CN115106071B - 一种污水处理用磁性材料及其应用 - Google Patents
一种污水处理用磁性材料及其应用 Download PDFInfo
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- B01J20/28002—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their physical properties
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- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
- B01J20/06—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04
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- B01J20/20—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
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- B01J20/223—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material containing metals, e.g. organo-metallic compounds, coordination complexes
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Abstract
本发明公开了一种污水处理用新型磁性材料,该磁性材料采用油酸表面修饰的磁性Fe3O4纳米颗粒,以香蕉皮基生物炭进行功能化修饰,即得;香蕉皮基生物炭采用无氧环境下干燥的香蕉皮进行热解处理获得。本发明以食物废料‑香蕉皮对磁性纳米颗粒进行功能化修饰,由于其中富含木质素、半纤维素、纤维素,其分子式中含有大量的羟基官能团,对磁性纳米颗粒进行修饰,能有效增加其对污水中金属离子的吸附作用。同时油酸表面修饰后的磁颗粒具有良好的沉降稳定性和有效避免聚团现象。
Description
技术领域
本发明涉及一种针对磁性材料进行功能化及修饰的技术,用以改良污水中重金属的处理。
背景技术
在环境治理中,重金属污染是尤其重要的问题。铜污染是其中的一种,指铜(Cu)及其化合物在环境中所造成的污染。主要污染来源是铜锌矿的开采和冶炼、金属加工、机械制造钢铁生产等。铜是生命所必需的微量元素,但过量的铜对人和动、植物都有害。
磁性纳米颗粒以及生物吸附剂的相关研究是近几年的热点。在环境处理领域,纳米技术是21世纪最受关注的高新技术之一;作为纳米材料的一个重要分支,磁性纳米颗粒(MNPs)兼具纳米粒子和磁性材料的特性。将其应用于废水吸附处理领域具有众多优势,包括MNPs具有超顺磁性、巨大比表面积、表面易于功能化等特点,即既能增强吸附能力,又能避免二次污染,实现吸附材料的多次回收利用。
生物炭是一类富含碳素的黑色固体物质。在热解过程中产生众多含氧官能团如羧基、羟基以及其他羧酸酯结构,这些结构令生物炭的吸附能力和抗氧化能力极为优秀。
金属有机骨架配合物(MOFs)是一类由无机金属中心(金属离子或金属簇)与桥连的有机配体通过自组装相互连接,形成的一类具有周期性网络结构的晶态多孔材料。金属有机框架化合物MIL-101(Cr),其单位分子式为C24O15FCr3.O,单位分子量为719.2339。是有配位金属Cr和配体对苯二甲酸通过配位反应制备的具有面心立方晶体结构的配位聚合物。
