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Article(id=1156908035001115264, tenantId=1146029695717560320, journalId=1146123166801305609, issueId=1156907871645556837, articleNumber=null, orderNo=null, doi=10.12404/j.issn.1671-1815.2309115, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=1700409600000, receivedDateStr=2023-11-20, revisedDate=1719158400000, revisedDateStr=2024-06-24, acceptedDate=null, acceptedDateStr=null, onlineDate=1753757969856, onlineDateStr=2025-07-29, pubDate=1737993600000, pubDateStr=2025-01-28, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1753757969856, onlineIssueDateStr=2025-07-29, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1753757969856, creator=13701087609, updateTime=1753757969856, updator=13701087609, issue=Issue{id=1156907871645556837, tenantId=1146029695717560320, journalId=1146123166801305609, year='2025', volume='25', issue='3', pageStart='879', pageEnd='1312', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=0, createTime=1753757930909, creator=13701087609, updateTime=1765095544280, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1204461268821320541, tenantId=1146029695717560320, journalId=1146123166801305609, issueId=1156907871645556837, language=EN, specialIssueTitle=, coverIllustrator=, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1204461268825514846, tenantId=1146029695717560320, journalId=1146123166801305609, issueId=1156907871645556837, language=CN, specialIssueTitle=, coverIllustrator=, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=1298, endPage=1305, ext={EN=ArticleExt(id=1156908035793838725, articleId=1156908035001115264, tenantId=1146029695717560320, journalId=1146123166801305609, language=EN, title=Removal Efficiency and Influencing Factors of Antibiotic Resistance Genes in Secondary Effluent by the Process of O3 -PAC-UF, columnId=1156262729993277777, journalTitle=Science Technology and Engineering, columnName=Papers·Environmental and Safe Science, runingTitle=null, highlight=null, articleAbstract=

ARGs(antibiotic resistance genes) as emerging environmental pollutants threaten human health, and studies show that secondary effluent from sewage treatment plants is an important source of ARGs in the environment. Ozone pre-oxidation combined with PAC(powdered activated carbon) and UF(ultrafiltration) was used to treat the secondary effluent from the wastewater treatment plant, and the factors and mechanisms of O3 dosage, pH, and temperature on the removal of different forms of ARGs in the secondary effluent were investigated. The results show that ARGs could be more effectively removed by PAC adsorption and UF after oxidative inactivation by O3; under the condition of optimal O3 dosage (2.0 mg/L), the combined O3-PAC-UF process could remove different types of ARGs (tetA, tetC, tetG, sulI, sulII) and other pollutants (intⅠ1, 16S rRNA) from the secondary effluent. The removal of different types of ARGs (tetA, tetC, tetG, sulI, sulII) and other pollutants (intⅠ1, 16S rRNA) by the combined process is 102.67~103.92 copies/mL, and the removal of cellular and free ARGs is significantly enhanced; the elevated pH and lower temperature facilitate the removal of ARGs; the direct oxidation of O3 molecules dominate the removal of ARGs in the secondary effluent. In conclusion, ozone combined with PAC and UF can effectively remove antibiotic resistance genes from secondary effluent.

