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Article(id=1241116647738634391, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1241116641321350143, articleNumber=null, orderNo=null, doi=null, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1724860800000, receivedDateStr=2024-08-29, revisedDate=null, revisedDateStr=null, acceptedDate=null, acceptedDateStr=null, onlineDate=1773834867653, onlineDateStr=2026-03-18, pubDate=1742400000000, pubDateStr=2025-03-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1773834867653, onlineIssueDateStr=2026-03-18, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1773834867653, creator=13701087609, updateTime=1773834867653, updator=13701087609, issue=Issue{id=1241116641321350143, tenantId=1146029695717560320, journalId=1234093305789726721, year='2025', volume='45', issue='3', pageStart='1185', pageEnd='1776', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1773834866123, creator=13701087609, updateTime=1773881366030, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1241311676130193619, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1241116641321350143, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1241311676130193620, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1241116641321350143, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=1290, endPage=1297, ext={EN=ArticleExt(id=1241116653044429195, articleId=1241116647738634391, tenantId=1146029695717560320, journalId=1234093305789726721, language=EN, title=Enhanced coagulation mechanism of fine bubbles in response to calcium ion concentration, columnId=1234106386360103680, journalTitle=China Environmental Science, columnName=Water Pollution Control, runingTitle=null, highlight=null, articleAbstract=

In order to further supplement the mechanism of the enhanced coagulation efficiency of the fine bubble co-coagulation process and the potential of the process for engineering applications, this paper investigated the effect of calcium ion concentration response on the enhanced removal of humic acid（HA）by the fine bubble co-coagulation process. The results showed that the fine bubbles could enhance the removal of HA with different calcium ion concentration responses, but the enhancement effect was different with different circulation times. When the cycle time of fine bubbles was kept constant at 1min, the participation of fine bubbles in the coagulation process could enhance the removal efficiency of HA by forcing the hydrolysis of polyaluminum chloride（PACl）, elevating the potential of the solution to the isoelectric potential, and promoting the complexation between HA and Ca2+, and the removal efficiency of HA increased with the increase of Ca2+ concentration, and the removal efficiency of HA increased about 42% with the increase of Ca2+ concentration, and increased about 42% with the increase of Ca2+ concentration, and increased about 42% with the increase of Ca2+ concentration. The HA removal efficiency increased with increasing Ca2+ concentration, up to about 42% compared to the conventional coagulation process without the presence of fine bubbles. In addition, with the extension of the fine bubbles circulation time, the Zeta potential of the solution gradually increased, which affected the enhanced removal efficiency of HA. The above findings provide data and theoretical support for the application of the fine bubble co-coagulation process in engineering practice.

, correspAuthors=Jin-suo LU, authorNote=null, correspAuthorsNote=null, copyrightStatement=null, copyrightOwner=null, extLink=null, articleAbsUrl=null, sourceXml=null, magXml=null, pdfUrl=null, pdf=null, pdfFileSize=null, pdfExtLink=null, richHtmlUrl=null, mobilePdfUrl=null, reviewReport=null, pdfFirstPage=null, abstractGraph=null, abstractGraphContent=null, abstractVideo=null, citation=null, cebUrl=null, magXmlContent=null, mapNumber=null, authorCompany=null, fund=null, authors=null, authorsList=Chun-bo LI, Xiao-jiang HUANG, Ping LI, Zi-ang ZHAO, Zhi-qiang ZHANG, Jin-suo LU), CN=ArticleExt(id=1241116656131437190, articleId=1241116647738634391, tenantId=1146029695717560320, journalId=1234093305789726721, language=CN, title=钙离子浓度响应下的微细气泡强化混凝机制, columnId=1234106386565624579, journalTitle=中国环境科学, columnName=水污染与控制, runingTitle=null, highlight=null, articleAbstract=

为进一步补充微细气泡共混凝工艺强化混凝效能机制及该工艺的工程应用潜力，本文探究了钙离子(Ca2+)浓度响应对微细气泡共混凝工艺强化去除腐殖酸(HA)的影响.研究结果表明，不同钙离子浓度响应下的微细气泡可以强化HA的去除效果，但不同循环时间下强化效果有所不同.当微细气泡循环时间恒定为1min时，混凝过程中微细气泡的参与可以通过强制聚合氯化铝(PACl)水解，提升溶液电位至等电点位以及促进HA与Ca2+之间的络合作用来强化HA的去除效能，且HA的去除效能随着Ca2+浓度升高而升高，最高可相较于没有微细气泡存在时的常规混凝工艺提升约42%.此外，随着微细气泡循环时间的延长，溶液Zeta电位逐渐提升，影响了HA的强化去除效能.上述研究结论为微细气泡强化混凝工艺应用于工程实践提供了数据支持与理论支撑.

