CN113651996B - 一种促进塑料降解的方法 - Google Patents

一种促进塑料降解的方法 Download PDF

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CN113651996B
CN113651996B CN202110785477.5A CN202110785477A CN113651996B CN 113651996 B CN113651996 B CN 113651996B CN 202110785477 A CN202110785477 A CN 202110785477A CN 113651996 B CN113651996 B CN 113651996B
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reducing bacteria
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陈姗姗
杨钰婷
李苏洁
栾天罡
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Guangdong University of Technology
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Abstract

本发明公开了一种促进塑料降解的方法，在含三价铁、铁还原菌和塑料的体系中实现塑料的降解。在含三价铁、铁还原菌和塑料的体系中，可以有效促进塑料污染的原位降解，该方法操作简单，成本低廉。

Description

一种促进塑料降解的方法
技术领域
本发明涉及环境治理领域，具体涉及一种促进塑料降解的方法。
背景技术
自然环境中的微塑料和纳米塑料尺寸微小且分布十分广泛、分散，其强吸附亲和性和迁移能力使之成为潜在的污染物载体，从而加剧了环境风险，此外，微塑料容易被水生生物摄食和陆生植物富集从而在体内积累，尤其当微塑料吸附污染物和病原体之后，毒性会随着微塑料沿食物网逐级传递，最终对人类产生威胁。微塑料体系小且分散的特点，使之难以回收和集中处理，因此原位自然降解塑料是解决该问题的有效手段之一，然而塑料在生态系统中的自然降解非常缓慢，完全降解需要数百或上千年时间。
发明内容
为了克服现有技术存在塑料在生态系统中难降解的问题，本发明的目的在于提供一种促进塑料降解的方法。
为了实现上述目的，本发明所采取的技术方案是：
一种促进塑料降解的方法，在含三价铁、铁还原菌和塑料的体系中实现塑料的降解。
优选的，这种促进塑料降解的方法，塑料的降解过程在无氧和有氧交替环境下进行；进一步优选的，无氧环境的氧浓度≤30μmol/L，有氧环境的氧浓度范围为130-180μmol/L。
优选的，这种促进塑料降解的方法，含三价铁、铁还原菌和塑料的体系中，还包含铁配位体；进一步优选的，铁配位体为三聚磷酸盐、乙二胺四乙酸(EDTA)、草酸(H2C2O4)、四聚磷酸钠、焦磷酸钠、磷酸钠中的至少一种；再进一步优选的，铁配位体为三聚磷酸盐、乙二胺四乙酸(EDTA)、草酸(H2C2O4)中的至少一种；更进一步优选的，铁配位体为三聚磷酸钠(TPP)、乙二胺四乙酸(EDTA)中的至少一种；乙二胺四乙酸(EDTA)，具有六个配位原子，能和碱金属、稀土元素和过渡金属等形成稳定的水溶性配合物，EDTA能与Fe2+形成Fe2+-EDTA配合物，该配体可原位活化分子氧产生H2O2，进而产生羟基自由基进行污染物降解，有利于Fe2 +的重新活化，产生更多的芬顿(Fenton)试剂；三聚磷酸钠(TPP)，含氧配合物与铁离子以“Fe-O”配位形成可溶性Fe2+-TPP配合物，保证了在宽范围pH内Fe2+以离子状态稳定存在于溶液中，TPP能够强化芬顿的氧化效能，氧化能力的提高得益于Fe2+-TPP配合物能够活化分子氧，遵循O2→O2·-→H2O2→·OH路径强化·OH产生。
优选的，这种促进塑料降解的方法中塑料为聚苯乙烯(PS)、聚乳酸(PLA)、聚氯乙烯(PVC)中的至少一种；进一步优选的，塑料为聚苯乙烯(PS)、聚乳酸(PLA)中的至少一种；再进一步优选的，塑料为聚苯乙烯(PS)。
优选的，这种促进塑料降解的方法中铁还原菌为兼性厌氧菌；进一步优选的，铁还原菌为Shewanella putrefaciens、Shewanella oneidensis、Rhodoferax ferrireducens、Pseudomonas aeruginosa中的至少一种；再进一步优选的，铁还原菌为Shewanellaputrefaciens、Shewanella oneidensis中的至少一种；菌种均来自市面上购买的到的，常规菌种保藏中心如美国菌种保藏管理中心(ATCC)、德国微生物菌种保藏中心(DSMZ)、中国普通微生物菌种保藏管理中心(CGMCC)等。
