CN115140811A - 一种电渗析海水脱盐协同电催化降解有机污水并产h2o2装置 - Google Patents
一种电渗析海水脱盐协同电催化降解有机污水并产h2o2装置 Download PDFInfo
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Abstract
本发明公开了一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,属于沿海工业用水处理领域。本发明包括接通直流电源的铂片阳极和炭黑气体扩散阴极以及两电极间的阴阳离子交换膜对。在外电压驱动下,阴阳离子交换膜对构成的脱盐室中的氯离子迁移进阳极室,钠离子迁移进阴极室,实现脱盐;铂片阳极通过析氯反应产生次氯酸降解有机污水;炭黑气体扩散阴极电催化还原氧气生成H2O2。该反应装置可实现有机污水和海水的高效、低耗、稳定处理并同步生成工业制成品H2O2,可降低沿海工业用水成本,拥有广阔的应用前景。
Description
技术领域
本发明属于沿海工业用水处理领域,更具体地说,涉及一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置。
背景技术
我国沿海地区水资源短缺日益凸显,11个沿海省(或直辖市)所辖的50多个沿海城市中近九成存在缺水问题,已严重影响了沿海地区经济社会可持续发展。人口稠密、工业发达、需水量大、水环境污染严重是造成沿海地区水资源不足的重要原因。沿海地区海水资源丰富,工业污水排放量大,其中以有机污水排放为主。海水淡化和有机污水的深度处理与回用是解决沿海地区用水紧张的两条重要途径。当前,海水淡化与有机污水处理往往是在不同场景下单独进行。海水淡化通常采用反渗透、多级闪蒸、多效蒸发等技术处理,存在高压力、高能耗、浓缩卤水难以处理等问题;有机污水处理通常采用生化法进行处理,存在污水成分复杂导致可生化性差,处理能耗高等问题。显然,将两者分开进行处理面临着建厂和运行成本高、水处理效果差、卤水难以处理等问题。
将有机污水与海水同步处理有望解决两者分开处理面临的问题。当前的有机污水与海水同步处理技术是将微生物燃料电池或光催化燃料电池与电渗析膜堆脱盐进行有效复合(Science of Total Environment,2020,748,141046;Applied Catalysis B:Environmental,2021,284,119745),将电渗析膜堆内置于微生物燃料电池或光催化燃料电池两电极之间,利用微生物燃料电池或光催化燃料电池所产电能作为电渗析膜堆脱盐动力,实现有机污水降解和海水脱盐。中国专利CN111816902A公开了一种应用于化工尾水处理的电容式微生物脱盐电池装置及方法,属于水资源处理技术领域。电池装置包括分别用阴、阳离子交换膜隔开的阳极室、除盐室和阴极室;阳极采用碳材料,阴极采用包括依次设置的中空碳纤维-碳膜电容层、钛基层、防水层和催化层形成的中空碳纤维-碳膜电容电极;阳极和阴极之间用外电路连接。但是微生物燃料电池利用微生物分解产生电流,运行复杂、产电不稳定,且微生物对特殊污染物敏感,难以处理高毒性难降解污染物。
光催化燃料电池的光生电子和空穴容易复合,半导体电极的光电转化效率较低,单靠光催化产电难以有效驱动系统运行。以微生物燃料电池、光催化燃料电池与反向电渗析膜堆构建的复合反应装置在同步处理有机污水与海水时存在着较大的缺陷,难以商业化应用。因此,设计一个结构简单、运行稳定且高效、可处理多种有机污水和海水的简易反应装置具有非常重要的意义。
经检索,专利公开号为CN105236527A,公开日2016为1月13日,该发明公开了一种废水同步连续脱盐除有机污染物的三维电极装置及绿色电化学处理方法。该装置包括阳离子交换树脂单元、阴离子交换树脂单元、极室单元和若干个OFR电催化单元;极室单元中放入硫酸纳作为极室循环液;离子交换树脂单元装有离子交换树脂填料,阴离子交换膜置于阴极区,阳离子交换膜置于阳极区;OFR电催化单元装有OFR专用填料;装置中部的OFR电催化单元为浓水的形成及收集区;废水依次经过OFR电催化单元、阳离子交换树脂单元、OFR电催化单元、阴离子交换树脂单元,最后排出装置,实现同步除盐除有机物的目的。该装置是采用三维电极催化产生羟基自由基去除有机污染物,利用电渗析和离子交换树脂进行脱盐,所处理的目标水体为含盐有机污水。其不足之处在于,该装置构成复杂,构建成本相对较高,运行前需对水体进行曝气处理,所用填料需进行预处理,运行相对复杂,效率低。