, correspAuthors=卢金锁, authorNote=null, correspAuthorsNote=
* 责任作者，教授，
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李春波(2000-)，男，河南登封人，西安建筑科技大学环境与市政工程学院硕士研究生，研究方向为饮用水品质提升与水质保障..

, authorsList=李春波, 黄晓江, 李萍, 赵子昂, 张志强, 卢金锁)}, authors=[Author(id=1241116658392167166, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116647738634391, orderNo=0, firstName=null, middleName=null, lastName=null, nameCn=null, orcid=null, stid=null, country=null, authorPic=null, dead=0, email=lcbyjya@163.com, emailSecond=null, emailThird=null, correspondingAuthor=0, authorType=1, ext={EN=AuthorExt(id=1241116658543162130, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116647738634391, authorId=1241116658392167166, language=EN, stringName=Chun-bo LI, firstName=Chun-bo, middleName=null, lastName=LI, prefix=null, suffix=null, authorComment=null, nameInitials=null, affiliation=null, department=null, xref=1, address=1.Shaanxi Key Laboratory of Environmental Engineering, School of Environmental and Municipal Engineering, Xi’an University of Architecture and Technology, Xi’an 710055, China, bio=null, bioImg=null, bioContent=null, aboutCorrespAuthor=null), CN=AuthorExt(id=1241116658710934300, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116647738634391, authorId=1241116658392167166, language=CN, stringName=李春波, firstName=null, middleName=null, lastName=null, prefix=null, suffix=null, authorComment=null, nameInitials=null, affiliation=null, department=null, xref=1, address=1.西安建筑科技大学环境与市政工程学院，陕西省环境工程重点实验室，陕西 西安 710055, bio={"content":"

李春波(2000-)，男，河南登封人，西安建筑科技大学环境与市政工程学院硕士研究生，研究方向为饮用水品质提升与水质保障..

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李春波(2000-)，男，河南登封人，西安建筑科技大学环境与市政工程学院硕士研究生，研究方向为饮用水品质提升与水质保障..

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figureFileSmall=GBFdszblqd9iSalxTIjYDA==, figureFileBig=OILGXL5dbTRJOCFlYtc47g==, tableContent=null), ArticleFig(id=1241116664692011321, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116647738634391, language=CN, label=图6, caption=钙离子响应下的微细气泡对HA颗粒粒径的影响以及强化混凝机制, figureFileSmall=GBFdszblqd9iSalxTIjYDA==, figureFileBig=OILGXL5dbTRJOCFlYtc47g==, tableContent=null), ArticleFig(id=1241116664851394886, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116647738634391, language=EN, label=Table 1, caption=

Characteristics of aluminum morphology distribution in PACl with alkalinity of 2.0

, figureFileSmall=null, figureFileBig=null, tableContent=
碱化度B = 2.0Ala (%)Alb (%)Alc (%)
22.2±0.259.5±1.018.3±0.7
), ArticleFig(id=1241116665031749978, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241116647738634391, language=CN, label=表1, caption=

碱化度为2.0的PACl中铝形态分布特性

, figureFileSmall=null, figureFileBig=null, tableContent=
碱化度B = 2.0Ala (%)Alb (%)Alc (%)
22.2±0.259.5±1.018.3±0.7
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钙离子浓度响应下的微细气泡强化混凝机制
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李春波 1 , 黄晓江 1 , 李萍 1 , 赵子昂 3 , 张志强 1, 2 , 卢金锁 1, 2, *
中国环境科学 | 水污染与控制 2025,45(3): 1290-1297
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中国环境科学 | 水污染与控制 2025, 45(3): 1290-1297
钙离子浓度响应下的微细气泡强化混凝机制
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李春波1 , 黄晓江1, 李萍1, 赵子昂3, 张志强1, 2, 卢金锁1, 2, *
作者信息
  • 1.西安建筑科技大学环境与市政工程学院，陕西省环境工程重点实验室，陕西 西安 710055
  • 2.西安建筑科技大学，绿色建筑全国重点实验室，陕西 西安 710055
  • 3.浙江天和建筑设计有限公司，浙江 湖州 313000

    • 李春波(2000-)，男，河南登封人，西安建筑科技大学环境与市政工程学院硕士研究生，研究方向为饮用水品质提升与水质保障..