现有技术中,针对不同材料的特性,考虑以不同材料、甚至多种材料结合进金属离子吸附研究。国内研究者孔维屏在1987年就提出过利用氧化铁对铜离子进行吸附(孔维屏.氧化铁、氧化锰及胡敏酸对铜离子吸附强度的初步比较[J].农业环境科学学报,1987(06):11-13.)。随后各种学者也利用不同的物质通过物理吸附或者化学吸附去除铜离子。利用生物炭(专利号:CN111085170A)(佟雪娇. 生物质炭对水体/红壤中Cu(Ⅱ)的去除和固定作用[D].南京农业大学,2011.)、(郭金越. 生物炭/铁酸锰复合材料对铜锌复合污染土壤的稳定化效果及机制研究[D].内蒙古科技大学,2019.DOI:10.27724/d.cnki.gnmgk.2019.000220.)、(李杰. 生物炭复合金属氧化物的制备及其去除水中重金属的机制研究[D].青岛科技大学,2018.);利用磁颗粒(专利号CN106315739B)、(李敏,曹允洁.磁性改性纳米碳管对Cu~(2+)吸附性能研究[J].化工技术与开发,2021,50(10):14-16+51.)、(姜艳慧,许丽丽,索红波,于琳琳,董炳刚,姜祥坤,薛庆旺,柳仁民.聚乙烯亚胺-磁性羧甲基纤维素复合物对铜离子和镉离子的吸附[J].分析试验室,2021,40(10):1135-1139.DOI:10.13595/j.cnki.issn1000-0720.2021.031501.);利用有机金属骨架(娄杰,付秋平,汪玲玲,刘秋霞,余磊,胡华林.金属有机骨架材料MOF(Ni)-74对水中Cu~(2+)的吸附性能研究[J].化工新型材料,2021,49(06):192-196.DOI:10.19817/j.cnki.issn1006-3536.2021.06.042.)、(专利CN1910191B)。这些材料在吸附水中铜离子方面有以下缺点:1.在制备生物炭过程中可能会生成一些环境污染物(如PAHs)或者重金属残留。2.生物炭处理过的水体,其固有的重金属和多环芳经等污染物可能会导致土壤污染。3.制备的磁颗粒粒径大小不好控制、会存在粒子团聚严重,从而导致吸附效果变弱。4.单独适用有机金属骨架吸附或降解污染物后分离步骤复杂,既不经济也不环保。
发明内容
本发明的目的是为了解决现有技术中存在的缺陷,提供一种新型的重金属离子吸附剂,该吸附剂能有效利用食品废料-香蕉皮,且制备工艺简便。
为了达到上述目的,本发明提供的技术方案如下:
一种污水处理用新型磁性材料,该磁性材料采用磁性Fe3O4纳米颗粒,以香蕉皮基生物炭对其进行功能化修饰,再使用油酸对其进行表面活性修饰,即得;香蕉皮基生物炭采用无氧环境下干燥的香蕉皮进行热解处理获得。
本发明以食物废料-香蕉皮对磁性纳米颗粒进行功能化修饰,由于其中富含木质素、半纤维素、纤维素,其分子式中含有大量的羟基官能团,与磁性纳米颗粒进行复合,能有效增加其对污水中金属离子的吸附作用,同时用油酸进行表面活性剂能有效改善磁颗粒的沉降稳定性和聚团现象。
在部分实施例中,作为优选的,所述污水处理用磁性材料采用磁性Fe3O4纳米颗粒,以香蕉皮基生物炭进行功能化修饰,再采用油酸对其进行表面活性修饰后,再与金属有机骨架材料进行复合即得;所述金属有机骨架材料以硝酸铬和对苯二甲酸为原料制备。
本发明同时利用金属有机骨架MOFs,由于其具有可设计和精准控制的拓扑结构、高的比表面积,对光生电子有多种传递机制等特性,污染物吸附与光催化降解方面有优良表现,将其与磁性纳米颗粒复合,增加其比表面积,有效增加吸附节点,进一步提高吸附率。
在部分实施例中,较为优选的,所述香蕉皮基生物炭的制备方法如下:在无氧环境下干燥香蕉皮,研磨成粉状;将干燥香蕉皮粉末置于无氧干燥箱中,梯度升温(每分钟升温5℃)至250~300℃(较佳在250~280℃,优选250℃),梯度热解5小时,即得所述香蕉皮基生物炭。
