当样品pH值从5增加到9时，UV/氯处理中sul1和intI1的减少呈下降趋势[44]。根据式（3）~（6），HOCl对∙OH和Cl∙的清除速度远低于OCl-，导致在碱性条件下sul1和intI1的降解减少。对于对ClO∙敏感的ARG，其降解可能会随着pH的增加而增加。Yao等[105]报道，随着pH从6增加到8，blaNDM-1和sul2的对数减少量略有增加，这主要是由于ClO∙水平的升高。在水/污水处理条件下，UV/H2O2处理ARB和ARG的效率通常随着pH值的增加而降低[64,106]。例如，在UV/H2O2处理污水期间，目标ARG（即sul1、intI1、tetX和tetG）的降解随着pH从3.5增加到9.0而减少[64]。在碱性条件下，H2O2/HO 2 -平衡（pK a = 11.7）中HO 2 -的生成变得显著[107]。生成的HO 2 -可以进一步与H2O2反应[式（16）]，导致∙OH浓度降低。此外，∙OH与HO 2 -的反应速率常数比与H2O2的反应速率常数[见方程式（8）和（17）]高出100倍以上，这意味着对∙OH的清除随pH值的增加而增强。

HO 2 - + H2O2 → O2 + H2O + OH-
H O 2 - + H O · → H O 2 · + H O - ( k   =   7.5 × 10 9   L · m o l - 1 · s - 1 )

在UV/PDS或UV/PMS工艺中，在水或污水处理中，随着pH值的增加，ARB的失活会减少[84,101]，这归因于PDS或PMS的分解增强以及自由基物种的转化[108]。同样，在pH值5~9的范围内，酸性条件下UV/PMS工艺对目标ARG（sul1和intI1）的还原效果更佳[42]。在碱性条件下，由UV激活的PDS或PMS形成的SO 4 · -可以与OH-反应生成∙OH[见方程式（18）]。SO 4 · -和∙OH的共存可能导致自由基迅速转化为PMS，如式（15）所示[109]，这对UV/过硫酸盐工艺的性能产生负面影响。然而，在pH值为3.4、7.3和11.1的UV/PDS处理中，有研究观察到目标ARG（即blaTEM、qnrS、tetW和tetE）的降解变化小于20% [110]，这可能是由于SO 4 · -和∙OH对ARG降解的贡献相当。

S O 4 · -   +   O H - → H O · +   S O 4 2 - ( k   =   6.5 × 10 7   L · m o l - 1 · s - 1 )

pH值也会影响H2CO3/HCO 3 -（pK a = 6.4）和HCO3 -/CO 3 2 -（pK a = 10.3）的分布。CO 3 · -可以通过∙OH、RCS或SO 4 · -与HCO 3 -或CO 3 2 -的反应产生[见式（19）至式（21）][103]。研究发现，在UV/氯过程中，CO 3 · -的浓度远高于UV/H2O2过程[104]，而后者又可能高于UV/过硫酸盐过程，这是由于HCO 3 -与Cl∙、∙OH和SO 4 · -的反应速率常数逐渐降低。随着pH值的增加，HCO 3 -和CO 3 2 -的比例也可能增加，这对ARB的失活和ARG的降解不利，因为它们具有自由基清除作用。

HCO 3 -/CO 3 2 - + HO· → CO 3 · - + H2O/OH-

( k H C O 3 - = 8.5×106 L·mol-1·s-1, k C O 3 2 - =

3.9 ×108 L·mol-1·s-1)

HCO 3 -/CO 3 2 - + Cl· → CO 3 · - + HCl/Cl-

( k H C O 3 - = 2.2×108 L·mol-1·s-1, k C O 3 2 - =

5.0 ×108 L·mol-1·s-1)

HCO 3 -/CO 3 2 - + SO 4 · - → CO 3 · - + HSO 4 -/SO 4 2 -

( k H C O 3 - = 1.6×106 L·mol-1·s-1, k C O 3 2 - =

6.1 ×106 L·mol-1·s-1)

3.4 水基质

越来越多的研究聚焦于真实水/污水中的ARB失活和ARG降解，其中水基质[如悬浮固体、溶解有机物（DOM）、无机阴离子和金属]可能会显著影响UV-AOPs的效率[71,111‒113]。悬浮固体对UV-AOPs效率的负面影响，即屏蔽ARB/ARG使其免受紫外线照射和化学氧化，已得到广泛认可。例如，在PBS中，UV/PDS对碳青霉烯类耐药肺炎克雷伯菌的失活率是二级污水出水中的三倍[45]。相对地，Yoon等[41]发现，与PBS相比，在过滤后的污水出水（即无悬浮固体）中，ARG降解只需要消耗稍高的紫外线通量。虽然水基质中的DOM是自由基的主要消耗者，但它对化学氧化剂和紫外线照射的消耗有限[49,103]。据报道，与无DOM的条件相比，DOM的存在会抑制UV/H2O2和UV/PDS过程对ARG的降解[63,95]，这是由于DOM对自由基的清除作用。在5 mg·L-1 DOM存在下，UV/氯过程中自由基显著减少，Cl∙、∙OH和ClO∙的浓度分别降低了18%、27%和99% [103]。有趣的是，当仅使用紫外线照射时，DOM的存在甚至可以增强ARG的降解，这归因于DOM可通过紫外线光解产生活性物种[63,95]。