通讯作者:

* 责任作者，教授，
Enhanced coagulation mechanism of fine bubbles in response to calcium ion concentration
Chun-bo LI1 , Xiao-jiang HUANG1, Ping LI1, Zi-ang ZHAO3, Zhi-qiang ZHANG1, 2, Jin-suo LU1, 2, *
Affiliations
  • 1.Shaanxi Key Laboratory of Environmental Engineering, School of Environmental and Municipal Engineering, Xi’an University of Architecture and Technology, Xi’an 710055, China
  • 2.National Key Laboratory of Green Building, Xi’an University of Architecture and Technology, Xi’an 710055, China
  • 3.Zhejiang Tianhe Architectural Design Co., Ltd, Huzhou 313000, China
出版时间: 2025-03-20
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摘要
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为进一步补充微细气泡共混凝工艺强化混凝效能机制及该工艺的工程应用潜力，本文探究了钙离子(Ca2+)浓度响应对微细气泡共混凝工艺强化去除腐殖酸(HA)的影响.研究结果表明，不同钙离子浓度响应下的微细气泡可以强化HA的去除效果，但不同循环时间下强化效果有所不同.当微细气泡循环时间恒定为1min时，混凝过程中微细气泡的参与可以通过强制聚合氯化铝(PACl)水解，提升溶液电位至等电点位以及促进HA与Ca2+之间的络合作用来强化HA的去除效能，且HA的去除效能随着Ca2+浓度升高而升高，最高可相较于没有微细气泡存在时的常规混凝工艺提升约42%.此外，随着微细气泡循环时间的延长，溶液Zeta电位逐渐提升，影响了HA的强化去除效能.上述研究结论为微细气泡强化混凝工艺应用于工程实践提供了数据支持与理论支撑.

微细气泡  /  混凝效能  /  铝形态  /  络合作用  /  饮用水处理

In order to further supplement the mechanism of the enhanced coagulation efficiency of the fine bubble co-coagulation process and the potential of the process for engineering applications, this paper investigated the effect of calcium ion concentration response on the enhanced removal of humic acid（HA）by the fine bubble co-coagulation process. The results showed that the fine bubbles could enhance the removal of HA with different calcium ion concentration responses, but the enhancement effect was different with different circulation times. When the cycle time of fine bubbles was kept constant at 1min, the participation of fine bubbles in the coagulation process could enhance the removal efficiency of HA by forcing the hydrolysis of polyaluminum chloride（PACl）, elevating the potential of the solution to the isoelectric potential, and promoting the complexation between HA and Ca2+, and the removal efficiency of HA increased with the increase of Ca2+ concentration, and the removal efficiency of HA increased about 42% with the increase of Ca2+ concentration, and increased about 42% with the increase of Ca2+ concentration, and increased about 42% with the increase of Ca2+ concentration. The HA removal efficiency increased with increasing Ca2+ concentration, up to about 42% compared to the conventional coagulation process without the presence of fine bubbles. In addition, with the extension of the fine bubbles circulation time, the Zeta potential of the solution gradually increased, which affected the enhanced removal efficiency of HA. The above findings provide data and theoretical support for the application of the fine bubble co-coagulation process in engineering practice.

