CN115624967A - 一种粒子电极电催化填料制备方法及其使用方法 - Google Patents
一种粒子电极电催化填料制备方法及其使用方法 Download PDFInfo
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Abstract
本发明公开了一种粒子电极电催化填料制备方法及其使用方法,步骤一:配置一定浓度的多组分金属盐溶液,并向该溶液中投加氧化石墨烯、分散助剂和溶剂,并分散成混合液;步骤二:向步骤一中的混合液中加入形成水凝胶的反应单体,经水热反应陈化为复合水凝胶粘结剂;步骤三:将步骤二中复合水凝胶粘结剂和载体材料、辅助粘结剂和增粘剂等按比例造粒成型,所得颗粒依次经过干燥,惰性气体保护下的煅烧碳化,最终制得用于电催化氧化反应的粒子电极电催化填料。污染物去除的增益效果十分显著。可调控污染物向反应位点富集,实现目标污染物的定向传质,可定向增益诸如极性/非极性和偏酸碱性种类污染物的去除效果。节能降耗。有效降低投资成本。
Description
技术领域
本发明涉及电催化氧化催化剂技术领域,具体涉及一种不溶出粒子电极的制备方法及其使用方法。
背景技术
电催化催化氧化法,相较于传统生物法,物理法等污水处理手段,其氧化降解有机污染物的能力更强,在处理难生物降解、高浓度、高毒性的废水时具备难以比拟的优势,更因其“简单高效”、“环境友好”等技术特性被认为是高级氧化水处理工艺中颇具应用潜力的技术之一。其具备以下技术优势:(1)过程中产生羟基自由基等强氧化性物质,可无选择性地降解有机废物,几乎不产生二次污染;(2)反应条件温和,常温常压;(3)模块化性能强,可直接与其他工艺相耦合;(4)操作简便,自动化、集成化程度高。因此,针对该技术亟待解决的技术瓶颈,无论学界还是工业界都十分重视机理和应用层面的深入研究。
电催化氧化去除污染物的机理包括通过在电极表面发生的直接电化学反应或通过电极表面产生的强氧化物种间接氧化有机污染物。其中直接电化学反应包括发生于阳极的氧化反应,以及于阴极上的还原反应:1)有机物在阳极直接发生电化学氧化反应,其氧化能力可以将未完全氧化的物质彻底氧化、有毒高分子物质转化为小分子无毒物质;2)有机物在阳极表面直接发生电化学燃烧,从而彻底矿化,这一步骤为纯电化学反应,其电流效率取决于污染物种类、浓度、电极材料和阳极电位等因素;3)重金属粒子等可还原性污染物在阴极上发生电化学还原进而从水体中去除。另一方面,间接氧化反应是在高电势的阳极作用下产生强氧化性的物种,包括羟基自由基、活性氧物种等,进而与水中有机物发生氧化反应实现彻底矿化。这一步骤为纯化学反应,起反应速率取决于污染物与活性物种的反应速率、浓度以及电极材料的产活性物种的能力决定的。
围绕电化学氧化水处理工艺机理方面的研究基础,工业界归纳出以下局限该工艺工程实用性的技术难点:1)经济易得的电极材料,选择范围十分有限;2)电极寿命普遍较短,更换成本较高;3)反应体系中普遍存在析氢、析氧和电解水等制约电流效率的副反应,高能耗、高运行成本致使其在与其他处理技术对标过程中往往受经济因素制约;4)缺乏系统性的电极反应传质模型,反应器设计受二维平板电极形貌制约,低效传质是推升效率和能耗的主要原因。其中1)受电极材料制约,2)和3)项主要由电极材料本身性质和反应操作条件决定,4)项涉及电化学反应体系本身,即有机污染物只有有效迁移至电极表面,其氧化降解反应才能顺利进行,但事实上不同种类有机物与电极的结合能力相差较大,同时,羟基自由基等在电极表面产生的活性物种的湮灭寿命较短,溶液中的迁移距离非常有限,且与有机物的结合能力也不同。因此,非有效的传质体系极大影响催化效果。
