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Article(id=1240689595290014633, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1240689590315569990, 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=1719763200000, receivedDateStr=2024-07-01, revisedDate=null, revisedDateStr=null, acceptedDate=null, acceptedDateStr=null, onlineDate=1773733050415, onlineDateStr=2026-03-17, pubDate=1739980800000, pubDateStr=2025-02-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1773733050415, onlineIssueDateStr=2026-03-17, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1773733050415, creator=13701087609, updateTime=1773733050415, updator=13701087609, issue=Issue{id=1240689590315569990, tenantId=1146029695717560320, journalId=1234093305789726721, year='2025', volume='45', issue='2', pageStart='593', pageEnd='1184', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1773733049228, creator=13701087609, updateTime=1773733150042, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1240690013239825123, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1240689590315569990, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1240690013239825124, tenantId=1146029695717560320, journalId=1234093305789726721, issueId=1240689590315569990, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=795, endPage=802, ext={EN=ArticleExt(id=1240689595608781759, articleId=1240689595290014633, tenantId=1146029695717560320, journalId=1234093305789726721, language=EN, title=Degradation mechanism of tetracycline in water by MoS2/PVDF porous membrane driven by water flow, columnId=1234106386360103680, journalTitle=China Environmental Science, columnName=Water Pollution Control, runingTitle=null, highlight=null, articleAbstract=

In advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS), efficient activation and utilization of PMS was considered to be an important goal for the removal of organic pollutants. The piezoelectric effect driven by water flow was introduced into PMS activation in this study, using the prepared MoS2/PVDF membrane as a piezoelectric membrane to remove tetracycline (TC) from water. The degradation efficiency of TC by MoS2/PVDF membrane was 77.9% within 60min was showed in the results, with a reaction rate constant of 0.0231min-1, which was higher than that of MoS2 (0.0135min-1) and PVDF (0.0085min-1). Sacrificial agent experiments combined with LC-MS were used to explore the intermediates of the TC degradation process and analyze the reaction mechanism. In cycling experiments, the excellent reusability and recyclability was exhibited in MoS2/PVDF membranes. These results indicated that under the mechanical vortex force of water flow, MoS2/PVDF membrane can trigger piezoelectric potential and generate abundant free electrons to activate PMS, thereby producing various active substances to degrade organic pollutants.

, correspAuthors=Yue-lu WANG, 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=Yue-lu WANG, Shi-kun HAI, Jia-jun HAN, Jin-xiao ZHANG, Yuan-meng ZHAI), CN=ArticleExt(id=1240689603095613803, articleId=1240689595290014633, tenantId=1146029695717560320, journalId=1234093305789726721, language=CN, title=水流驱动的MoS2/PVDF多孔膜降解水中四环素机理, columnId=1234106386565624579, journalTitle=中国环境科学, columnName=水污染与控制, runingTitle=null, highlight=null, articleAbstract=

以过氧单硫酸盐(PMS)为基础的高级氧化工艺(AOPs)中,高效活化和利用PMS是去除有机污染物的一个重要目标.因此,本研究将水流驱动的压电效应引入到PMS活化中,利用制备的MoS2/PVDF膜作为压电催化膜,以去除水中的四环素(TC).结果表明,在60min内,MoS2/PVDF膜对TC的降解效率为77.9%,反应速率常数为0.0231min-1,高于单独的MoS2(0.0135min-1)和PVDF(0.0085min-1).通过牺牲剂实验结合LC-MS探究TC降解过程的中间产物并分析反应机理.在循环实验中,MoS2/PVDF膜表现出优异的可重用性和可回收性.上述结果表明,在水流的机械漩涡力作用下,MoS2/PVDF膜可以触发压电电位并产生丰富的自由电子来激活PMS,从而产生各种活性物质来降解有机污染物.

, correspAuthors=王玥璐, authorNote=null, correspAuthorsNote=
*责任作者，讲师，
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王玥璐(1982-)，女，河南商丘人，讲师，硕士，主要从事化学化工.发表论文7篇. .