fine bubbles  /  coagulation efficiency  /  aluminum species  /  complex interaction  /  drinking water treatment
李春波, 黄晓江, 李萍, 赵子昂, 张志强, 卢金锁. 钙离子浓度响应下的微细气泡强化混凝机制. 中国环境科学, 2025 , 45 (3) : 1290 -1297 .
Chun-bo LI, Xiao-jiang HUANG, Ping LI, Zi-ang ZHAO, Zhi-qiang ZHANG, Jin-suo LU. Enhanced coagulation mechanism of fine bubbles in response to calcium ion concentration[J]. China Environmental Science, 2025 , 45 (3) : 1290 -1297 .
正文
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混凝基于电性中和、吸附架桥以及网捕卷扫等多种作用机制实现对以天然有机物(NOM)为主的有机污染物的去除[1-2]，是饮用水处理工艺流程中不可或缺的一部分，是关乎饮用水安全的第一道防线.对于常规金属盐混凝剂而言，其混凝效能依赖于金属盐混凝剂中优势物种的占比[3-4].如具有高正电荷的聚合物混凝形态和丰富比表面积的胶体形态的聚合氯化铝(PACl)而言，大部分高分子NOM可以通过单体Al或是低聚态Al(Ala)所发挥的电性中和作用去除[5]，而相较之下难以有效去除的低分子NOM则需依靠中等聚合态Al(Alb)和高等聚合态Al(Alc)所发挥的吸附架桥与网捕卷扫作用[6-7].因此对于使用PACl为混凝剂的常规混凝工艺而言，采用合适的技术手段来强制PACl水解以提高中高聚合态Al物种占比有益于提高低分子NOM的去除[8-9]，对保障饮用水安全具有重要意义.
现有的强制水解技术主要是通过向溶液中添加碱性试剂(如NaOH)[10]，使溶液pH值分布不均，进而促进了需要较高pH值的八面体配位铝向四面体配位铝的转化以及促进了铝原子之间羟基桥连的发生[11].为推动国家“十四五”期间的减污降碳协同增效战略，减少化学药剂在饮用水处理过程中的投加，现有研究利用微细气泡通过表面吸附溶液中氢氧根离子(OH-)而形成的碱性微界面的特性[12]，使微观界面存在两侧差异较大的pH值环境，以此驱动PACl的强制水解[13-15].微细气泡强制PACl水解过程中，碱性微界面的形成有益于四面体配位铝(Al(OH)4-)的产生，而酸性微界面的形成则有助于二聚体和三聚体的形成.这一过程推动了以Al(OH)4-为核心，二聚体和三聚体为前驱体的优势中等聚合态(Alb)中Keggin-Al13的形成，亦或是推动了优势高等聚合态(Alc)中Al30的形成.
Ca2+是天然水体中最常见的硬度离子，其在混凝去除NOM的过程中起着重要作用[16-17]. Ca2+作为金属离子所发挥的中和NOM负电荷的作用以及与NOM表面官能团所产生的络合作用能够有效缓解NOM浓度过高时对PACl水解的抑制作用[18-19]，进而促进混凝过程中对NOM的去除[20-21].微细气泡共混凝工艺作为一种新工艺在面对复杂的水体环境时，势必要探究各种因素对其混凝效能的影响.因此，本研究以NOM中占比最多且分子量分布广泛的腐殖酸(HA)作为NOM的代表性污染物[22-23]，探究了不同钙离子浓度响应下，微细气泡共混凝工艺中目标污染物的强化去除效能变化，并从PACl水解物种分布、溶液Zeta电位以及络合作用角度分析了不同钙离子浓度响应下的污染物去除效能变化机制，以拓宽微细气泡共混凝工艺在水处理领域的应用方向.
1　材料与方法
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1.1　试验用水及混凝剂特性
本研究所使用的包括AlCl3·6H2O、Na2CO3，HCl、CaCl2、NaAc、C12H8N2、HCl、NaOH以及高岭土均为分析纯，购买自国药集团化学试剂有限公司.所用的Ferron试剂(C9H6INO4S)购自麦克林，腐殖酸(HA)购自Sigma-Aldrich(53680，美国).
1.1.1　实验用水特性