鉴于此背景,早期的行业内部主要攻关高效的电极材料及改性方法,至今已形成形稳阳极(DSA,如钛基体金属氧化物)和掺硼金刚石(BDD)两大较为成熟的阳极体系,其中BDD电极受成本、加工方面制约,而钛基体金属氧化物的应用更为广泛。全新的供电方式,如脉冲供电和线性衰减供电,有利于降低能量的过度消耗,但实际工况中仍主要采取恒流供电的模式。现如今,针对上述电极材料的反应体系优化被认为是克服传质因素制约的有效途径,其降本增效的效果最为立杆见影。电化学反应优化手段的核心是优化流体与电极的接触方式。例如,以非过流方式强制溶液和电极接触,在传统二维平板电极体系中对反应效率有一定增益。为进一步改善反应体系传质,“2.5维”和“3维”电极材料被认为是最具潜力的解决方案。“2.5维”电极指的是“内部磁体-阳极套管-外部磁性颗粒”的新型结构,旨在解决颗粒填料极化不均匀的缺陷。某种程度上仍然是对二维电极材料的表面改性。“3维”电极指的是在二维电极体系之间填充大量复合颗粒,即在外加电场的情况下,通过三维构相中发生的氧化还原反应形成大量微电极,极大地增加电极有效反应面积,显著提升反应速率。通过合理设计的三维电催化体系,具有更小的反应器体积,更少的极板数量,更低的操作电流和功率,以及更长的极板寿命等诸多优点。
文献报道中的粒子电极多采用过渡金属氧化物作为引发剂,专利CN1303257C中介绍了一种铁、铜、锰等过渡金属氧化物为主要引发剂成份的粒子电极,其促进反应的机理为在脉冲直流电的激发下,生成过氧化氢,并在引发剂的催化下,发生类芬顿反应产生强氧化性的羟基自由基,进而降解有机污染物。这类过渡金属氧化物组成的粒子电极其氧化能级往往较低,在由外加电场激发的电子迁移过程中,组份容易以离子形式析出和流失,脱离粒子电极在水体和阴极发生反应,长期将导致电极失效,严重时会导致粉化。此外,在专利文本中作者也提到了该填料因活性物质析出而带来的絮凝作用。
专利CN103539229B中采用了氧化镍为中间层的贵金属银、过渡金属铈和铜掺杂负载的活性氧化铝作为三维粒子电极处理煤化工废水,取得了较好的效果。但由于其引发剂成本中采用了大约9.2g/kg铝基载体的贵金属银,每吨产品的银元素成本高达40000元/吨,成本的大幅增加,对于自身成本较高的电催化氧化工艺来说,不符合成本设计理念。另一方面,由于活性氧化铝本身导电性较低,可能造成运行功率较高,理论能耗可能较高。
专利CN108928890B中直接在电极板之间以CuFe2O4、CoFe2O4、ZnFe2O4、MnFe2O4、NiFe2O4等磁性尖晶石型铁氧体MFe2O4纳米颗粒作为粒子电极,运行过程中需额外投加双氧水、臭氧等氧化剂,在尖晶石粒子电极活性组分和电催化双重作用下促进氧化剂生成氧化能力更强的羟基自由基降解有机污染物,其粒子电级的作用机理主要为类芬顿和电芬顿催化氧化。运行过程中纳米尺寸级别的粒子电极需借助额外搅拌等手段充分混合以及流化才能取得较好效果。此外,文章中并未提及去除出水中纳米颗粒的方法。
专利CN103739043B中介绍了一种双过渡金属负载,二氧化钛P25共掺杂活性炭结构的粒子电极,可通过光催化和电催化两种途径降解有机污染物,遵循的是光致引发和电芬顿生成氧化物种的反应机理,有机物去除效果电催化效应占据主导。其本质仍为一种非稳态电极,活性成份具有溶出的可能性。另一方面,专利中的经过双金属掺杂的二氧化钛,粒子电极的载体活性碳经过酸化改性,用以提升对双金属掺杂二氧化钛的负载,以及极性污染物的吸附。这种弱键能的键合导致二氧化钛具有脱落的潜在可能性,影响长期稳定性。