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王玥璐(1982-)，女，河南商丘人，讲师，硕士，主要从事化学化工.发表论文7篇. .

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王玥璐(1982-)，女，河南商丘人，讲师，硕士，主要从事化学化工.发表论文7篇. .

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水流驱动的MoS2/PVDF多孔膜降解水中四环素机理
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王玥璐 1, * , 海士坤 1 , 韩佳骏 2 , 张锦晓 2 , 翟圆梦 2
中国环境科学 | 水污染与控制 2025,45(2): 795-802
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中国环境科学 | 水污染与控制 2025, 45(2): 795-802
水流驱动的MoS2/PVDF多孔膜降解水中四环素机理
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王玥璐1, * , 海士坤1, 韩佳骏2, 张锦晓2, 翟圆梦2
作者信息
  • 1.商丘医学高等专科学校公共学科教学部，河南 商丘 476000
  • 2.河南工程学院材料工程学院，河南 郑州 450000

    • 王玥璐(1982-)，女，河南商丘人，讲师，硕士，主要从事化学化工.发表论文7篇. .

通讯作者:

*责任作者，讲师，
Degradation mechanism of tetracycline in water by MoS2/PVDF porous membrane driven by water flow
Yue-lu WANG1, * , Shi-kun HAI1, Jia-jun HAN2, Jin-xiao ZHANG2, Yuan-meng ZHAI2
Affiliations
  • 1.Department of Public Discipline Teaching, Shangqiu Medical College, Henan 476000, China
  • 2.School of Materials Engineering, Henan University of Engineering, Henan 450000, China
出版时间: 2025-02-20
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摘要
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以过氧单硫酸盐(PMS)为基础的高级氧化工艺(AOPs)中,高效活化和利用PMS是去除有机污染物的一个重要目标.因此,本研究将水流驱动的压电效应引入到PMS活化中,利用制备的MoS2/PVDF膜作为压电催化膜,以去除水中的四环素(TC).结果表明,在60min内,MoS2/PVDF膜对TC的降解效率为77.9%,反应速率常数为0.0231min-1,高于单独的MoS2(0.0135min-1)和PVDF(0.0085min-1).通过牺牲剂实验结合LC-MS探究TC降解过程的中间产物并分析反应机理.在循环实验中,MoS2/PVDF膜表现出优异的可重用性和可回收性.上述结果表明,在水流的机械漩涡力作用下,MoS2/PVDF膜可以触发压电电位并产生丰富的自由电子来激活PMS,从而产生各种活性物质来降解有机污染物.

过氧单硫酸盐  /  压电效应  /  四环素  /  聚偏二氟乙烯

In advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS), efficient activation and utilization of PMS was considered to be an important goal for the removal of organic pollutants. The piezoelectric effect driven by water flow was introduced into PMS activation in this study, using the prepared MoS2/PVDF membrane as a piezoelectric membrane to remove tetracycline (TC) from water. The degradation efficiency of TC by MoS2/PVDF membrane was 77.9% within 60min was showed in the results, with a reaction rate constant of 0.0231min-1, which was higher than that of MoS2 (0.0135min-1) and PVDF (0.0085min-1). Sacrificial agent experiments combined with LC-MS were used to explore the intermediates of the TC degradation process and analyze the reaction mechanism. In cycling experiments, the excellent reusability and recyclability was exhibited in MoS2/PVDF membranes. These results indicated that under the mechanical vortex force of water flow, MoS2/PVDF membrane can trigger piezoelectric potential and generate abundant free electrons to activate PMS, thereby producing various active substances to degrade organic pollutants.