将1g HA溶于1L 0.1mol/L的NaOH溶液中，搅拌6h获得HA储备液.为了去除HA储备液中不可溶解的杂质，用0.45µm滤膜过滤HA储备液.之后移取10mL HA储备液于1L去离子水中使实验用水中的HA浓度达到10mg/L(DOC浓度为(6.06±0.18)mg/L)，并在实验用水中加入一定量的高岭土使实验用水浊度稳定在6NTU左右，并以CaCl2作为钙离子来源，以模拟水中钙离子的存在，其中不同分子量NOM水样(MW>100kDa和MW<100kDa)由压力驱动膜分离手段对混凝沉淀后出水筛分而来.
1.1.2　混凝剂特性
本研究以碱化度([OH-]/[Al3+])为2.0的自制PACl作为实验所用的混凝剂.根据以往的研究报道[24]，分别将22.4g的AlCl3·6H2O和9.8g的Na2CO3分别溶于一定超纯水中，在恒温水浴25℃以及磁力搅拌的作用下将溶解好的Na2CO3溶液缓慢滴加到AlCl3溶液中，并恒温搅拌6h，定容后即可得到碱化度为2.0的PACl储备液.本实验所用的PACl铝形态分布如表1所示.
1.2　微细气泡共混凝实验
与常规混凝工艺相比，微细气泡共混凝工艺(图1)最大的区别在于混凝剂投加方式的不同.与常规混凝工艺直接投加PACl相比，微细气泡共混凝工艺中的PACl投加在含有500mL去离子水的气泡罐中，通过微细气泡发生器的自循环系统将其所产生的微细气泡与PACl和Ca2+充分反应一定时间后将携带有PACl以及微细气泡的水溶液转移至混凝罐中，整个过程大约持续45s.根据以往的研究将混凝罐中的搅拌程序设置为快搅(250r/min)1min，慢搅(50r/min)10min以及沉淀10min.
1.3　分析方法
UV254采用Hitachi U-3900分光光度计检测，DOC采用Multi N/C 2100S TOC分析仪检测，粒度及Zeta电位采用Malvern Nano Zetasizer纳米粒度仪与Zeta电位仪测定，EEMs采用荧光分光光度计(F-7000)检测，红外光谱采用傅里叶变换红外光谱(Nicolet iS50)检测PACl水解形态采用Al-Ferron逐时络合比色法检测[25].
2　结果与讨论
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2.1　钙离子浓度响应下的混凝效能变化
为探明不同钙离子浓度对微细气泡共混凝工艺强化HA去除效能的影响，本研究在pH = 7以及微细气泡循环时间恒定为1min的条件下，检测了不同微细气泡发生器进气流量(Qg)以及不同钙离子浓度下混凝沉淀出水中UV254和DOC的去除效率变化.从图2(a)可以看出在没有微细气泡参与的常规混凝工艺(Qg=0mL/min)过程中，UV254的去除效率随着钙离子浓度的升高而升高.在微细气泡共混凝工艺中，钙离子的增加同样有助于UV254的去除.然而与常规混凝工艺不同的是，在相同的钙离子浓度梯度下，混凝过程中微细气泡的参与对UV254的强化去除更为显著.即当溶液中Ca2+=0.5mmol/L时，混凝沉淀后UV254可接近完全去除.
与此同时，混凝过程中钙离子浓度响应对DOC去除的影响趋势与UV254去除的影响趋势一致.如图2(b)所示，混凝过程中有无微细气泡的参与下，DOC的去除效率随钙离子浓度的升高而升高的同时，DOC的去除效率同样随着微细气泡进气流量的升高而升高.当Qg=60mL/min以及Ca2+=5mmol/L时DOC的去除效果最佳，DOC的去除效率较相同工况下的常规混凝工艺可以提升42%.以上结果表明，钙离子浓度响应下微细气泡的参与可以进一步提升混凝过程中UV254与DOC的去除效率.
2.2　不同微细气泡循环时间下的混凝效能变化
为进一步探究微细气泡共混凝工艺下钙离子对混凝效能的影响，研究了相同钙离子浓度下不同微细气泡循环时间对混凝沉淀出水中污染物去除效率的影响.如图3(a)所示，在Ca2+=0mmol/L和Qg=60mL/min的条件下DOC的去除效率在微细气泡循环1min时达到最高(DOC去除效率最高为69%)，后随微细气泡循环时间的延长DOC的去除效率出现了下降趋势.同时，无论是分子量MW>100kDa还是MW<100kDa的NOM，其浓度随循环时间的延长而提升.如图3(b)所示，当添加5mmol/L Ca2+后不同微细气泡循环时间下的DOC的去除效率呈现出相同的趋势.有所不同的是，虽然微细气泡循环时间超过1min后混凝效能有所下降，但与没有微细气泡参与的常规混凝工艺相比不同分子量NOM的去除效率均有所提升，且钙离子的投加有助于NOM的强化去除.