综上所述,本发明克服传统平板电极以下不足,1、氧化还原反应仅发生二维尺度的极板表面;2、常常需引入电解质等二次污染物;3、针对不同污染物的微观传质仅取决于电极板本身性质,难以实现三维尺度的传质优化;以及因此带来的4、处理效率偏低,设备投入和运行成本均偏高。另一方面,针对常规三维电极,极板。
发明内容
本发明的目的在于提供一种三维稳态粒子电极形式的电催化氧化催化剂的配方和制备方法及其使用方法,以解决上述背景技术中提出的问题。
为实现上述目的,本发明提供如下技术方案:一种粒子电极电催化填料制备方法,包括以下步骤:
步骤一:配置一定浓度的多组分金属盐溶液,并向该溶液中投加氧化石墨烯、分散助剂和溶剂,并分散成混合液;
步骤二:向步骤一中的混合液中加入形成水凝胶的反应单体,经水热反应陈化为复合水凝胶粘结剂;
步骤三:将步骤二中复合水凝胶粘结剂和载体材料、辅助粘结剂和增粘剂等按比例造粒成型,所得颗粒依次经过干燥,惰性气体保护下的煅烧碳化,最终制得用于电催化氧化反应的粒子电极电催化填料,优选的颗粒形貌为直径3.4-6.0mm、长度10-20mm的的圆柱、拉西环、三叶草和蝶形颗粒中的一种。
优选的,步骤一中,所述多组分金属盐溶液使用金属钨、钒、锡、镉和锑的硫酸盐,盐酸盐,硝酸盐和酒石酸盐中至少一种,较为特殊的是硼酸的钠盐,所述溶剂为去离子水,金属盐的固含量为5-30wt%,所述混合液的配置方法是向多组分金属盐溶液加入氧化石墨烯的粉体、质量分数为10-30%的溶液其中一种,该混合液所用的溶剂是无水乙醇、乙二醇、异丙醇和叔丁醇中的一种。
所述质量分数为10-30%的溶液的溶剂为去离子水,无水乙醇,丙醇、丙酮、聚乙烯醇中的一种或几种的混合物
优选的,所述步骤一中混合液的分散助剂为阴离子、阳离子、非离子表面活性剂其中一种,具体为阳离子表面活性剂烷基三甲基卤化铵、烷基二甲基苄基卤化铵,阴离子表面活性剂烷基苯磺酸盐、α-烯烃磺酸盐,脂肪酸磺烷基酯,非离子表面活性剂长链脂肪醇聚氧乙烯醚、烷基酚聚氧乙烯醚、脂肪酸聚氧乙烯酯中的一种,优选的阳离子表面活性剂为十六烷基三甲基溴化铵CTAB,阴离子表面活性剂为十二烷基苯磺酸钠SDBS和非离子表面活性剂山梨醇单油酸酯聚氧乙烯醚Tween-80。
混合液的分散方法为机械搅拌或超声乳化,获得的混合液为悬浮液或乳液的分散形式。
优选的,所述步骤二中的水凝胶为有机水凝胶,具体为水溶性酚醛树脂,聚丙烯酰胺和聚酰亚胺中的一种。
优选的,所述水溶性酚醛树脂,其反应体系为苯酚、间苯二酚、2氯-间苯三酚,儿茶酚单体,在碱性和有机酸其中一种催化剂的作用下,与甲醛和糠醛在室温至120℃条件下,老化6-48h,最终得到复合酚醛树脂水凝胶粘结剂。其中碱性催化剂包括碳酸钠,碳酸铵,碳酸氢铵,乙酸铵和氢氧化铵中的一种或多种。有机酸催化剂包括甲酸、乙酸、丙酸、马来酸、草酸、尿酸和乳酸中的一种或多种。溶剂为去离子水,乙醇,乙二醇的一种或多种。酚类单体的醛基官能团和催化剂的摩尔比为(20-200):1,醛基官能团:酚类单体的酚基官能团的摩尔比为1:1.02-1.10,单体与溶剂总量的质量比为1:(4-10)。