发明内容
1.要解决的问题
针对现有有机污水与海水同步处理装置运行不稳定,效率低的问题,本发明提供一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置。该装置运行稳定、高效,可用于海水脱盐和处理不同种类的有机污水并产H2O2。
2.技术方案
为了解决上述问题,本发明所采用的技术方案如下:
一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,包括电源、阴极、发生阴极反应的阴极室以及靠近阴极室的阳离子交换膜;阳极、发生阳极反应的阳极室以及靠近阳极室的阴离子交换膜;脱盐室,位于阴离子交换膜和阳离子交换之间。
其中,所述阴极室和阳极室中盛有电解质,阳极室中盛有有机污水,所述脱盐室中盛有海水,所述海水中的NaCl浓度为35g/L,也可适用于NaCl浓度为15g/L-45g/L的海水或NaCl溶液,实际使用过程中,NaCl浓度无限制。所述电解质可以是K2SO4,也可以是Na2SO4,能满足导电即可。
本发明的装置可用于氨苄西林的降解,还可用于其他有机污染物的降解,能被次氯酸降解即可。
进一步地,所述电源为直流电源,电压为3-5V,电流为20-90mA,其中,电压需要满足大于1.36V,其原因在于,氯离子被氧化生成氯气的反应在电压大于1.36V的情况下才能实现。其通过太阳能、风力或水力发电提供,可以充分利用广阔的沿海户外环境,安装相应的太阳能、风力或水力发电设施给直流电源充电,以提高整个装置的持续稳定性和使用寿命。所述电源也可以是交流电,但需要匹配整流器转化为直流电运行。
进一步地,所述阴极为气体扩散电极,电极材料可为铂碳、活性焦、石墨、炭黑等,优选的为炭黑气体扩散电极,所述炭黑气体扩散电极中以钛丝网为电极骨架,由炭黑、高纯导电石墨粉复合而成,除此之外,还可使用其他气体扩散电极,能实现电催化产H2O2即可,利用炭黑气体扩散电极,含有的碳元素是生成H2O2的优良电极材料,无毒,低成本,且电极的多孔材料可使空气中的氧气自主渗透进入阴极溶液中,参与阴极还原反应,其中,电解水生成H2O2的电位是0.695V,阴极还原反应式为2H++2e-+O2→H2O2。
进一步地,所述阳极为析氯电极,可以选用铂片电极,也可采用其他析氯电极如钛电极、二氧化铅电极、钛涂钌铱电极等。
进一步地,所述阳极的形状为板状,还可以为片状、棒状或网状等。
进一步地,所述阴离子交换膜和阳离子交换膜成对设置构成电渗析膜,所述电渗析膜的数量为一组或多组,多组离子交换膜成对堆叠而成,根据盐度负荷进行匹配。
现有技术中采用微生物燃料电池实现海水脱盐协同降解有机污水,如专利CN111816902A,钠离子和氯离子在渗透压和微生物产电电压的作用下分别向阴极和阳极迁移。阳极中微生物通过新陈代谢吞入待降解的物质,并释放电子和质子,其中电子被收集后经电极输出产生电压,微生物产电电压输出低且不稳定,驱动效果差。迁移进阳极室的氯离子无法被消耗,与微生物代谢产生的质子结合形成盐酸,导致溶液酸性增强,对微生物生存不利,影响降解和产电效果。此外,微生物燃料电池利用微生物将有机物中的化学能直接转化成电能,运行前有准备期,运行后有恢复期,运行复杂。
因此本发明采用电渗析耦合电化学催化,使用过程中,在渗透压和外电压共同驱动下,脱盐室中的氯离子向阳极室迁移,钠离子向阴极室迁移,实现海水脱盐,相较于渗透压和微生物产电、光催化产电驱动的离子迁移,电能输出更稳定,驱动力更强,催化反应也更高效。其中,氯离子在阳极室中被氧化,生成氯气,氯气溶于水中生成次氯酸,通过电催化析氯反应生成次氯酸降解有机污水;电子通过外电路迁移至炭黑气体扩散阴极,将氧气还原为H2O2。利用该装置进行海水脱盐协同催化降解有机污水并产H2O2,可有效解决微生物脱盐装置和光催化脱盐装置运行启动慢、处理效率低、运行不稳定、难以处理高毒性和难降解有机污水等问题,实现对有机污水和海水同步高效、低耗、长期稳定处理。