水基质中无机阴离子（如Cl-、Br-和SO 4 2 -）的存在可能会通过自由基清除作用影响基于UV的AOP的性能[104]。对于不易受自由基影响的ARB/ARG，无机阴离子对其去除效果的影响微乎其微[72,105]。研究发现，在PMS处理系统中，氯化物的存在会增强对大肠杆菌和芽孢杆菌孢子的灭活作用，这是由于PMS与Cl-反应形成HOCl/OCl- [114]。文献[111,115]报道，由于金属对ARG的共选择作用以及在亚抑制浓度下金属对水平基因转移的促进作用，金属[如Ag(I)、Cu(II)、Hg(II)、Zn(II)和Cr(VI)]与水环境中的ARG水平呈正相关。例如，环境相关浓度（1~100 μmol·L-1）的Cu(II)可以通过增加细胞膜通透性和改变接合调节因子来增加质粒编码ARG的接合频率[112]。在基于UV的AOP中，具有多种氧化还原状态的金属[如Cu(I)/Cu(II)、Fe(II)/Fe(III)和Mn(II)/Mn(IV)]的存在可以催化H2O2和过硫酸盐的分解，并通过Fenton和类Fenton反应分别产生∙OH和SO 4 · - [116,117]。铜与H2O2、PDS或PMS在紫外线系统中的反应如式（22）至式（25）所示。在含Fe(II)的系统中，可以形成Fe(IV)，并有助于脂质过氧化和DNA损伤[113]。

Cu2+ + h ν → Cu+
Cu+ + H2O2 → HO· + OH- + Cu2+
Cu+ + S2O 8 2 - → SO 4 · - + SO 4 2 - + Cu2+
Cu+ + HSO5 - → SO 4 · - + OH- + Cu2+

4 UV-AOPs的成本效益分析

影响新技术应用的最关键因素之一是成本，这包括资本成本和运营成本。有报道表明，UV-AOPs的资本成本低于其他高级处理技术，如臭氧氧化和膜技术（如反渗透）[118]。为了进一步评估本研究中讨论的UV-AOPs的成本效益，我们评估了它们在ARB/ARG处理中的运营成本（包括能耗和化学氧化剂成本）。运营成本可以通过EE/O [即将一立方米水样中的ARB/ARG水平降低一个数量级所需的电能（kW·h·m-3·order-1）]进行粗略估算[109,119]，包括紫外线源的电能（EE/OUV）和氧化剂消耗的等效电能（EE/Ooxidant）。EE/O值可以使用式（26）至式（28）计算：

E E / O   = E E / O U V   +   E E / O o x i d a n t
E E / O U V   =   A   ×   I   ×   t 1000   ×   E   ×   V   ×   l g C 0 C t
E E / O o x i d a n t   =   E q o x i d a n t   ×   D o x i d a n t   × 1000 l g C 0 C t

式中，A代表受照射表面积（cm2）；I代表紫外线通量（mW·cm-2）；t代表反应时间（h）；V代表处理水样的体积（L）；E代表电光转换效率。由于在对利用UV-AOPs处理ARB和ARG的研究中，LPUV是最常用的紫外线源，根据Wan等[120]的研究，我们采用了E = 0.32取值。C 0和C t分别代表所选ARG的初始浓度和最终浓度。Eqoxidant表示生成一摩尔氧化剂所需的电能消耗（kW·h·mol-1），而D oxidant表示氧化剂的剂量（mol·L-1）。利用平均电费[约为0.193 美元·(kW·h)-1] [121]以及知名电子商务平台上制造商和供应商提供的化学品价格，我们计算出氯、H2O2、PDS和PMS的Eqoxidant值分别为4.64 kW·h·mol-1、3.44 kW·h·mol-1、4.98 kW·h·mol-1和7.79 kW·h·mol-1。根据先前研究中报道的用于ARB/ARG处理的紫外线通量和化学剂量（表2至表4），我们确定了不同UV-AOPs中能源消耗和化学氧化剂的成本。