本发明通过对香蕉皮基生物炭的制备工艺进行研究,筛选出较为优选的热解时间,以较低温度得到生物炭和固体的酸碱性为弱酸性或中性,可以简化一般高温制备中得到的碱性生物炭还需要调节pH值至中性的步骤;且在低温热解的条件下,香蕉皮内富含的木质素不会被破坏,最终获得的生物炭表面官能团含量高,对磁性纳米颗粒修饰后针对可离子化溶质的吸附有很大的提升作用。
进一步的,对磁性Fe3O4纳米颗粒采用以下方法将香蕉皮基生物炭搭载到四氧化三铁磁颗粒中并进行表面活性修饰:取六水合氯化铁和四水合氯化铁,分布加入超纯水中溶解制备溶液,将制备获得的氯化铁溶液和氯化亚铁溶液混合加热,在混合溶液中缓慢滴加一水合氨水溶液(体积浓度为25%),滴加同时充分搅拌;一水合氨溶液滴定的同时加入香蕉皮基生物炭;待一水合氨溶液滴定结束后加入油酸;再加入硅烷偶联剂,充分搅拌;采用去离子水、无水乙醇交替洗涤,所得湿沉淀,置于真空干燥箱中干燥得到黑色固体颗粒,即为香蕉皮基生物炭复合的四氧化三铁磁性纳米颗粒。
在部分实施例中,作为优选的,所述六水合氯化铁、四水合氯化铁、一水合氨溶液、香蕉皮基生物炭、油酸、硅烷偶联剂的加入比例为21.6g:8.1g:100mL: 5g:6ml:4ml。
进一步的,香蕉皮基生物炭复合的四氧化三铁磁性纳米颗粒通过以下方法与金属有机骨架材料进行复合:将硝酸铬和对苯二甲酸加入醋酸钠水溶液(0.05mol/L)中,充分搅拌后,加入表面活性修饰后的香蕉皮基生物炭复合四氧化三铁磁性纳米颗粒,放置于水热反应釜中。密封好以后放入已经提前加热到180℃的恒温鼓风干燥箱中24小时,得到湿沉淀。反应结束后,分别用去离子水、无水乙醇清洗,磁分离。100℃下真空干燥12h,即得BPB/Fe3O4@ MIL-101(Cr)/OA。
在部分实施例中,作为优选的,所述硝酸铬、对苯二甲酸和香蕉皮基生物炭复合的四氧化三铁磁性纳米颗粒的加入比例为(2.0~4.0)g:(1.0~2.0)g:100mg,最佳的,硝酸铬、对苯二甲酸和香蕉皮基生物炭复合的磁性纳米颗粒的加入比例为2.0g:1.0g:100mg。
本发明还提供了上述污水处理用新型磁性材料回收利用的方法:将使用后的磁性材料置于0.1的HCL,在60℃的温度下磁力搅拌器旋转80min。
本发明还提供了上述污水处理用新型磁性材料在去除污水中铜离子上的应用。
本发明相比现有技术具有以下优点:
1.本发明在对磁性纳米颗粒吸附剂进行表面活性修饰时,使用油酸作为表面活性剂:油酸为疏水性烷烃分子,其中的碳氢链是亲油基团。使用油酸提高了吸附剂的疏水性能。在吸附剂与金属离子发生络合作用以及由于电负性而导致的吸附之后,其高疏水性能可以使金属离子脱离水溶液,不易重新回归到原溶液中,增强吸附强度以及稳定性。
2.同时本发明采用香蕉皮基生物炭BPB作为功能化修饰材料,制备BPB的温度在250℃-300℃左右:使用较低温度得到生物炭和固体的酸碱性为弱酸性或中性,可以简化一般高温制备中得到的碱性生物炭还需要调节Ph至中性的步骤。同样,吸附铜离子主要是依靠氨基、羧基等官能团,香蕉皮本身富含的木质素,在250℃-300℃左右木质素不会被破坏同时低温下制备的生物炭表面官能团含量较高,针对可离子化溶质的吸附有很大益处。
3.本发明通过功能化表面修饰改性磁流体,可以有效改善磁颗粒的沉降稳定性和聚团现象。提高吸附剂比表面积来提高吸附节点来达到提高吸附率的作用。
4.此外,本发明还通过加载金属有机骨架MIL-101(Cr)增加其比表面积。
附图说明
图1为本发明污水处理用新型磁性材料的制备流程图;
图2为本发明污水处理用新型磁性材料的吸附原理图;