优选的,所述聚丙烯酰胺水凝胶,其反应体系为氧化石墨烯还原剂水合肼,硼氢化钠,抗坏血酸中的一种,反应单体丙烯酰胺,交联剂甲叉双丙烯酰胺和N,N-亚甲基双丙烯酰胺中的一种,在催化剂N,N,N',N'-四甲基乙二胺和过硫酸钾作用下,经30-120℃条件水热反应3-24h,最终得到复合聚丙烯酰胺水凝胶。所述氧化石墨烯和还原剂的质量比为(2-8):1,所述丙烯酰胺和所述氧化石墨烯的质量比为(4~20):1;所述丙烯酰胺、N,N-亚甲基双丙烯酰胺和过硫酸钾的摩尔比为100:(1-5):(0.1-1)。单体与溶剂质量比为1:(5-20)。
优选的,所述的聚酰亚胺水凝胶,其反应体系为二元胺单体、与二元酸酐,在极性溶剂中和冰水浴条件下反应生成聚酰胺酸预聚体,预聚体溶液在水中沉析得到固体,再在去离子或混合溶液(混合溶剂中水和乙醇的质量比为100:1~20与混合溶剂的质量比为1:0.5~1:10~20)中与有机胺或吡啶反应,经70-100℃条件下进行1-12h的溶胶-凝胶反应生成水溶性聚酰胺酸盐水凝胶,即聚酰亚胺水凝胶的预聚体,经后续干燥和煅烧工艺完成亚胺化处理过程。所述二元胺单体为4,4'-二氨基二苯醚,3,5-二氨基苯甲酸,3,3'-二氨基-4,4'-二羟基二苯砜,1,3-双(4-氨基苯氧基)苯中的一种。所述的二元酸酐为3,3',4,4'-联苯四羧酸二酐,3,3',4,4'-二苯基砜四羧酸二酸,3,3',4,4'-二苯甲酮四甲酸二酐,吡嗪-2,3,5,6-四甲酸二酐中的一种。所述的有机胺为三乙胺,N-甲基二乙醇胺和三乙醇胺中的一种。所述的混合溶剂为水、N-甲基吡咯烷酮、二甲基乙酰胺的一种或多种。所述的二元胺:二元酸酐摩尔比为1:1,单体与混合溶剂的质量比为1:(4-10)。预聚体聚酰胺酸、有机胺和去离子水的质量比为1:(0.5-1):(4-20)。
优选的,所述步骤三中,载体材料为300目以上、碘值1200以上,灰分在8%以下的椰壳、果壳或经深度酸洗的煤制活性炭粉末,所述辅助粘结材料为铝溶胶、硅溶胶、高岭土膨润土中的一种,以及羟甲基纤维素和田菁粉增粘剂中的一种,辅助粘结剂和增粘剂的添加量为固体总量的10-20%和1-4%,所述成型造粒方法为液压挤出、螺杆挤出或液压压片造粒方法中的一种,成型后干燥条件为80-120℃,120-240分钟,干燥后颗粒的煅烧条件为N2、CO2气氛保护,或水蒸气活化的条件下,经750-950℃条件下碳化处理120-240分钟;冷却后最终得到粒子电极。
一种粒子电极电催化填料使用方法,将上述的电极电催化填料辅以15-30%体积的惰性颗粒,诸如陶瓷、石英砂和活性氧化铝颗粒,组成复性填料装填在二维平板电极板之间,形成三维形稳粒子电极,装填量为极板高度的50-70%,电催化氧化反应使用恒流的供电方式,电流密度为10-30mA/cm2,采用从下至上的溢流进水方式,采用垂直于二维电极板的过流接触方式,反应时间为30-240min,适用于COD>2000mg/L,NH4-N<1500mg/L,有机氯化物<1000mg/L和电导率1-10ms/cm的废水
与现有技术相比,本发明一种粒子电极电催化填料制备方法和使用方法,具有以下优点:
1、污染物去除的增益效果十分显著,这是由于降解有机物的氧化还原电化学反应不受限于二维主电极表面附近,同时发生在三维粒子电极表面,电化学反应位点及反应微界面更加丰富。
2、通过对三维电极材料的配方设计及材料改性,可调控污染物向反应位点富集,实现目标污染物的定向传质,可定向增益诸如极性/非极性和偏酸碱性种类污染物的去除效果。
3、原水电导率较低时,减少甚至无需额外投加溶解性硫酸钠,氯化钠等增强电导率的电解质,避免了二次污染,有效降低设备功率,节能降耗。