优选的，这种促进塑料降解的方法，含三价铁、铁还原菌和塑料的体系中，每毫克塑料中的铁还原菌有效活菌数≥0.5×109cfu；进一步优选的，在含三价铁、铁还原菌和塑料的体系中，每毫克塑料中的铁还原菌有效活菌数≥1×109cfu；铁还原菌取对数生长期的铁还原菌。
优选的，这种促进塑料降解的方法，塑料降解过程无氧和有氧交替环境交替周期为4-8h进行一次；进一步优选的，无氧和有氧交替环境交替周期为6h进行一次；再进一步优选的，通过曝氮气维持无氧环境的氧浓度；在交替有氧-无氧的含铁体系中，发生类芬顿反应，生成羟基自由基，兼性厌氧铁还原微生物持续消耗电子供体并生成电子，厌氧条件下，微生物以Fe(III)作为电子受体，Fe(III)得到电子后被还原为Fe(II)；好氧条件下，微生物以O2作为电子受体，O2得到电子后被还原为H2O2，生成的Fe(II)和H2O2两者再进一步发生反应生成羟基自由基。
优选的，这种促进塑料降解的方法，含三价铁、铁还原菌和塑料的体系中，加入铁配位体，铁配位体与含三价铁、铁还原菌和塑料的体系中总铁的摩尔比为(0.08-0.5)：1；进一步优选的，这种促进塑料降解的方法中铁配位体为三聚磷酸盐时，铁配位体与总铁(Fe)的摩尔比为(0.08-0.2)：1；再进一步优选的，铁配位体为三聚磷酸盐时，铁配位体与总铁(Fe)的摩尔比为0.09：1。
进一步优选的，这种促进塑料降解的方法中铁配位体为乙二胺四乙酸(EDTA)时，铁配位体与含三价铁、铁还原菌和塑料的体系中总铁(Fe)的摩尔比为(0.2-0.5)：1；再进一步优选的，铁配位体为乙二胺四乙酸(EDTA)时，铁配位体与总铁(Fe)的摩尔比为0.3：1。
本发明还提供了上述塑料降解方法在水体、土壤、底泥和污泥环境中塑料污染治理的应用。
本发明的有益效果是：
含三价铁、铁还原菌和塑料的体系中，可以有效促进塑料污染的原位降解，该方法操作简单，成本低廉。
在交替有氧-无氧的含铁环境中，会发生类芬顿(Fenton)反应生成羟基自由基，类芬顿反应产生的自由基能促进塑料的降解；兼性厌氧铁还原微生物持续消耗电子供体并生成电子，厌氧条件下，微生物以Fe(III)作为电子受体，Fe(III)得到电子后被还原为Fe(II)；好氧条件下，微生物以O2作为电子受体，O2得到电子后被还原为H2O2，生成的Fe(II)和H2O2两者再进一步发生反应生成羟基自由基。
附图说明
图1赤铁矿水体环境不投加铁配位体14天后聚苯乙烯塑料扫描电镜图；
图2赤铁矿水体环境投加铁配位体乙二胺四乙酸14天后聚苯乙烯塑料扫描电镜图；
图3赤铁矿水体环境投加铁配位体三聚磷酸钠14天后聚苯乙烯塑料扫描电镜图；
图4针铁矿水体环境不投加铁配位体14天后聚苯乙烯塑料扫描电镜图；
图5针铁矿水体环境投加铁配位体乙二胺四乙酸14天后聚苯乙烯塑料扫描电镜图；
图6针铁矿水体环境投加铁配位体三聚磷酸钠14天后聚苯乙烯塑料扫描电镜图；
图7潮间带底泥投加铁配位体与不投加配位体14天后XPS扫描谱图。
具体实施方式
以下通过具体的实施例对本发明的内容作进一步详细的说明。实施例和对比例中所用的原料、试剂或装置如无特殊说明，均可从常规商业途径得到，或者可以通过现有技术方法得到。除非特别说明，试验或测试方法均为本领域的常规方法。
实施例1
(1)在含聚苯乙烯塑料和赤铁矿(Hematite)的液体环境中，投加对数期铁还原菌Shewanella putrefaciens和铁配位体，聚苯乙烯用量为500mg/L，赤铁矿总铁量为10mmol/L，每毫克塑料中的铁还原菌有效活菌数为1×109cfu，铁配位体选用三聚磷酸钠(TPP)或乙二胺四乙酸(EDTA)。
(2)以TPP与总铁摩尔比为0.09:1的比例投加TPP，以EDTA与总铁摩尔比为0.3:1的比例投加EDTA，一次性投加，运行期间无需补充。
(3)曝氮气和空气分别维持无氧和有氧环境，无氧6小时，有氧6小时然后重复，反应在常温下进行，反应时间为14d。
对比例1
在实施例1的基础上，不投加铁配位体，其余与实施例1相同。
实施例2
(1)在含聚苯乙烯塑料和针铁矿(Goethite)的液体环境中，投加对数期铁还原菌Shewanella putrefaciens和铁配位体，聚苯乙烯用量为500mg/L，针铁矿总铁量为10mmol/L，每毫克塑料中的铁还原菌有效活菌数为1×109cfu，铁配位体选用三聚磷酸钠(TPP)或乙二胺四乙酸(EDTA)。
(2)以TPP与总铁摩尔比为0.09:1的比例投加TPP，以EDTA与总铁摩尔比为0.3:1的比例投加EDTA，一次性投加，运行期间无需补充。
(3)曝氮气和空气分别维持无氧和有氧环境，无氧6小时，有氧6小时然后重复，反应在常温下进行，反应时间为14d。