本发明的装置可用于氨苄西林的降解,还可用于其他有机污染物的降解,能被次氯酸降解即可。
3.有益效果
相比于现有技术,本发明的有益效果为:
(1)本发明的一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,可有效解决微生物脱盐装置和光催化脱盐装置运行启动慢、处理效率低、运行不稳定、难以处理高毒性和难降解有机污水等问题,实现对有机污水和海水同步高效、低耗、长期稳定处理;
(2)本发明的一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,应用范围广,可处理水质较差、有机污染严重超标的工业有机污水,同步海水脱盐并产H2O2;电催化处理效果显著,氨苄西林去除率>90%,海水脱盐率>50%,H2O2产量高达3g/L;
(3)本发明的一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,可有效规避高管网建设成本、复杂的有机污水和海水处理工艺设施、浓缩卤水的处理与处置等问题,具有流程短、投资省、运行与维护成本低等特点,在面向未来的低碳水处理市场有望得到大力推广应用;
(4)本发明的一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,可针对沿海工业城市的工业有机污水再生和淡化海水作为工业用水,为这些城市工业用水处理提供理论依据和技术参考。
附图说明
以下将结合附图和实施例来对本发明的技术方案作进一步的详细描述,但是应当知道,这些附图仅是为解释目的而设计的,因此不作为本发明范围的限定。此外,除非特别指出,这些附图仅意在概念性地说明此处描述的结构构造,而不必要依比例进行绘制。
图1为本发明反应装置运行示意图;
图2为不同电压下反应装置运行效果,(a)氨苄西林去除率,(b)海水脱盐率,(c)H2O2产量,(d)输出电流;
图3为不同氨苄西林浓度下反应装置运行效果,(a)氨苄西林去除率,(b)海水脱盐率,(c)H2O2产量,(d)输出电流,其中电压为4V;
图4为不同海水盐度下反应装置运行效果,(a)氨苄西林去除率,(b)海水脱盐率,(c)H2O2产量,(d)输出电流。
具体实施方式
下文对本发明的示例性实施例的详细描述参考了附图,该附图形成描述的一部分,在该附图中作为示例示出了本发明可实施的示例性实施例。尽管这些示例性实施例被充分详细地描述以使得本领域技术人员能够实施本发明,但应当理解可实现其他实施例且可在不脱离本发明的精神和范围的情况下对本发明作各种改变。下文对本发明的实施例的更详细的描述并不用于限制所要求的本发明的范围,而仅仅为了进行举例说明且不限制对本发明的特点和特征的描述,以提出执行本发明的最佳方式,并足以使得本领域技术人员能够实施本发明。因此,本发明的范围仅由所附权利要求来限定。
将铂片作为阳极插入阳极室中,将所制备的炭黑气体扩散电极作为阴极插入阴极室中,阳极室与脱盐室之间固定有一张阴离子交换膜,阴极室与脱盐室之间固定有一张阳离子交换膜,构成一个三室反应装置。其中,阳极室内含有难降解有机污水及0.05M硫酸钾电解质,阴极室内含有0.05M硫酸钾电解质,脱盐室含有35g/L氯化钠溶液。所述阳极和阴极通过外部电路连通并由所述外电源驱动催化反应产电,阳极发生析氯反应产生次氯酸降解有机污水,阴极通过电催化氧还原反应生成H2O2,通过电压驱动中间脱盐室海水脱盐,从而实现有机污水降解、海水脱盐和产H2O2。
实施例1-6
将铂片作为阳极插入阳极室,将炭黑气体扩散电极作为阴极插入阴极室,用导线连接两电极并外接直流电源。在阳极室和阴极室之间分别固定一张阳离子交换膜和阴离子交换膜,其中阳离子交换膜靠近阴极室一侧。阳极室中含有200mg/L氨苄西林(AMP)和0.05M硫酸钾溶液,阴极室中含有0.05M硫酸钾溶液,脱盐室中含有浓度为35g/L氯化钠溶液。接通外电源后,考察不同电压下反应装置的降解、脱盐和产H2O2性能。