peroxymonosulfate  /  piezoelectric effect  /  tetracycline  /  polyvinylidene difluoride
王玥璐, 海士坤, 韩佳骏, 张锦晓, 翟圆梦. 水流驱动的MoS2/PVDF多孔膜降解水中四环素机理. 中国环境科学, 2025 , 45 (2) : 795 -802 .
Yue-lu WANG, Shi-kun HAI, Jia-jun HAN, Jin-xiao ZHANG, Yuan-meng ZHAI. Degradation mechanism of tetracycline in water by MoS2/PVDF porous membrane driven by water flow[J]. China Environmental Science, 2025 , 45 (2) : 795 -802 .
正文
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基于过氧单硫酸盐（PMS）的高级氧化工艺（AOPs）引起了人们对原位化学氧化法修复污染废水的极大兴趣[1-2].具有不对称结构的PMS（HO-O-SO3−）需要通过能量输入或电子转移断裂O-O键，从而产生强氧化性的活性氧物种（ROS）来去除水中的有机污染物[3-5].金属离子、紫外线（UV）、加热或超声（US）等各种策略已被应用于分解和有效活化PMS[6-8].然而，过渡金属的引入可能产生二次污染，UV、加热或US所产生的高能耗极大限制了它们在废水处理中的应用[9].因此，寻找一种环保、简单而有效的PMS活化方法来提高PMS的利用效率是当务之急.
压电效应作为一种将机械振动转化为电能的物理现象受到人们的广泛关注[10].这一过程中外部机械力通过诱导压电材料的变形和极化，形成驱动自由电子转移和迁移的压电电位[11].压电效应已被应用于消除污染物和激活PMS[12].虽然压电催化已被证明是一种具有良好催化性能的方法，但颗粒形态催化剂稳定性低、回收难、颗粒团聚等问题严重限制了其实际应用.聚偏氟乙烯是一种典型的压电聚合物.其良好的柔韧性、耐化学性和生物相容性使其成为自功率传感器和能量收集器的理想压电材料[13].PVDF的压电性能与其β晶相的含量有关[14].Singh等[15]和Ma等[16]分别利用溶剂铸造法和静电纺丝技术制备了β相Ag/LN-PVDF复合膜和β相MoS2/PVDF压电催化活性膜，对四环素和土环素的去除率分别达到69%和93.08%.然而，这些应用大多需要来自频率较高的超声波振动的外部能量来触发压电材料的变形，造成了高能量消耗.最近，Liu等[17]利用低频流体力学实现高效的压电催化消毒.因此，具有低频能量的水流机械能诱导压电效应有效激活PMS具有重要的现实意义.
为了有效利用低频机械能实现PMS的压电活化，本文以多层MoS2作为催化剂，以PVDF作为压电基底，通过溶剂交换法合成了MoS2/PVDF压电催化材料.以水体中的四环素（TC）作为目标有机污染物，利用低频搅拌水体形成的机械涡旋力作为机械能源.水机械涡旋力可以激发PVDF的压电响应，在复合膜表面产生丰富的自由电荷进行PMS活化，最终产生ROS，降解水中的有机污染物.系统地研究了水涡驱动的PVDF压电活化PMS的压电活化降解过程及其应用潜力.为利用水流机械涡流活化PMS去除水中有机污染物提供了新的策略.
1　实验部分
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1.1　试剂与仪器
聚偏二氟乙烯（PVDF）、N，N-二甲基甲酰胺（DMF）、聚乙烯吡咯烷酮（PVP）、乙醇（EtOH），天津市大茂化学试剂厂；四水钼酸铵（（NH4）6Mo7O24•4H2O），纯度99.9%）、硫脲（CH4N2S，纯度99.0%）、甘油（C3H8O3）、四环素（TC）、过氧单硫酸盐（PMS），上海麦克林生化科技股份有限公司；叔丁醇（TBA）、糠醇（FFA）、对苯醌（PBQ），上海麦克林生化科技股份有限公司.所有试剂均为分析纯，无需进一步处理，可直接使用.