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抗生素抗性基因(antibiotic resistance genes, ARGs)作为新兴环境污染物已对人类健康造成威胁,有研究表明,污水处理厂的二级出水是环境中ARGs的重要来源。采用O3预氧化结合粉末活性炭(powdered activated carbon,PAC)与超滤(ultrafiltration,UF)组合工艺处理污水厂二级出水,考察O3投加量与水样的pH、温度对二级出水中不同形态ARGs去除效果的影响因素和作用机理。结果表明:ARGs被O3氧化失活后,经过PAC吸附与UF膜的过滤能得到更为有效的去除;在O3最佳投加量(2.0 mg/L)条件下,O3-PAC-UF组合工艺对二级出水中不同类型ARGs(tetA、tetC、tetG、sulI、sulII)和其他污染物(intⅠ1、16S rRNA)的去除量为102.67 ~ 103.92 copies/mL,且对细胞态和游离态ARGs去除效果明显增强;升高pH和较低温度均利于ARGs的去除;O3分子的直接氧化作用居于二级出水中ARGs去除机制的主导地位。综上,臭氧联合粉末活性炭与超滤组合可以有效去除二级出水中的抗生素抗性基因。

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孙丽华(1978—),女,汉族,山东烟台人,博士,教授。研究方向:再生水处理及膜法水处理技术。E-mail:。

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孙丽华(1978—),女,汉族,山东烟台人,博士,教授。研究方向:再生水处理及膜法水处理技术。E-mail:。

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孙丽华(1978—),女,汉族,山东烟台人,博士,教授。研究方向:再生水处理及膜法水处理技术。E-mail:。

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臭氧氧化-粉末活性炭-超滤对污水厂二级出水中抗生素抗性基因的去除效能及影响因素
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孙丽华 1 , 邓斯 2 , 史鹏飞 3 , 王春芳 1
科学技术与工程 | 论文·环境科学、安全科学 2025,25(3): 1298-1305
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科学技术与工程 | 论文·环境科学、安全科学 2025, 25(3): 1298-1305
臭氧氧化-粉末活性炭-超滤对污水厂二级出水中抗生素抗性基因的去除效能及影响因素
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孙丽华1 , 邓斯2, 史鹏飞3, 王春芳1
作者信息
  • 1.北京建筑大学城市, 雨水系统与水环境教育部重点实验室, 北京 100044
  • 2.北京建筑大学环境与能源工程学院, 北京 100044
  • 3.北京市市政工程设计研究总院有限公司, 北京 100082

    • 孙丽华(1978—),女,汉族,山东烟台人,博士,教授。研究方向:再生水处理及膜法水处理技术。E-mail:。

Removal Efficiency and Influencing Factors of Antibiotic Resistance Genes in Secondary Effluent by the Process of O3 -PAC-UF
Li-hua SUN1 , Si DENG2, Peng-fei SHI3, Chun-fang WANG1
Affiliations
  • 1. Key Laboratory of Urban Rainwater System and Water Environment Ministry of Education,Beijing University of Civil Engineering and Architecture, Beijing 100044, China
  • 2. School of Environmental and Energy Engineering, Beijing University of Civil Engineering and Architecture, Beijing 100044, China