本实施例的反应装置在运行3h后可有效实现有机污水降解、海水脱盐和产H2O2,但在不同外电压作用下的处理效果有较大差别,具体结果见图2、表1。
表1实施例1-6运行效果
运行效果 | 实施例1 | 实施例2 | 实施例3 | 实施例4 | 实施例5 | 实施例6 |
施加电压 | 0V | 1V | 2V | 3V | 4V | 5V |
AMP去除率 | 0% | 0% | 41.6% | 70.7% | 90.1% | 92.4% |
输出电流 | 0mA | 0mA | 2-3mA | 20-26mA | 29-48mA | 40-90mA |
NaCl去除率 | 18.6% | 20% | 24.7% | 48.4% | 74.2% | 92% |
H<sub>2</sub>O<sub>2</sub>产量 | 0mg/L | 0mg/L | 165mg/L | 1793mg/L | 3083mg/L | 3588mg/L |
如表1所示,当外电压为0、1、2、3、4、5V时,AMP的去除率分别为0%、10%、41.6%、70.7%、90.1%、92.4%;输出电流分别为0mA、0mA、2-3mA、20-26mA、29-48mA、40-90mA;NaCl去除率分别为18.6%、20%、24.7%、48.4%、74.2%、92%;H2O2产量分别为0mg/L、0mg/L、165mg/L、1793mg/L、3083mg/L、3588mg/L。电压为零,脱盐室仅依靠渗透压进行脱盐,离子迁移产生的电压不足以发生析氯反应和氧还原反应,因此系统中没有AMP降解和H2O2产生。当电压为1V时,未达到析氯反应电压,因此没有AMP去除,没有电子迁移和H2O2生成。当电压为3-5V时,达到了析氯反应和氧还原反应电压,电压越高,脱盐室离子迁移越快,阴极室和阳极室中催化反应越快,因此AMP去除率、NaCl去除率和H2O2产量越高。
因此,从AMP降解、脱盐室脱盐、H2O2产量以及用电量等方面综合考虑,外电压为2V以上,优选为3V以上,更优选为3-5V。
实施例7-9
按照实施例1的方法进行测试,只改变AMP的浓度,具体如图3、表2。
表2实施例7-9运行效果
运行效果 | 实施例7 | 实施例8 | 实施例9 |
AMP浓度 | 100mg/L | 200mg/L | 300mg/L |
AMP去除率 | 100% | 91% | 77.5% |
输出电流 | 26-50mA | 27-55mA | 26-52mA |
NaCl去除率 | 64.7% | 62.1% | 62.5% |
H<sub>2</sub>O<sub>2</sub>产量 | 3053mg/L | 3823mg/L | 3410mg/L |
如表2所示,当AMP浓度为100mg/L、200mg/L、300mg/L时,AMP的去除率分别为100%、91%、77.5%,AMP去除率随着AMP浓度的增加而降低;输出电流分别为26-50mA、27-55mA、26-2mA,反应装置输出电流不受AMP浓度影响;NaCl去除率分别为64.7%、62.1%、62.5%,脱盐室中NaCl去除率不受AMP浓度影响;H2O2产量分别为3053mg/L、3823mg/L、3410mg/L,H2O2产量基本不受AMP浓度影响。其原因在于,反应装置中阳极为析氯反应,AMP的浓度只影响其与次氯酸的反应,并不影响阳极析氯反应,因此对反应装置的产电、脱盐和产H2O2基本无影响。
因此,从AMP降解、脱盐室脱盐、H2O2产量以及用电量等方面综合考虑,AMP浓度为100mg/L以上,优选为200mg/L。
实施例10-13
按照实施例1的方法进行测试,只改变海水的盐度,即NaCl浓度,具体如图4、表3。
表3实施例10-13运行效果