1.2　实验过程
MoS2的制备：采用水热合成法制备MoS2.首先，分别称取0.1mmol（NH4）6Mo7O24•4H2O和3mmol CH4N2S，将（NH4）6Mo7O24•4H2O和CH4N2S溶解在35mL去离子水中.将配好的的溶液转移至反应釜中，设置烘箱温度180℃，保温时间24h，待反应结束后取出.用去离子水和乙醇反复清洗，在80℃下干燥6h，即得到MoS2.
MoS2/PVDF的制备：采用溶剂铸造法制备了MoS2/PVDF膜.将得到的MoS2溶解在16mL DMF中，在60℃下依次加入0.1mmol PVP和3mmol PVDF，搅拌4h后形成均匀的铸造液.随后超声3h以彻底消除内部气泡.通过间隙厚度为300µm的铸刀将铸造液均匀流延到玻璃板上，并立即浸入充满去离子水和甘油（体积比2：1）的凝固浴中.将原始膜在凝固浴中储存8h，以确保完全去除膜中的残留溶剂，在空气中干燥后将得到聚合物膜命名为MoS2/PVDF.
1.3　测试与表征
通过X射线衍射法（XRD）表征膜的晶体结构；扫描电子显微镜（SEM）和高分辨率透射电子显微镜（HRTEM）用于观察样品的形态；使用X射线光电子能谱（XPS）分析样品中不同元素的类型和价态；使用紫外分光光度计（UV-Vis）测定了TC的紫外可见吸收光谱.
压电催化去除TC：对MoS2/PVDF复合膜的压电催化性能进行了评价.将MoS2/PVDF膜裁剪为3×3cm2，配置pH=7，TC=10mg/L的初始反应溶液，将复合膜至于反应溶液内进行60min的吸附.待吸附结束后，将反应溶液施加磁力搅拌以引起水的流动触发复合膜的压电效应，将PMS（0.5mmol/L）加入到TC溶液中以引发反应.反应溶液按一定的时间间隔提取，加入100mmol/L的EtOH对压电催化反应进行猝灭，淬灭剂与反应液大致体积比为1：170.所有的实验都是重复进行的，在本研究中给出了平均值.对于连续9次循环的降解实验，反应结束后，膜只用去离子水冲洗，然后在下一个循环中使用.研究了选择性自由基捕获试验，以探索参与TC降解过程的主要活性氧.其中，叔丁醇（TBA）作为•OH的牺牲剂，乙醇（EtOH）作为•OH和SO4•−的牺牲剂，对苯醌（PBQ）作为O2•−的牺牲剂，糠醇（FFA）作为1O2的牺牲剂.通过UV-Vis测定了TC在357nm最大吸收波长处的吸光度，催化降解效率通过浓度与吸光度之间的方程式（1）计算获得：
式中：C0和Ct分别表示在初始时刻和t时刻的溶液浓度；A0和At分别表示在初始时刻和t时刻的吸光度数值.
电流响应测试：压电增强光电流分析由CS电化学工作站在三电极设置下进行.在一个典型的三电极石英电池，采用Ag/AgCl电极和Pt网电极分别作为参比电极和对电极，被催化膜覆盖的ITO玻璃作为工作电极.其中，工作电极的制备过程为：利用导电胶将催化膜固定到ITO玻璃上，在0.1mol/L磷酸盐缓冲溶液中浸泡5h，待体系稳定后在室温下进行表征测试，以10mV/s的扫描速率将电位向正方向扫描.
2　结果与讨论
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2.1　催化剂的表征分析
2.1.1　MoS2和MoS2/PVDF的形貌分析
由图1（a）可以清楚地观察到属于MoS2的纳米级花状结构，0.62nm的晶格间距对应于MoS2的（002）晶面（图1（b））.如图1（c），（d）所示，原始PVDF膜显示出均匀光滑的表面和横截面.将MoS2引入到PVDF后，在MoS2/PVDF膜表面形成了大量的孔隙，横截面显示出均匀的大孔结构（图1（e），（f））.MoS2/ PVDF膜孔隙率的提高与合成过程中的瞬态相变有关，MoS2的加入同时提高了溶剂相和非溶剂相的交换速率，这种互渗速率导致膜中形成孔洞[18].这种独特的孔洞结构有利于污染物进入孔内部，被快速催化降解.此外，MoS2/PVDF复合膜是由O，F，S，C，N，Mo六种元素组成的（图1（g）~（l））.