  • 3. Beijing General Municipal Engineering Design & Research Institute Co., Ltd., Beijing 100082, China
出版时间: 2025-01-28 doi: 10.12404/j.issn.1671-1815.2309115
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摘要
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抗生素抗性基因(antibiotic resistance genes, ARGs)作为新兴环境污染物已对人类健康造成威胁,有研究表明,污水处理厂的二级出水是环境中ARGs的重要来源。采用O3预氧化结合粉末活性炭(powdered activated carbon,PAC)与超滤(ultrafiltration,UF)组合工艺处理污水厂二级出水,考察O3投加量与水样的pH、温度对二级出水中不同形态ARGs去除效果的影响因素和作用机理。结果表明:ARGs被O3氧化失活后,经过PAC吸附与UF膜的过滤能得到更为有效的去除;在O3最佳投加量(2.0 mg/L)条件下,O3-PAC-UF组合工艺对二级出水中不同类型ARGs(tetA、tetC、tetG、sulI、sulII)和其他污染物(intⅠ1、16S rRNA)的去除量为102.67 ~ 103.92 copies/mL,且对细胞态和游离态ARGs去除效果明显增强;升高pH和较低温度均利于ARGs的去除;O3分子的直接氧化作用居于二级出水中ARGs去除机制的主导地位。综上,臭氧联合粉末活性炭与超滤组合可以有效去除二级出水中的抗生素抗性基因。

抗生素抗性基因  /  二级出水  /  超滤  /  臭氧  /  粉末活性炭

ARGs(antibiotic resistance genes) as emerging environmental pollutants threaten human health, and studies show that secondary effluent from sewage treatment plants is an important source of ARGs in the environment. Ozone pre-oxidation combined with PAC(powdered activated carbon) and UF(ultrafiltration) was used to treat the secondary effluent from the wastewater treatment plant, and the factors and mechanisms of O3 dosage, pH, and temperature on the removal of different forms of ARGs in the secondary effluent were investigated. The results show that ARGs could be more effectively removed by PAC adsorption and UF after oxidative inactivation by O3; under the condition of optimal O3 dosage (2.0 mg/L), the combined O3-PAC-UF process could remove different types of ARGs (tetA, tetC, tetG, sulI, sulII) and other pollutants (intⅠ1, 16S rRNA) from the secondary effluent. The removal of different types of ARGs (tetA, tetC, tetG, sulI, sulII) and other pollutants (intⅠ1, 16S rRNA) by the combined process is 102.67~103.92 copies/mL, and the removal of cellular and free ARGs is significantly enhanced; the elevated pH and lower temperature facilitate the removal of ARGs; the direct oxidation of O3 molecules dominate the removal of ARGs in the secondary effluent. In conclusion, ozone combined with PAC and UF can effectively remove antibiotic resistance genes from secondary effluent.