图3展示了不同UV-AOPs工艺在PBS或污水中处理ARB/ARG时的EE/OUV和EE/Ooxidant。EE/O值较高表明相应处理的能效较低[119]。在PBS和污水中，UV/氯、UV/H2O2和UV/过硫酸盐工艺对ARG降解的EE/O中值分别是ARB灭活的中值的7.7倍和29.7倍。这表明，与ARG降解相比，基于UV的AOP在ARB灭活方面通常非常有效。在PBS溶液中，UV/过硫酸盐工艺是最具成本效益的UV-AOPs [图3（a）]。在UV/过硫酸盐工艺中，用于ARG降解的EE/OUV和EE/Ooxidant的中值（分别为0.064 kW·h·m-3和0.324 kW·h·m-3·order-1）低于UV/氯（分别为0.334 kW·h·m-3·order-1和0.408 kW·h·m-3·order-1）和UV/H2O2（分别为0.266 kW·h·m-3·order-1和1.720 kW·h·m-3·order-1）工艺的相应值。在没有水基质干扰的PBS溶液中，UV/H2O2工艺的EE/Ooxidant相对较高，这可能是由于H2O2的吸光系数（18.6 mol-1·cm-1）低于其他氧化剂（例如，HOCl的吸光系数为59 mol-1·cm-1，PDS的吸光系数为27.5 mol-1·cm-1）在紫外254 nm处的吸光系数[55,122]。UV/H2O2工艺通常需要过量的H2O2，因为只有5%~10%的H2O2被紫外线光解消耗，这导致化学成本增加[122]。需要额外的化学物质来去除剩余的H2O2；因此，UV/H2O2工艺的操作相对复杂，在能量利用方面效率较低[123]。然而，在污水基质中，UV/氯工艺的能量效率高于其他基于UV的AOPs [图3（b）]。尽管UV/过硫酸盐工艺对ARG降解的中值EE/OUV（0.179 kW·h·m-3·order-1）低于UV/氯和UV/H2O2工艺（分别为0.421 kW·h·m-3·order-1和0.277 kW·h·m-3·order-1），但中值EE/Ooxidant显著增加至9.68 kW·h·m-3·order-1。在污水中UV/氯的较高能量效率可能源于氯比H2O2和过硫酸盐具有更高的消毒效率[76‒77]，以及RCS与∙OH和SO 4 · -相比具有较高的选择性[124]。关于去除废水中的新兴污染物成本效益的分析，也报道了类似的结果[118,125]。Guo等[119]报道，UV/氯工艺去除有机污染物所需的电能低于UV/H2O2工艺。在降解新兴污染物方面，与UV/H2O2工艺相比，UV/氯工艺可节省30%~75%的电能，从而显著降低30%~50%的运营成本，并可能降低资本成本，因为UV/氯工艺所需的反应室数量更少[118]。之前的一项综述[126]总结了基于UV的AOP在药物降解方面的能量效率，并指出EE/O值遵循以下顺序：EE/OUV/catalyst > E E / O U V / H 2 O 2 > EE/OUV/persulfate > EE/OUV/chlorine。

值得注意的是，在EE/O分析中，UV/氯（n = 9）和UV/过硫酸盐（n = 13）工艺的可用数据量（n）小于UV/H2O2工艺（n = 27），这可能是因为UV/氯和UV/过硫酸盐是新型的AOP。因此，有必要对不同UV-AOPs降解ARG进行更多研究，以进一步完善EE/O分析。此外，尽管UV/氯工艺在处理ARB和ARG方面成本效益较高，但在此过程中，DOM与氯和RCS的反应容易形成卤代消毒副产物（DBP）[104,127,128]。据报道，UV/氯处理饮用水和污水产生的卤代DBP比单独氯化产生的更多[128,129]。由于许多卤代DBP具有细胞毒性、遗传毒性和发育毒性[130‒135]，已观察到经UV/氯处理的污水因生成DBP而毒性增加[136]。因此，在应用UV/氯工艺之前，应全面评估因有毒卤代副产物形成而带来的风险。

5 结论与展望

基于UV的AOPs（如UV/氯、UV/H2O2和UV/过硫酸盐）被视为解决与 ARB 和 ARGs 相关的紧迫健康问题的前景较好的控制技术。由于其能产生多种活性物种，这些AOP系统显示出比单独的紫外线光解或化学氧化更高的处理效率。然而，主要负责ARB灭活和ARG降解的特定活性物种取决于目标细菌菌株和基因类型。UV-AOPs的效率可能受到诸如目标ARB和ARG的类型和条件、化学剂量和紫外线通量、pH值及水基质特性等因素的影响。这些影响因素的组合效应进一步增加了基于UV-AOPs控制ARB和ARG的复杂性。为了评估使用UV-AOPs工艺控制ARB和ARG的可行性，我们分析了UV/氯、UV/H2O2和UV/过硫酸盐工艺的EE/O值（考虑了LPUV灯消耗的电能和所需化学氧化剂）。EE/O的计算结果表明，虽然UV/过硫酸盐工艺在PBS溶液中显示出最佳的能量效率，但UV/氯过程在实际污水中最为有效。不同的EE/O排名顺序凸显了水基质对UV-AOPs效率的影响。此外，所使用的紫外线灯类型（如LPUV与MPUV和UV-LED）和处理能力（如实验室规模与中试规模和全规模）也可能影响对不同UV-AOPs的成本评估，因此需要进一步的调查和系统评估。值得注意的是，尽管UV/氯过程在控制ARB和ARG方面比其他UV-AOPs更具成本效益，但在UV/氯工艺中形成的有毒副产物可能会抵消其优势，因此对该工艺的应用需要谨慎评估。

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