2.1.2　XRD分析
图2为MoS2、PVDF以及MoS2/PVDF的XRD图谱.对于MoS2/PVDF膜，在2θ=13.8°处观察到宽的衍射峰，对应于MoS2的（002）晶面，表明MoS2成功掺杂在PVDF中.在2θ=20.24°和36.25°处观察到PVDF的不稳定β相，分别指向（110/200）和（101）晶面，这是MoS2/PVDF膜具有压电性的主要原因.除了存在的β相，PVDF中带正电的–CH2–偶极将与带负电的MoS2形成静电相互作用[19]，产生更多的电偶极子[20].XRD的结果证明了MoS2/PVDF膜的成功制备.
2.1.3　XPS分析
利用X射线光电子能谱（XPS）分析进一步验证了MoS2/PVDF膜中元素的化学组成和状态.宽测量光谱如图3（a）所示，证实了膜表面存在的主要元素是F、O、N、C、Mo和S元素.在O 1s光谱中（图3（b）），可以拟合为531.6eV，530.87eV和529.87eV 3个主峰，分别对应于OH、C=O和S=O.
在图3（c）中的Mo 3d光谱中，结合能位于228.27和231.47eV处的峰依次归属于MoS3中Mo4+.在229.17和232.57eV处的峰归属于Mo5+，位于236.17eV的小峰归属于Mo6+.此外，位于225.47eV处的峰归属于S 2s轨道.对于S 2p光谱（图3（d）），167.76eV的结合能属于SO42-，162.88和161.87eV处的两个峰属于不饱和bridge S22-或apical S2-，161.48和160.87eV处的两个峰被归属于terminal S22-.图3（e）显示了C 1s的光谱，286.27和290.67eV处的峰分别属于PVDF的CH2和CF2，284.8和287.77eV处的峰分别对应于C—C（C=C）和O—C=O.对于N 1s光谱（图3（f）），399.7、398.6和397.7eV处的峰分别对应于Graphitic-N、Pyridinic-N和Pyrrole N.
2.2　TC降解效果的影响因素分析
2.2.1　不同体系的分析
以降解TC为目标污染物，研究了MoS2/PVDF膜的压电催化降解性能.采用搅拌的方法驱动水体涡流产生，从而触发压电响应.为了确保吸附平衡，在压电光降解反应前进行了60min的暗吸附研究.如图4（a）所示，在60min内，MoS2/PVDF+PMS+压电体系对TC的去除率为77.9%，高于单一的压电（50.8%）或PMS（67.7%）体系.这是由于涡流驱动的压电介质促进了PMS、TC和多孔膜之间的传质.相比之下，由于TC的自降解能力十分有限，在没有任何催化剂的情况下，TC的自降解率为8.1%.降解结果符合一级动力学模型，如图4（b）所示.在所有样品中，MoS2/PVDF+PMS+压电体系对TC的压催化降解性能最高.
2.2.2　不同pH值的分析
众所周知，氧化自由基的产生和污染物的降解高度依赖于溶液pH值[21].本文研究了初始pH值对MoS2/PVDF+PMS+压电体系中TC降解的影响.如图5所示，在酸性和中性条件下，超过75.0%的TC可以被有效降解.有研究表明，MoS2的边缘S在酸性环境中会被H+解离捕获，导致Mo4+暴露[22].这种变化可以促进Mo4+与PMS的相互作用.在pH值为9时，TC的降解率略有下降，为70.9%.这是由于在碱性条件下，PMS是不稳定的，可以转化为SO52−，而OH−则会清除具有较强氧化能力的SO4•−，导致氧化效率降低[23].总的来说，MoS2/PVDF+PMS+压电体系在3~9的宽pH范围内仍能保持大于70.0%的TC降解效率，说明MoS2/PVDF膜具有良好的耐酸性能.
2.3　机理分析
2.3.1　活性物种分析