ARGs  /  secondary effluent  /  UF  /  O3  /  PAC
孙丽华, 邓斯, 史鹏飞, 王春芳. 臭氧氧化-粉末活性炭-超滤对污水厂二级出水中抗生素抗性基因的去除效能及影响因素. 科学技术与工程, 2025 , 25 (3) : 1298 -1305 . DOI: 10.12404/j.issn.1671-1815.2309115
Li-hua SUN, Si DENG, Peng-fei SHI, Chun-fang WANG. Removal Efficiency and Influencing Factors of Antibiotic Resistance Genes in Secondary Effluent by the Process of O3 -PAC-UF[J]. Science Technology and Engineering, 2025 , 25 (3) : 1298 -1305 . DOI: 10.12404/j.issn.1671-1815.2309115
正文
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再生水可有效应对水资源短缺,已被广泛应用于市政杂用、居民生活等领域[1]。其中,污水处理厂的二级出水具有水量大、水质稳定等优点,是再生水深度净化的补给水源。而抗生素抗性基因(antibiotic resistance genes, ARGs)是一种新兴的环境污染物[2],其可致细菌耐药性增加,使抗生素失去疗效,并在水环境中持久存在,对公共健康和生态安全造成了严重威胁[3-4]。四环素和磺胺是全球最常用的抗生素,研究表明,四环素类抗性基因(tetA 、tetC和tetG)和磺胺类抗性基因(sulⅠ和sulⅡ)在国内外的污水处理厂二级出水中被高频检出[5]。此外,16S rRNA为核糖体RNA的一个亚基,其浓度可用来表征微生物总量。整合子是一种常见的可移动遗传元件,已成为环境中不同菌属间ARGs和多重抗药性传播的重要途径[6-7]。目前发现了5种整合子,其中Ⅰ类整合子(intI1)最为常见。
传统污水处理厂无法有效控制废水中抗生素和ARGs的排放,亚抑制浓度抗生素的持续选择和污水处理厂内丰富的营养环境所造就的高密度微生物环境为ARGs的传播提供了有利的环境,故而污水处理厂被认为是 ARGs 水平转移的高发区[8-9]。因此,在常规污水处理后增加深度处理,以提高ARGs的去除率已迫在眉睫。已有研究表明,采用膜过滤、活性炭吸附或氧化等深度处理工艺可有效去除ARGs[10]。膜技术中的超滤(ultrafiltration,UF)因所需压力及成本较低等优点,更适合于处理污水处理厂二级出水。Yang等[11]发现,ARGs分子量区间为1.0×1 0 - 1  ~ 9.0×103 kDa,当高速水流通过膜孔时,ARGs由于其柔性可以在流体中伸展和拉长,挤压通过比其小得多的膜孔。因此直接UF对水中ARGs去除效果有限,分子量较小、亲水性较强的污染物难以被有效去除[12],可将粉末活性炭(powdered activated carbon,PAC)引入UF系统。PAC具有高比表面积、发达的孔隙结构和较强的吸附能力,在去除水中污染物等方面具有突出优势[13],姜蕾等[14]发现粉末活性炭投加量为10~30 mg/L、反应时间为30~1 800 min条件下,抗生素总去除率为13.8%~52.5%。但PAC-UF工艺仅把污染物从水中转移到了PAC或UF的表面,未对其造成实质性破坏,可以进一步联用氧化工艺利用氧化反应损坏DNA结构[15],O3因其具有氧化彻底、过程不产生二次污染等优点而备受学者关注,相较于标准氢电极,O3的标准氧化还原电位高达2.07 V[16],其对微生物的氧化非常迅速,可通过与细菌细胞壁脂类双键反应穿入菌体内部,改变细胞通透性[17]。苏超[18]的研究表明,低浓度的O3也可有效去除废水中30%~50%的tet基因和sul基因。由此可见,单个的处理方式对ARGs的去除各有利弊,构建合适的组合工艺有望解决这一困境,但目前采用O3预氧化-PAC-UF组合工艺用于处理二级出水中ARGs的研究,国内外鲜见报道。