图3为410nm波长下铜离子(浓度0-60mg/L)吸光度的标准曲线图;
图4为410nm波长下铜离子(浓度0-2mg/L)吸光度的标准曲线图;
图5为均方差图;
图6为吸附10min条件下吸附次数与吸光度的曲线;
图7为吸附20min条件下吸附次数与吸光度的曲线;
图8为实施例1吸附剂吸附率散点图;
图9为实施例2吸附剂吸附率散点图;
图10为实施例3吸附剂吸附率散点图;
图11为实施例4吸附剂吸附率散点图;
图12为实施例5吸附剂吸附率散点图;
图13为实施例6吸附剂吸附率散点图;
图14为吸附率随重复利用次数的变化曲线。
实施方式
下面结合具体实施例对本发明进行详细说明。
实施例
如图1所示,本发明污水用吸附剂BPB/Fe3O4@ MIL-101(Cr)/OA的制备过程如下:
一、香蕉皮基生物炭制备
1. 在无氧环境下以100℃的温度干燥洗净的香蕉皮4小时并研磨得到固体粉末。
2. 在无氧干燥箱中将粉末以5℃/分钟的梯度升温至250℃,梯度热解总时长5小时,制备得到香蕉皮基的生物炭BPB。
二、BPB/Fe3O4/OA的制备
3. 称取21.6g的六水合氯化铁和8.1g的四水合氯化亚铁,分别加入100ml和50ml超纯水进行溶解。
4. 将溶解后的氯化铁溶液和氯化亚铁溶液混合在60℃的水浴锅中加热30分钟。
5. 在混合溶液中滴加一水合氨水溶液(体积浓度为25%)100ml,并使用磁力搅拌器充分搅拌,滴加速度为3秒4-5滴。
6. 在一水合氨溶液滴加的同时,加入步骤2得到的香蕉皮基生物炭BPB 5g。
7. 在一水合氨溶液滴定结束后,加入6ml OA(油酸)表面活性剂并搅拌1小时。
8. 加入硅烷偶联剂4ml并搅拌30min。
9. 使用去离子水、无水乙醇交替清洗3-4次得到湿沉淀(BPB/Fe3O4/OA)。
三、磁性MOF材BPB/Fe3O4@ MIL-101(Cr)/OA的制备
10. 称取2.0g的和 1.0 g的对苯二甲酸(H2BDC)溶于25ml 0.05mol/L的醋酸钠水溶液中
11. 使用强力搅拌器搅拌20min。
12. 将11所得到的混合溶液加入100mg的BPB/Fe3O4/OA放置于水热反应釜中。
13.密封好以后放入已经提前加热到180℃的恒温鼓风干燥箱中24小时,得到湿沉淀。
14.反应结束后,分别用去离子水、无水乙醇清洗,磁分离。100℃下真空干燥12h,即得BPB/Fe3O4@ MIL-101(Cr)/OA。
如图2所示,本发明制备获得的吸附剂BPB/Fe3O4@ MIL-101(Cr)/OA进行铜离子吸附的作用原理如下:
本发明中的吸附剂吸附原理如图所示,其对铜离子的吸附过程中涉及到了配位键的相互作用、化学键的作用、酸碱的相互作用、静电力的相互作用、范德华力等多种机制:
(1)根据软硬酸碱理论所述水溶液中铜离子属于交界酸,所以容易与弱作用位点反应并附着在其上。
(2)MIL-101吸附剂在金属吸附过程的理论是基于电子对还原的路易斯酸碱理论。在MIL-101中,N和O等电子供体原子在水溶液中铜离子的吸附中起着重要作用。吸附剂中的电子供体原子在酸环境下带正电荷,当PH增加时,电子供体原子被脱质子化,适合带正电荷的重金属离子的吸附。
(3)吸附剂的高比表面积使得在于铜离子吸附时有较多的活性位点,使得范德华力也参与到吸附机制中。
(4)四氧化三铁纳米颗粒在本发明吸附剂中,除了促进吸附分离外胞内扩散机制、络合作用和孔隙结构都提高了吸附剂对铜离子的吸附效率。
(5)四氧化三铁颗粒也可由于其电负性从而达到吸收铜离子的目的。
(6)BPB对铜离子吸附的影响机制包括BPB结构中孔隙和孔容的存在、阳离子交换、化学沉积和静电作用等。
首先通过铜试剂得到在410nm波长下铜离子吸光度的标准曲线如图3、图4所示。