图3(c)表明，随着微细气泡循环时间的推进，污染物的荧光强度逐渐增强，从侧面验证了DOC的去除效率随循环时间的增加而降低.与此同时在每一个时间段添加5mmol/L Ca2+后混凝沉淀出水中的荧光强度总是低于不添加Ca2+的工况，这一实验结果与上述DOC的去除效率变化情况一致.
2.3　Ca2+浓度响应对混凝效能的影响机制
2.3.1　PACl水解形态变化
以往的研究表明，微细气泡共混凝工艺能够强化混凝效能的一个关键作用在于微细气泡表面吸附的氢氧根(OH-)能够形成碱性微界面进而具备了强制PACl水解的能力.微细气泡通过调控PACl中优势Al物种占比以此来强化混凝效能[5-6].为了探究钙离子浓度响应下微细气泡是否同样具备强制PACl水解的能力以及PACl水解形态变化与混凝效能之间是否具有一定的相关性，本研究在Qg=60mL/min以及pH=7的条件下探究了不同Ca2+浓度对PACl水解形态分布的影响.
如图4(a)、(b)和(c)所示，随着微细气泡循环时间的增加，不同Ca2+浓度投加情况下均能够强制PACl水解，且随着钙离子浓度的增加微细气泡强制PACl水解的能力也逐渐上升.随着微细气泡循环时间的增加，Ala和Alb的占比逐渐减少，在900s内可几乎将PACl中所有的单聚态Al和低聚态Al转变为多聚态Al，且当Ca2+ = 5mmol/L时PACl中Alb从原先的占比61%降低至约23%.与此同时，随着Ala和Alb占比的降低，随之而来的则是Alc占比的上升.当Ca2+ =5mmol/L时PACl中Alc从原先的占比22%上升至约78%.以上结果说明钙离子响应下微细气泡能够进一步促进PACl的强制水解，且微细气泡强制PACl水解的能力随钙离子浓度的升高而提升.
为了进一步说明微细气泡强制PACl水解与混凝效能强化去除之间的关系，研究了不同工况下PACl水解形态分布与DOC去除效率间的相关性.由图4(d)所示，在不同钙离子响应浓度及微细气泡循环1min的反应条件下，DOC的强化去除与Alc占比呈显著正相关.上述结果说明了在相同微细气泡循环时间以及不同钙离子浓度响应的条件下，混凝效能的强化与微细气泡强制PACl水解之间呈现一定的正相关.但随着微细气泡循环时间的推移，DOC的去除效率并没有随着PACl的进一步强制水解而随之提升，相反DOC的去除效率呈现出了一定程度的下降(如图4(e)和4(f)所示).虽然混凝过程中微细气泡的参与在一定程度上能够通过强制PACl水解来强化混凝效能，但微细气泡其特殊的理化特性也会影响性能.因此仅仅考虑混凝过程中微细气泡参与对PACl的水解形态分布的影响不足以合理解释钙离子浓度响应下微细气泡强化混凝效能的机制.
2.3.2　溶液Zeta电位的变化
HA为异构型多官能团聚合物，虽然不同结构和化学特征的有机物和混凝剂之间的作用各不相同，但其主要依靠电性中和作用去除[26-27].因此通过检测微细气泡参与前后溶液Zeta电位的变化为解释不同钙离子浓度响应下微细气泡强化混凝效能的相关机制有所帮助.如图5(a)所示，在pH=7、Qg=60mL/min以及微细气泡循环时间恒定为1min的条件下研究了不同钙离子浓度对混凝前溶液Zeta电位的影响.研究发现在微细气泡参与下，所有钙离子浓度下溶液的Zeta电位都得到了提升，0mmol/L钙离子对应的Zeta电位从3mV提高到9mV左右.与此同时，溶液Zeta电位随钙离子浓度的升高而升高，溶液的Zeta电位在钙离子浓度为5mmol/L时达到最高(Zeta电位由9mV提高到14mV左右).以上结果表明，在不同钙离子浓度响应下的微细气泡会促进混凝过程中的电中和作用.
图5(b)显示了恒定钙离子浓度时不同微细气泡循环时间对混凝后溶液Zeta电位的影响.实验结果表明，混凝后溶液的Zeta电位均随着微细气泡循环时间的延长而得到相应的提升，其中在溶液中添加5mmol/L钙离子时溶液的Zeta电位上升速度更快，并在微细气泡循环1min时到达混凝的等电点位.这一结果合理地解释了为何在微细气泡循环1min后混凝效率随着微细气泡循环时间的增加而逐渐降低，而不是随着PACl中优势Al物种占比的提升而升高.考虑到微细气泡可以吸附和聚集水溶液中的OH-，检测了微细气泡循环过程中溶液pH值的变化(如图5 (c)所示)，发现随循环时间的延长溶液的pH值持续下降，这可能是溶液Zeta电位升高的原因[28].
2.3.3　络合作用的影响