通过与直接UF,PAC-UF联用等工艺比较,评价O3-PAC-UF组合工艺对城市污水厂二级出水中不同种类ARGs(tetA、tetC、tetG、sulⅠ,sulⅡ)与其他污染物(intⅠ1,16S rRNA)浓度的去除效能,分析氧化、吸附及过滤过程对水中不同形态(细胞态和游离态)ARGs的作用机制,并探究该组合工艺的影响因素(pH和温度)和自由基作用机理,为再生水的安全回用提供技术保障。
1 试验材料与方法
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1.1 试剂材料
二级出水水样,为北京市某污水厂二沉池出水(4 ℃恒温保存,在24 h 内完成处理),其部分水质指标均值分别是pH=7.40,浊度为1.35 NTU,溶解性有机碳(dissdoved organic carbin,DOC)质量浓度为18.30 mg/L,NH3-N质量浓度为1.75 mg/L,总磷(total phosphorus,TP)质量浓度为1.56 mg/L。
试验采用的硫代硫酸钠为分析纯;超滤膜片材质为再生纤维素的平板超滤膜(Mmodel 8400,美国Millipore公司),膜孔径为100 kDa,4 ℃恒温储存;PAC为上海熙碳环保科技有限公司生产,材质为杏壳,粒度为200 ~ 300 目,粒径为0.048 ~ 0.075 mm,比表面积为587.38 m2/g,平均孔径为3.351 nm。
1.2 试验装置
1.2.1 臭氧氧化装置
试验中采用普通纯氧通过臭氧发生器(3S-T10,北京同林臭氧有限公司)制备臭氧,通过流量计和臭氧分析仪(3S-J5000,北京同林臭氧有限公司)固定有效臭氧气体浓度为1.0 mg/min,臭氧接触时间设置为1.0、2.0、3.0、4.0 min,以分别达到1.0、2.0、3.0、4.0 mg/L的目标臭氧投加量。臭氧化反应需要20 min,投加硫代硫酸钠溶液终止反应。
1.2.2 超滤装置
经氧化后的水样分别投加20 mg/L PAC并恒温振荡24 h,随后进行超滤试验。超滤实验是在超滤杯(Amicon 8400,美国Millipore公司)中以死端模式进行,恒定压力为100 kPa,由连接到超滤杯的氮气瓶提供。试验装置如图1所示。
1.3 试验方法
1.3.1 ARGs检测分析
剪碎超滤杯中过滤后的膜片,提取DNA,采用荧光定量聚合酶链式反应(PCR)进行PCR扩增,检测水中3种四环素类基因(tetA、tetC、tetG)、2种磺胺类基因(sul I、sulⅡ )、Ⅰ类整合子(intI1)和微生物总量(16S rRNA),通过PCR筛选阳性克隆并测序,制作定量PCR标准曲线,并计算每毫升质粒溶液中ARGs基因的拷贝数以表示抗性基因在水中的含量,计算公式为拷贝数(copies/μL)=浓度(ng/μL)×6.02×1014/[(2 692+片段长度)×660],其中2 692为载体长度。
1.3.2 细胞态及游离态ARGs检测
水样存放于1 L体积的无菌瓶后分装成两份,一份用于检测总ARGs浓度,直接提取DNA进行检测;另一份水样用于检测细胞态ARGs浓度,向水样中加入脱氧核糖核酸酶500 U单位,先在15 ℃下振荡2 h,然后升温至80 ℃维持10 min,对游离态ARGs进行降解后再提取水样中的 DNA,检测细胞态ARGs浓度。由ARGs总浓度与细胞态ARGs 浓度之差可以得到游离态ARGs 浓度。
1.3.3 自由基浓度测定
羟基自由基OH·含量可通过高效液相色谱法(high performance liquid chromatography,HPLC)对羟基苯甲酸(p-HBA)含量进行测定,以定量分析体系中产生 OH·的含量。p-HBA 是由OH·与苯甲酸(BA)反应生成的稳定产物。使用Cosmosil C18-PAQ色谱柱(4.6×250 mm)对羟基苯甲酸(p-HBA)进行检测,流动相是乙腈和1% TFA / 水(65.35,体积比)的混合物,流速为1 mL/min,检测波长为255 nm,仪器检出限为 0.1 μmol/L。
2 结果与讨论
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2.1 组合工艺对ARGs的去除效能
2.1.1 最佳O3投加量的确定