当海水盐度为15g/L、25g/L、35g/L、45g/L时,AMP的去除率分别为61.1%、76.5%、91%、92.5%,AMP去除率随着海水盐度的增加而增加;输出电流分别为25-32mA、27-51mA、27-55mA、34-70mA,反应装置输出电流随着海水盐度的增加而增加;NaCl去除率分别为88.3%、81.1%、62.5%、60.5%,NaCl去除率随着海水盐度的增加而降低;H2O2产量分别为1950mg/L、2945mg/L、3738mg/L、4720mg/L,H2O2产量随着海水盐度的增加而增加。海水盐度的增加会提高海水与阴极室、阳极室溶液之间的渗透压,加快脱盐室内离子向阴极室、阳极室迁移速度,使阳极内氯离子浓度升高,促进了析氯反应,提高了有机物降解速率,加速电子向阴极迁移速度,从而提高装置输出电流和H2O2产量。
因此,从AMP降解、脱盐室脱盐、H2O2产量以及用电量等方面综合考虑,海水盐度为15g/L以上,优选为35-45g/L。
本发明的电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,将电催化降解污水与电渗析海水脱盐进行有效复合。本发明在较低电压驱动下即可将脱盐室中海水脱盐,通过电催化将海水中的氯离子转化为次氯酸降解有机污水并同步生成工业制成品H2O2,实现了工业有机污水和海水的同步高效、低耗、稳定、资源化处理。
Claims (10)
1.一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,包括电源;阴极、发生阴极反应的阴极室以及靠近阴极室的阳离子交换膜,所述阴极室中盛有电解质;阳极、发生阳极反应的阳极室以及靠近阳极室的阴离子交换膜,所述阳极室中盛有电解质和有机污水;脱盐室,位于阴离子交换膜和阳离子交换之间,所述脱盐室中盛有海水,所述电源的正极连接阳极,电源的负极连接阴极。
2.根据权利要求1所述一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,所述有机污水为包含氨苄西林的污水。
3.根据权利要求2所述一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,所述电源为直流电源,所述电源的电压为3-5V。
4.根据权利要求3所述一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,所述阳极为析氯电极,所述析氯电极为铂片电极、钛电极、二氧化铅电极、钛涂钌铱电极中的一种或多种。
5.根据权利要求4所述一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,所述阳极的形状为板状、片状、棒状、网状中的一种或多种。
6.根据权利要求5所述一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,所述阴极为气体扩散电极,所述气体扩散电极的材质为铂碳、活性焦、石墨、炭黑中的一种或多种。
7.根据权利要求6所述一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,所述阴极为炭黑气体扩散电极,所述炭黑气体扩散电极中以钛丝网为电极骨架,由炭黑、高纯导电石墨粉复合而成。
8.根据权利要求7所述一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,所述阴离子交换膜和阳离子交换膜成对设置构成电渗析膜,所述电渗析膜的数量为一组或多组。
9.根据权利要求8所述一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,所述海水中的NaCl浓度为15g/L-45g/L。
10.根据权利要求9所述一种电渗析海水脱盐协同电催化降解有机污水并产H2O2装置,其特征在于,所述电解质包括K2SO4和Na2SO4中的一种或多种。
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