以往研究表明，络合作用在混凝过程中去除含有大量羧基、酚羟基和羰基的HA而言同样重要[29-30].混凝过程中带正电的金属离子可以与HA表面带负电的有机官能团相互作用，络合为更大粒径的颗粒[8].为进一步探究钙离子浓度响应下混凝过程中微细气泡参与对络合特性的影响，选择在不添加高岭土、pH=7、Qg=60mL/min以及微细气泡循环时间恒定为1min的条件下探究不同钙离子浓度对HA颗粒粒径的影响.
由图6(a)可以看出在微细气泡参与后HA粒径得到明显提升.当Ca2+=1mmol/L时，微细气泡参与前后HA颗粒的粒径由130nm提高到550nm左右，且HA颗粒的粒径随钙离子浓度的升高而升高.当Ca2+=5mmol/L时，在微细气泡的作用下HA颗粒粒径从1500nm增加至1850nm左右.以上结果说明，微细气泡能够通过促进不同浓度钙离子与HA颗粒之间的络合作用来提升混凝效果.
接着研究了恒定钙离子浓度时不同微细气泡循环时间对HA颗粒粒径的影响.如图6(b)所示，发现在0mmol/L钙离子浓度条件下，随着微细气泡循环时间的延长HA颗粒粒径变化并不明显，仅由初始的60nm变为140nm左右.这一结果虽然证明了微细气泡本身具备吸附团聚HA的能力，但该能力并不显著.当溶液中投加5mmol/L钙离子时，HA颗粒粒径随着微细气泡循环时间的延伸得到了明显的提升，HA颗粒粒径可由原先的1500nm提升至2400nm.微细气泡能够增强钙离子与HA颗粒之间的络合强度，一方面是由于微细气泡表面吸附的OH-具有较高的亲水性，它能将吸附和团聚的HA颗粒运输给水中的钙离子从而增强HA和钙离子之间的络合；另一方面是由于微细气泡能够影响羧基等官能团的含量.如图6(c)所示，在1600nm处为羧基官能团，在微细气泡循环1min时羧基官能团的提升并不明显，但在30min时可以明显看到羧基官能团的增多，因此钙离子可以与更多的羧基等官能团相结合从而提高了其与HA的络合效果.图6(d)总结了微细气泡驱动下钙离子浓度响应对混凝效能的相关影响机制，即钙离子的浓度变化可以促进微细气泡强制PACl水解，提高溶液Zeta电位以及强化钙离子与HA颗粒之间的络合作用来强化微细气泡驱动下的混凝效能.
3　结论
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3.1　Ca2+浓度响应下微细气泡共混凝工艺的强化效能随微细气泡的循环时间而变化.当微细气泡循环时间为1min时，混凝效果随Ca2+浓度的升高而升高，DOC去除率较相同工况下的常规混凝工艺可提升约42%.
3.2　随着微细气泡循环时间的推移混凝去除NOM的效果出现下降趋势，但仍大于无微细气泡参与时的常规混凝工艺，同时在每个时间段钙离子的添加也有利于混凝的去除效果.
3.3　当微细气泡循环时间为1min时，可以通过强制PACl水解，提升溶液电位至等电点位以及促进HA与Ca2+之间的络合作用来强化HA的去除.
3.4　随着微细气泡循环时间的推移，溶液Zeta电位进一步提升，逐渐偏离等电点位，不利于HA颗粒脱稳进而影响了该工艺的混凝效能.
基金
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  • 国家自然科学基金资助项目(52470014)
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2025年第45卷第3期
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  • 接收时间：2024-08-29
  • 首发时间：2026-03-18
  • 出版时间：2025-03-20
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  • 收稿日期：2024-08-29
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国家自然科学基金资助项目(52470014)
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    1.西安建筑科技大学环境与市政工程学院，陕西省环境工程重点实验室，陕西 西安 710055
    2.西安建筑科技大学，绿色建筑全国重点实验室，陕西 西安 710055
    3.浙江天和建筑设计有限公司，浙江 湖州 313000

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