O3投加量影响着组合工艺对二级出水中ARGs的去除效果。试验过程中,改变氧化剂O3的剂量为1.0、2.0、3.0、4.0 mg/L,预氧化20 min后的水样分别投加20 mg/L PAC并恒温振荡24 h,对吸附后水中的不同种类 ARGs、intⅠ1和16S rRNA体积浓度进行检测,结果如图2所示。
由图2可知,随着O3投加量的增加,各类ARGs和intI1出水浓度呈现先降低后增加的趋势。当O3投加量为2.0 mg/L时,处理后水中5种ARGs和intI1基因检出含量最低,此时水中tetA、tetC、tetG、sulI、sulII和intI1的丰度分别为102.92 、104.27 、103.40 、104.45 、104.01 、106.04 copies/mL,因此确定最佳O3投加量为2.0 mg/L。这是因为,O3具有很强的氧化性,能够与细胞结构迅速发生反应,同时O3极易被二级出水中的溶解性有机物消耗,导致O3对ARGs的去除效果并不会随投加量增加而提高[19]。
2.1.2 组合工艺对ARGs的去除效果
试验过程中,在最佳O3投加量(2.0 mg/L)下比较PAC-UF和O3-PAC-UF两种工艺对二级出水中ARGs削减情况,分别对二级出水、不同组合工艺的膜进水和膜出水中不同种类ARGs、intIl 和16S rRNA体积浓度进行检测,结果如图3所示。
由图3可知,二级出水中仍含有浓度较高的ARGs, 这说明污水处理厂无法完全去除水中ARGs;其中,sul基因浓度要高于tet基因,这可能与sul基因更易通过intⅠ1和质粒发生水平转移有关[19]。另一方面,PAC-UF、O3-PAC-UF两种工艺对原水中ARGs、intⅠ1和16S rRNA均有去除效果;PAC-UF与O3-PAC-UF工艺对抗性基因tetA、tetC、tetG、sulⅠ、sulⅡ、intⅠ1和16S rRNA的去除量范围分别为101.55 ~ 102.12 copies/mL和102.67 ~ 103.92 copies/mL, O3-PAC-UF组合工艺相较于PAC-UF工艺可以更加有效地削减二级出水中的ARGs,说明氧化剂的预氧化起了重要作用。这是因为,预氧化可以破坏细胞结构,导致携有大量ARGs的游离DNA释放到水样中[20],而水样中的PAC可继续吸附这部分游离态ARGs,最终通过UF膜截留达到去除之效。
2.1.3 不同形态ARGs的去除效果
细胞态和游离态是污水厂二级出水中的ARGs的两种存在形态。其中,游离态ARGs具有持久性和低衰减的特性,更容易造成环境中ARGs的扩散[21]。不同处理工艺对二级出水中不同形态ARGs的去除效果如图4所示。
由图4可知,污水厂二级出水中细胞态tetA、tetC、tetG、sulⅠ、sulⅡ的浓度范围为104.82 ~ 106.30 copies/mL,游离态tetA、tetC、tetG、sulⅠ、sulⅡ的浓度范围为104.70 ~ 106.05 copies/mL,表明原水中游离态ARGs浓度高于细胞态ARGs浓度,与文献[22]的研究结果一致[22]。这是因为污水厂中细胞态 ARGs广泛存在于活性污泥中,随着宿主细菌的代谢死亡,部分细胞态ARGs会转变成游离态ARGs,使其浓度增高。另一方面,细胞态ARGs分子较大,可利用活性污泥进行吸附沉淀,而游离态ARGs不易在二沉池中沉淀,最终导致污水厂二级出水中游离态 ARGs 浓度较高。
直接UF对二级出水中各细胞态ARGs的去除量为100.81 ~ 100.93 copies/mL,去除率达85.9%,而对各游离态ARGs去除量仅为100.33 ~ 100.40 copies/mL。这是由于细胞态ARGs粒径尺寸较大,大部分可以被UF膜截留,而游离态ARGs尺寸小且为柔性分子,可以在高速水流中伸长,能够挤压通过比其小得多的膜孔[23];PAC-UF组合工艺对细胞态和游离态ARGs的去除量分别为102.89 ~ 103.76 copies/mL和101.78 ~ 101.91 copies/mL,比直接UF去除量要多。这是因为,水样中分子量较大的细胞态 ARGs可被超滤膜直接截留,而分子量较小的的细胞态ARGs和游离态ARGs可以被水中 PAC吸附,最终通过UF膜的截留作用得以去除;O3-PAC-UF组合工艺处理后细胞态ARGs未检出,说明几乎实现了完全去除,对各游离态ARGs去除量为102.87 ~ 103.05 copies/mL。可以看出,较于PAC-UF组合工艺,O3-PAC-UF组合工艺对游离态ARGs的去除量也得到了提升,因此,预氧化-PAC-UF组合实现了对二级出水中细胞态和游离态ARGs的高效去除。
2.2 组合工艺去除ARGs的影响因素