对比例2
在实施例2的基础上，不投加铁配位体，其余与实施例2相同。
实施例3
(1)在含聚苯乙烯塑料的潮间带底泥(Sediment)中，投加对数期铁还原菌Shewanella oneidensis和铁配位体，聚苯乙烯用量为100mg，潮间带底泥干重500g，潮间带底泥总铁含量为141.12±26.32mmol/kg、TN含量为1.19±0.21g/kg、TOC含量为14.18±1.58g/kg，每毫克塑料中的铁还原菌有效活菌数为1×109cfu，铁配位体选用三聚磷酸钠(TPP)或乙二胺四乙酸(EDTA)。
(2)以TPP与总铁摩尔比为0.09:1的比例投加TPP，以EDTA与总铁摩尔比为0.3:1的比例投加EDTA，一次性投加，运行期间每7天补充投加1次配位体，后期补充投加量为初始投加量的50％。反应在常温下进行，反应时间为14d。
对比例3
在实施例3的基础上，不投加铁配位体，其余与实施例3相同。
实施例4
(1)在含聚苯乙烯塑料的污泥中，投加对数期还原菌Shewanella oneidensis和铁配位体，聚苯乙烯用量为100mg，污泥干重100g，污泥总铁含量为111.43±26.32mmol/kg，每毫克塑料中的铁还原菌有效活菌数为1×109cfu，铁配位体选用三聚磷酸钠(TPP)或乙二胺四乙酸(EDTA)。
(2)以TPP与总铁摩尔比为0.09:1的比例投加TPP，以EDTA与总铁摩尔比为0.3:1的比例投加EDTA，一次性投加，运行期间无需补充。
(3)曝氮气和空气分别营造无氧和有氧环境，无氧6小时，有氧6小时然后重复，反应在常温下进行，反应时间为14d。
对比例4
在实施例4的基础上，不投加铁配位体，其余与实施例4相同。
测试结果
对实施例1-2和对比例1-2的·OH累积量进行测试，·OH累积量的测试方法为：苯甲酸为羟基自由基的捕获剂，再用液相色谱测捕获自由基后生成的对羟基苯甲酸的含量，得到羟基自由基的量，测试结果如表1所示；对实施例1-2和对比例1-2的塑料减重率进行测试，根据反应前后塑料的重量确定塑料减重率，测试结果如表2所示；对实施例1-2和对比例1-2的O/C比进行测试，O/C比通过XPS测定，测试结果表3所示；实施例1-2和对比例1-2反应14天后聚苯乙烯塑料扫描电镜图如附图1-6所示。
表1实施例1-2、对比例1-2羟基自由基累积量
Figure BDA0003158569810000051
表2实施例1-2、对比例1-2塑料减重率
赤铁矿 赤铁矿+TPP 赤铁矿+EDTA
减重率(％) 10.44 13.65 11.65
针铁矿 针铁矿+TPP 针铁矿+EDTA
减重率(％) 6.90 17.87 15.60
表3实施例1-2、对比例1-2O/C比测试结果
赤铁矿 赤铁矿+TPP 赤铁矿+EDTA
O/C比(％) 6.25 11.54 10.01
针铁矿 针铁矿+TPP 针铁矿+EDTA
O/C比(％) 7.49 8.25 11.42
在含聚苯乙烯塑料的液体环境中，如表1-3所示，当赤铁矿组中有配位体时(赤铁矿+TPP和赤铁矿+EDTA组)聚苯乙烯塑料减重率比无配体对照组(赤铁矿组)增加10％-30％，·OH累积量增加18％-250％，O/C比增加60％-84％；含针铁矿组中有配位体时(针铁矿+TPP和针铁矿+EDTA组)聚苯乙烯塑料减重率比无配体对照组(针铁矿组)增加126％-159％，·OH累积量增加91％-198％，O/C比增加10％-52％；如图1-6所示，添加铁配位体组塑料的表面出现孔洞比不添加铁配位体组的多且大，表明在交替无氧-有氧环境中添加铁配位体促进了水体中塑料的降解。
对实施例3-4和对比例3-4的·OH累积量进行测试，测试结果如表4所示；对实施例3-4和对比例3-4的O/C比进行测试，测试结果如表5所示；实施例3与对比例3聚苯乙烯14天后XPS扫描谱图如附图7所示。
表4实施例3-4、对比例3-4羟基自由基累积量
Figure BDA0003158569810000061
表5实施例3-4、对比例3-4O/C比测试结果
潮间带底泥 潮间带底泥+TPP 潮间带底泥+EDTA
O/C比(％) 5.11 24.69 17.08
污泥 污泥+TPP 污泥+EDTA
O/C比(％) 4.92 11.97 19.58
在含聚苯乙烯塑料的潮间带底泥、污泥环境中，如表4-5所示，当潮间带底泥组中有配位体时(潮间带底泥+TPP和潮间带底泥+EDTA组)比无配体对照组(潮间带底泥组)·OH累积量增加74％-121％，O/C比增加234％-383％；含污泥组中有配位体时(污泥+TPP和污泥+EDTA组)比无配体对照组(污泥组)·OH累积量增加89％-155％，O/C比增加143％-297％；交替无氧-有氧环境或添加铁配位体均能有效促进塑料的降解。