使用数值分析软件分析,发现其标准曲线在0-2mg/L时满足比尔定律,如图5所示。
为了探究吸附剂的去铜离子能力,取含铜离子浓度为200mg/L的水溶液模拟含铜污水,并将上述制备获得的吸附剂BPB/Fe3O4@ MIL-101(Cr)/OA(2g)加入铜离子含量为200mg/L的溶液(50ml),进行铜离子吸附除杂。含铜污水置于除杂装置的时间分别设置为10min、20min、40min,同时设置不同的处理次数(每次处理时间结束后,将处理后的污水再次通入新的吸附剂中再次进行吸附除杂),每组试验重复三次,测定其吸光度如图6、7所示,其铜离子吸附率如图8所示。
从图中可以发现,采用本发明吸附剂进行铜离子吸附,在30min的吸附处理后,就可以达到吸附率为97%,其对铜离子具有优越的吸附效果。
实施例
本实施例吸附剂BPB/Fe3O4@MIL-101(Cr)/OA的制备同实施例1,仅在制备香蕉皮基生物炭BPB的热解处理时,梯度升温至300℃后进行热解处理。
采用与实施例1相同的测定方法测定其吸附率,如图9所示。
实施例
本实施例吸附剂BPB/Fe3O4@MIL-101(Cr)/OA的制备同实施例1,仅在制备香蕉皮基生物炭BPB的热解处理时,梯度升温至280℃后进行热解处理。
采用与实施例1相同的测定方法测定其吸附率,如图10所示。
从实施例1、实施例2、实施例3所制备的吸附剂吸附率试验结果来看,随着香蕉皮基生物炭BPB制备过程中热解温度的上升,所获得的的吸附剂的吸附性能随之有所下降,可能与所得到的吸附剂官能团数量减少有关。
实施例
本实施例吸附剂BPB/Fe3O4@MIL-101(Cr)/OA的制备同实施例1,仅在步骤10中和对苯二甲酸(H2BDC)的用量分别为4.0g的2.0 g。
采用与实施例1相同的测定方法测定其吸附率,如图11所示。
实施例
本实施例吸附剂BPB/Fe3O4@MIL-101(Cr)/OA的制备同实施例1,仅在步骤10中和对苯二甲酸(H2BDC)的用量分别为2.2g的1.3g。
采用与实施例1相同的测定方法测定其吸附率,如图12所示。
实施例
本实施例吸附剂BPB/Fe3O4@MIL-101(Cr)/OA的制备同实施例1,仅在步骤10中和对苯二甲酸(H2BDC)的用量分别为1.2g的1.2 g。
采用与实施例1相同的测定方法测定其吸附率,如图13所示。
从实施例1、实施例4、实施例5、实施例6所制备的吸附剂吸附率试验结果来看,随着和对苯二甲酸(H2BDC)加入量的增加,所获得的的吸附剂的吸附性能随之提高,当/>和对苯二甲酸(H2BDC)加入量达到2.0g、1.0g后,两者加入量增加反而使得成品吸附剂的吸附性能有所下降,是由于当对苯二甲酸含量过高以后,合成的吸附剂内会残留未洗净的对苯二甲酸,造成吸附剂比表面积和孔容的下降。,说明/>和对苯二甲酸(H2BDC)的最佳加入量应选择2.0g和1.0g。
实施例
取实施例1中步骤2制备获得的香蕉皮基生物炭BPB、步骤9中制备获得的BPB/Fe3O4/OA、及步骤13中制备获得的BPB/Fe3O4@ MIL-101(Cr)/OA,并以相同方法制备获得的仅以油酸作为表面活性剂的磁性纳米颗粒Fe3O4/OA,四种吸附剂进行对比。
实验环境:室温;100ml铜离子含量为200mg/L的溶液;溶液pH为7-9均可;吸附剂为5g均达到饱和吸附。测定其达到饱和吸附的吸附时间和铜离子吸附率入下表所示:
从表格中可以看出,以香蕉皮基生物炭进行磁性颗粒表面活性修饰后,即可大幅提高其吸附效率,结合有机金属骨架后,所获得的吸附效率得到了进一步的提升。
实施例
吸附剂重复利用次数的吸附效率变化
取实施例1制备获得的吸附剂进行回收利用实验