文献[24]表明,O3的氧化能力很大程度上受水样pH和温度的影响。pH可以影响O3在水样中分解生成OH·的能力,而温度则是O3在水中溶解度的重要影响条件。因此,试验过程中改变二级出水的pH和温度,评价O3-PAC-UF组合工艺(投加O3最佳量2.0 mg/L,预氧化20min后投加20 mg/L的PAC,恒温振荡24 h。随后进行超滤试验,以死端模式进行,恒定压力100 kPa)对水中不同种类ARGs的去除效能。
2.2.1 pH的影响
向二级出水中投加盐酸或氢氧化钠来调节原水的pH分别为4、7、10,在不同pH下,O3-PAC-UF工艺膜出水中不同ARGs 体积浓度变化如图5所示。
由图5可知,O3-PAC-UF组合工艺对ARGs的削减效果随pH升高而增强。当水样pH=4时,组合工艺膜出水中tetA、tetC、tetG、sulI、sulII 浓度分别为 102.27、103.32、 102.76、 103.78、103.45 copies/mL;而当pH=10时,上述ARGs浓度分别降至101.67、102.54、101.95、103.02、102.65 copies/mL。这是由于,O3在水中的分解速度会随pH升高而加快,pH每提高一个单位,可使臭氧分解的促进剂OH-更快速地分解产生OH·[25]。此外,OH·具有非常强的氧化性,可以无选择地氧化水中污染物,使ARGs彻底氧化分解[26]。尽管有研究表明[27],PAC在酸性条件下吸附速率较高,但从整体结果来看,pH 越高越有利于组合工艺对水中 ARGs 的去除。
2.2.2 温度的影响
试验过程中,采用水浴方式调节水样温度分别为15、25、35 ℃。探究在不同温度下,O3-PAC-UF工艺膜出水中各ARGs体积浓度变化如图6所示。
由图6可知,O3-PAC-UF组合工艺对ARGs的去除效果随水样温度的升高而降低。当水样温度为15 ℃时,组合工艺膜出水中tetA、tetC、tetG、sulI、sulII 浓度分别为101.53、102.57、101.86、102.99、102.67 copies/mL;而当水样温度上升至35 ℃时,组合工艺膜出水中上述ARGs 浓度分别增大为102.88、103.84、103.19、104.29、103.94 copies/mL。这是因为当水温为15 ℃时,O3在水中溶解度为68%,当水温升至35℃时,O3溶解度仅为20%,导致O3对ARGs氧化去除能力大幅下降[28]。尽管有研究表明,温度升高后污染物在水中和炭孔内的热运动更加剧烈,有利于PAC吸附ARGs[27]。但整体结果来看,温度升高对臭氧的氧化过程产生了严重影响,不利于组合工艺对ARGs的去除。
2.3 组合工艺去除ARGs的机理研究
2.3.1 预氧化过程中氧化剂O3分解产生的自由基浓度
OH·是氧化反应中最主要的活性自由基,OH·和有机物反应的二级速率常数很高,通常可以达到109 mol/(L·s),从而无选择的去除水中各类有机污染物[29]。试验过程中,分别投加O3最佳剂量(2.0 mg/L)与苯甲酸溶液(BA,50 mg/L),反应时间30 min,再使用高效凝胶液相色谱对反应后水中的羟基苯甲酸(p-HBA)含量进行检测。由于p-HBA是OH·与BA反应生成的稳定产物,故OH·浓度可通过测定p-HBA来定量,根据p-HBA浓度的5.87倍计算出累积的OH·浓度[30]。
试验共生成了0.987 6 mg/L的p-HBA,其摩尔质量为138.12 g/mol,折合后即O3分子在氧化过程中产生了0.041 9 mmol/L OH·。但OH·去除ARGs的作用机理仅凭此试验并不明晰,需要进一步研究。
2.3.2 自由基在预氧化去除ARGs中的作用
为确定 O3预氧化过程中生成的OH·对ARGs去除效能的影响,本试验采用叔丁醇(TBA)作为自由基抑制剂。TBA与OH·的反应速率很快,可用作OH·的捕获剂[31]。试验中,O3采用最佳投加量(2.0 mg/L),向臭氧预氧化体系中加入过量的TBA(OH·∶TBA=1∶50)来验证 OH·对ARGs的重要作用,TBA抑制前后预氧化出水中ARGs浓度变化如图7所示。