为了确定MoS2/PVDF+PMS+压电体系中负责TC去除的主要反应物质，采用不含α-氢的叔丁醇（TBA）作为•OH的强牺牲剂，含α-氢的乙醇（EtOH）作为•OH和SO4•−的牺牲剂，对苯醌（PBQ）作为O2•−的牺牲剂，糠醇（FFA）作为1O2的牺牲剂进行自由基竞争实验[24].如图6（a）和6（b）所示，在MoS2/PVDF+PMS+压电体系中，当不添加牺牲剂时，处理60min后，TC去除率达到77.9%.对比地，当反应溶液中加入100mmol/L的TBA和EtOH时，TC去除率分别降至60.4%和65.1%.而在加入PBQ和FFA后，TC去除率分别降至48.1%和43.4%.也就是说，与不添加清除剂相比，分别添加TBA和EtOH时，TC去除率降低了约12%~17%，而在分别加入PBQ和FFA下，TC去除率降低了近30%.证明PBQ、FFA对TC去除率的抑制作用远大于EtOH和TBA.如图6（d）所示，利用电子顺磁共振（EPR）对MoS2/PVDF+压电系统进行ROS捕获实验，在溶液中检测到DMPO-O2•−、TEMP-1O2、DMPO-•OH和DMPO-SO4•−的EPR信号，说明MoS2/PVDF膜在压电条件下能有效激活PMS，产生能氧化降解TC的活性物质，其中，O2•−和1O2是控制氧化反应的主要活性物质.
2.3.2　电化学分析
进一步进行了电化学表征，探讨了PVDF的压电性和MoS2修饰的作用.如图7（a）所示，在光照条件下，MoS2/PVDF膜的电流强度高于MoS2和PVDF的.此外，在水流的机械应力作用下，MoS2/PVDF膜的瞬态压电电流响应强度明显增强，说明压电场的存在加速了电荷分离，从而促进了压催化过程[25]，表现出较高的压电光电流值.在电化学阻抗谱中，MoS2/PVDF+压电条件下获得了更小的阻抗.这些结果表明，作为优良的电子导体，MoS2可以通过肖特基结加速压电诱导的电子转移.因此，MoS2/PVDF膜的压催化效果将得到改善.
2.3.3　降解路径分析
采用高效液相色谱-质谱法检测了MoS2/PVDF膜压电降解TC过程中的中间产物.HPLC-MS分析结果表明，TC主要通过去甲基化、羟基化、脱胺和开环降解，并提出3种可能的降解路径.路径一：TC经过羟基化、氧化和加成聚合，被1O2强制降解形成P1（m/z=478），随后脱烷基生成P2（m/z=417）；在1O2的强制作用下，通过去甲基化、脱酰胺化和开环反应进一步降解为P3（m/z=337）；并通过脱羟基、脱烷基和开环反应转化为P4（m/z=272）.路径二：由TC通过去甲基化和脱氨产生P5（m/z=401），P5开环形成P6（m/z=305），随后生成P7（m/z=181）.路径三：由于TC的脱酰胺作用，产生P8（m/z=405），然后由于二甲胺的脱落而转化为P9（m/z=362）.由于苯环的打开和加成，羟基和乙基脱落，检测到P10（m/z=318）和P11（m/z=274）.最后，通过乙酰基脱落和氧化反应生成P12（m/z=225）[26].TC因连续遭受攻击而降解，最终矿化为无污染的CO2，H2O和其他小分子物质.
2.3.4　降解机理
基于上述讨论，提出了MoS2/PVDF膜对TC的降解机制，涉及压电催化活化PMS的过程.如图8所示，MoS2/PVDF膜在水流的压电作用下会发生机械形变，从而导致载流子有效分离分别形成e-和h+.水中的O2会与穿梭在催化膜上的e-反应形成O2•−，而h+会与水反应生成•OH.同时，PMS能够分别于e-和h+反应生成1O2和SO4•−.MoS2中的许多不饱和S原子与水溶液中的质子结合产生H2S，导致Mo4+暴露.然后，暴露的还原性位点Mo4+能够与PMS反应生成SO4•−和Mo5+/Mo6+，而Mo5+/Mo6+在PMS的辅助下会转化为Mo4+.值得注意的是，还原的S22-很可以与Mo6+或Mo5+反应产生S空位，促进Mo4+金属活性位点的再生.最终，所有的产生的活性氧物种聚集在压电通道中，在降解过程中不断攻击和氧化TC.
2.4　适用性测试
进一步评价了催化膜的可行性.对含TC的雨水和自来水进行了同样的去除实验.图10（a）显示通过MoS2/PVDF/PMS/压电体系降解后，60min内TC去除率分别为70.2%和50.4%.虽然性能不如去离子水，但这一结果证实了MoS2/PVDF/PMS/压电系统在实际废水处理中的巨大潜力.