Claims (6)

1.一种促进塑料降解的方法，其特征在于，在含三价铁、铁还原菌和塑料的体系中实现塑料的降解；
所述塑料为聚苯乙烯、聚乳酸、聚氯乙烯中的至少一种；
所述含三价铁、铁还原菌和塑料的体系中，还包含铁配位体；
所述铁配位体为三聚磷酸盐、乙二胺四乙酸、草酸、四聚磷酸钠、焦磷酸钠、磷酸钠中的至少一种；
所述铁配位体与含三价铁、铁还原菌和塑料的体系中总铁的摩尔比为(0.08-0.5)：1。
2.根据权利要求1所述的一种促进塑料降解的方法，其特征在于，所述塑料的降解过程在无氧和有氧交替环境下进行。
3.根据权利要求1所述的一种促进塑料降解的方法，其特征在于，所述铁还原菌为兼性厌氧菌。
4.根据权利要求1所述的一种促进塑料降解的方法，其特征在于，在含三价铁、铁还原菌和塑料的体系中，每毫克塑料中的铁还原菌有效活菌数≥0.5×109cfu。
5.根据权利要求2所述的一种促进塑料降解的方法，其特征在于，所述无氧和有氧交替环境交替周期为4-8h进行一次。
6.权利要求1至5任一项所述的促进塑料降解的方法在水体、土壤、底泥和污泥环境中塑料污染治理的应用。
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