由图7可知,单独O3处理后水中tetA、tetC、tetG、sulI、sulII浓度分别为104.32、 105.39、104.66、105.80、105.47 copies/mL;而投加TBA后,水中tetA、tetC、tetG、sulI、sulII 浓度稍有增加,分别为104.57、105.60、104.82、105.94、105.65 copies/mL。通常认为,O3体系可以通过两种机制氧化去除污染物,分别是O3分子直接氧化去除和由O3分解产生的OH·间接氧化[32]。一方面,有研究表明,O3分子能够在预氧化过程中攻击双键和存在于不同种类 ARGs 中的负电子部分[33],此为O3分子直接氧化作用。另一方面,OH·可以破坏蛋白质侧链和主链,使其片段化,但是OH·通常会与大多数化合物非选择性地快速反应,即OH·会被污水中溶解性有机物迅速消耗,并且该反应速率超过了OH·与ARGs的反应速率[15],此为O3分解产生OH·的间接氧化作用。以上结果表明,在O3体系中,TBA的投加对ARGs的去除有着并不突出的抑制效果,即O3分解产生的自由基含量较少。综上,针对二级出水的ARGs去除机制,占主导地位的是O3分子的直接氧化作用。
2.3.3 组合工艺去除ARGs的机理分析
根据上述试验结果,分析O3预氧化-PAC-UF组合工艺对ARGs的去除机理,如图8所示。
由图8可知,组合工艺中的预氧化过程对二级出水中ARGs的去除中发挥了重要作用。O3对ARGs的去除属于氧化反应过程,O3分子与OH·可迅速氧化细胞膜,导致细胞成分泄漏,核酸芳香结构与蛋白质碳氮键被破坏,从而去除水中细胞态ARGs并释放部分游离DNA[34]。
在O3预氧化-PAC-UF组合工艺中,氧化剂可侵入细胞内破坏遗传物质并使细胞破裂,有效灭活水中抗生素抗性细菌(antibiotic resistant bacteria,ARB),从而有效去除水样中细胞态ARGs[35],将减缓后续细胞态ARGs对PAC吸附位点的竞争,进而促进了PAC对水中游离态ARGs的吸附作用。另当指出,采用PAC吸附工艺对二级出水进行处理时,水中的溶解性有机物会与ARGs竞争吸附位点,以降低PAC对ARGs的吸附容量[36]。而预氧化过程中的O3可氧化去除一部分溶解性有机物,间接使PAC释放更多的吸附容量,从而促进了PAC-UF对水中游离态ARGs的去除效能。因此,组合工艺通过预氧化、PAC吸附和UF膜截留等单元的相互协同作用实现了对二级出水中细胞态和游离态ARGs的高效去除。
3 结论
收起
(1)在PAC-UF工艺之前增加O3预氧化可以进一步加强对二级出水中ARGs的去除效果,在O3最佳投加量条件下(2.0 mg/L),PAC-UF与O3-PAC-UF工艺对ARGs、intⅠ1和16S rRNA的去除量范围分别为101.55 ~ 102.12 copies/mL和102.67 ~ 103.92 copies/mL。
(2)二级出水中游离态ARGs浓度高于细胞态ARGs浓度;相较于直接UF和PAC-UF工艺,O3-PAC-UF组合工艺对游离态和细胞态ARGs去除效果明显增强,对各游离态ARGs的去除量为102.87 ~ 103.05 copies/mL,而膜出水中未检测到细胞态ARGs。
(3)O3-PAC-UF组合工艺处理二级出水时,较高pH值和较低温度均利于ARGs 的去除。
(4)预氧化过程中氧化剂O3分解产生的OH·浓度为0.041 9 mmol/L;针对二级出水的ARGs去除机制,占主导地位的是O3分子的直接氧化作用。
基金
收起
  • 国家自然科学基金(52370004)
  • 国家自然科学基金(52070011)
  • 北京建筑大学研究生创新项目(PG2024085)
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doi: 10.12404/j.issn.1671-1815.2309115
  • 接收时间：2023-11-20
  • 首发时间：2025-07-29
  • 出版时间：2025-01-28
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  • 收稿日期：2023-11-20
  • 修回日期：2024-06-24
基金
国家自然科学基金(52370004)
国家自然科学基金(52070011)
北京建筑大学研究生创新项目(PG2024085)
作者信息
    1.北京建筑大学城市, 雨水系统与水环境教育部重点实验室, 北京 100044
    2.北京建筑大学环境与能源工程学院, 北京 100044
    3.北京市市政工程设计研究总院有限公司, 北京 100082
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2种不同金属材料的力学参数
科
Family		 属数
Number of
genus		 种数
Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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