在优化条件下测定了不同催化剂反应后溶液中溶解Mo离子的浓度（图10（b））.值得注意的是，MoS2和MoS2/PVDF反应溶液中溶解Mo离子浓度分别为8.27mg/L和2.45mg/L.结果表明，MoS2/PVDF膜可以抑制Mo的溶解，这些离子浓度很难对环境造成二次污染.同时，在MoS2/PVDF/PMS/压电系统降解过程中还测量了总有机碳（TOC）值，如图10（c）所示，60min内TOC去除率达到52.35%，证明了该系统能够快速、连续地矿化TC.图10（d）显示在经过连续9次循环后，TC去除率略有下降，这与Mo4+很难原位再生有关[27]，但MoS2/PVDF膜经过多次循环后的XPS和形貌几乎没有变化（图10（e），（f））.以上结果证明，MoS2/PVDF/PMS/压电体系在TC降解方面表现出优异的可重用性和可回收性.
3　结论
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3.1　通过溶剂交换法合成了具有独特的孔洞结构的压电催化材料MoS2/PVDF复合膜，有利于加速污染物到达催化剂内部.SEM和HRTEM证明了MoS2/PVDF复合膜的成功合成.XRD表明MoS2/PVDF中存在大量极性β相，这是MoS2/PVDF膜具有压电性的主要原因.
3.2　在MoS2/PVDF+PMS+压电体系中，TC的降解效率在60min内达到77.9%，相应的降解速率常数达到0.0229min-1.猝灭实验分析发现O2•−和1O2在降解过程中起主导作用.光电流响应证明水流压电的存在，加速了复合膜的电荷分离过程，促进了电流响应.
3.3　分析了TC在MoS2/PVDF+PMS+压电体系中的降解路径和的反应机理.此外，MoS2/PVDF膜具有优异的可回收性和可重用性.该研究为环境修复中具有出色压电催化活化PMS的催化剂设计提供了思路.因此，水流驱动法为水处理领域降低能耗、提高效率提供了方向.
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  • 科技厅科技攻关项目(222102320188)
  • 河南省高等学校重点科研项目计划(21A430008)
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2025年第45卷第2期
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  • 接收时间：2024-07-01
  • 首发时间：2026-03-17
  • 出版时间：2025-02-20
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  • 收稿日期：2024-07-01
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科技厅科技攻关项目(222102320188)
河南省高等学校重点科研项目计划(21A430008)
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    1.商丘医学高等专科学校公共学科教学部，河南 商丘 476000
    2.河南工程学院材料工程学院，河南 郑州 450000

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鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
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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
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