实验环境:室温;100ml铜离子含量为200mg/L的溶液;溶液pH为7-9均可;吸附剂为5g且达到饱和吸附。回收使用操作:使用0.1的HCL在加热下磁力搅拌器旋转。其吸附效率随重复利用次数变化如图14所示。
由实验数据可以发现,在前五次重复利用时其对铜离子吸附性能表现良好,均在90%以上,表明吸附剂结构比较稳定,本发明获得的吸附剂具有一定的可重复利用性。在第六次重复利用后吸附能力下降,在第十次重复利用后其吸附能力大大减弱。其原因是由于溶液同铜离子和吸附剂的反应或活性位点的损伤(多孔结构的损伤)导致其吸附能力下降。
Claims (9)
1.一种污水处理用磁性材料,其特征在于,所述污水处理用磁性材料采用磁性Fe3O4纳米颗粒,以香蕉皮基生物炭进行功能化修饰以及油酸对其进行表面活性修饰,即得;所述香蕉皮基生物炭采用无氧环境下干燥的香蕉皮进行热解处理获得;所述香蕉皮基生物炭的制备方法如下:在无氧环境下干燥香蕉皮,研磨成粉状;将干燥香蕉皮粉末置于无氧干燥箱中,梯度升温至250~280℃,梯度热解5小时,即得所述香蕉皮基生物炭。
2.根据权利要求1所述的污水处理用磁性材料,其特征在于,所述污水处理用磁性材料采用磁性Fe3O4纳米颗粒,以香蕉皮基生物炭进行功能化修饰、油酸对其进行表面活性修饰之后,再与金属有机骨架材料进行复合即得;所述金属有机骨架材料以硝酸铬和对苯二甲酸为原料制备。
3.根据权利要求1所述的污水处理用磁性材料,其特征在于,所述干燥香蕉皮粉末在进行梯度热解时,梯度升温至250℃后进行热解。
4.根据权利要求1所述的污水处理用磁性材料,其特征在于,对磁性Fe3O4纳米颗粒采用以下方法进行功能化及修饰:取六水合氯化铁和四水合氯化亚铁,分别加入超纯水中溶解制备溶液,将制备获得的氯化铁溶液和氯化亚铁溶液混合加热,在混合溶液中缓慢滴加一水合氨溶液,滴加同时充分搅拌并加热;在滴加一水合氨溶液的同时加入香蕉皮生物炭,充分搅拌并加热;待一水合氨溶液滴定结束后,加入油酸,充分搅拌并加热;再加入硅烷偶联剂,充分搅拌并加热;采用去离子水、无水乙醇交替洗涤,所得湿沉淀;将湿沉淀置于100℃真空干燥箱中12小时即为表面活性修饰后的香蕉皮基生物炭复合四氧化三铁磁性纳米颗粒。
5.根据权利要求4所述的污水处理用磁性材料,其特征在于,所述六水合氯化铁、四水合氯化亚铁、一水合氨溶液、香蕉皮基生物炭、油酸、硅烷偶联剂的加入比例为21.6g:8.1g:100mL:5g:6ml:4ml;所述一水合氨溶液的体积浓度为25%。
6.根据权利要求2所述的污水处理用磁性材料,其特征在于,表面活性修饰后的香蕉皮基生物炭复合四氧化三铁磁性纳米颗粒通过以下方法与金属有机骨架材料进行复合:将硝酸铬和对苯二甲酸加入醋酸钠水溶液中,充分搅拌后,加入表面活性修饰后的香蕉皮基生物炭复合四氧化三铁磁性纳米颗粒,放置于水热反应釜中;密封好以后放入已经提前加热到180℃的恒温鼓风干燥箱中24小时,得到湿沉淀;反应结束后,分别用去离子水、无水乙醇清洗,磁分离;100℃下真空干燥12h,即得BPB/Fe3O4@ MIL-101(Cr)/OA;醋酸钠水溶液的浓度为0.05mol/L。
7.根据权利要求6所述的污水处理用磁性材料,其特征在于,所述硝酸铬、对苯二甲酸和表面活性修饰后香蕉皮基生物炭复合的四氧化三铁磁性纳米颗粒的加入比例为(2.0~4.0)g:(1.0~2.0)g:100 mg。
8.根据权利要求7所述的污水处理用磁性材料,其特征在于,所述硝酸铬、对苯二甲酸和表面活性修饰后香蕉皮基生物炭复合的磁性纳米颗粒的加入比例为2.0g:1.0g:100mg。
9.权利要求1或2所述污水处理用磁性材料在去除污水中铜离子上的应用。
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