4、在处理COD浓度>5000mg/L,[NH4 +-N]>2000mg/L,[有机氯化物]>1500mg/L的废水时增益效果优势明显,去除率>75%,效果优于二维平板电极25-50%以上,有效降低设备体积,即投资成本。另外,恒流供电方式下,运行功率可降低10-25%,即运行成本。
附图说明
附图用来提供对本发明的进一步理解,并且构成说明书的一部分,与本发明的实施例一起用于解释本发明,并不构成对本发明的限制,在附图中:
图1为传统平板电极填充粒子电极进行电催化氧化处理废水中的污染物;
图2为实施例#1-3中平板电极v.s.粒子电极电催化氧化反应产水水质对比本发明的结构示意图;
图3为实施例#1-3中经平板电极和粒子电极处理COD去除率随时间变化;
图4为实施例#1-3中经平板和粒子电极处理氨氮、有机氯化物去除率随时间变化。
具体实施方式
下面将结合本发明实施例中的附图,对本发明实施例中的技术方案进行清楚、完整地描述,显然,所描述的实施例仅仅是本发明一部分实施例,而不是全部的实施例。基于本发明中的实施例,本领域普通技术人员在没有做出创造性劳动前提下所获得的所有其他实施例,都属于本发明保护的范围。
为评测本专利中所述的粒子电极催化剂对电催化氧化反应的增益效果,采用两组平板钌铱钛网状阳极和两组钛网阴极作为工作电极,电极规格为100mmх50mm,极板间距为120mm,反应器容积为300mL,极板间填充50-60%的粒子电极和惰性粒子,粒子电极与惰性粒子的体积比为(2-4):1。
实施案例1:
(1)混合液的制备:氯化锡、氯化钨、氧化石墨烯和分散剂十二烷基苯磺酸钠的投料质量比2:1:4:0.05,混合金属盐总量与溶剂的质量比为1:5,经60-150rpm机械搅拌15分钟-1小时,最终分散成的混合液即配即用,贮存时间(pot-life)不超过2h;
(2)酚醛树脂水凝胶的制备:向上述混合液中加入摩尔浓度比1:2.2:0.02的间苯二酚、甲醛单体和碳酸钠催化剂,单体的总固含量为溶剂的50%,经70℃水热陈化24h,如遇溶液变得特别粘稠则补充水和乙醇1:1的混合溶液,之后以10%的醋酸水溶液进行酸化反应6h,最终得到气凝胶前躯体,复合水凝胶粘结剂;
(3)成型造粒的工艺条件:步骤(2)中的酚醛树脂的理论固含量,木质活性炭粉体,40wt%铝溶胶,高粘度田菁粉的质量比为1:5:0.5:0.05,制成直径3.4mm,长度6-12mm,三叶草形貌的颗粒,经70℃,6h干燥。
(4)煅烧条件:步骤(3)所得干燥颗粒经回转炉在N2惰性气体保护下经850℃煅烧2h,炉体出料端设置外加水冷的惰性气体保护容器中,进行隔氧强制降温,出料温度低于100℃且不复燃,经ASTM E11标准中规定的6目和10目直线振动筛筛分后,取筛上料为最终产品,可用于电催化氧化反应的粒子电极填料。
本实施例中的粒子电极电催化氧化反应原水,采用山西某煤制醇生产企业水处理系统中的膜系统进水,原水具有深黄色度,其他水质指标参见附图2中表格,电催化氧化反应采用恒流供电模式,电流密度10mA/cm2,水力停留时间为2h,产水色度基本褪去,主要污染物去除率均大于80%,具体为COD<500mg/L,NH4-N<50mg/L和有机氯化物<25mg/L。
实施案例2:
(1)混合液的制备:氯化锡、酒石酸锑钾、氧化石墨烯和分散剂Tween-80的投料质量比1:1:3:0.02,混合金属盐总量与溶剂(体积比1:1的水和乙醇)的质量比为1:10,在冷水浴下经超声分散15分钟,最终分散成的混合液即配即用,贮存时间(pot-life)不超过2h;
(2)聚丙烯酰胺水凝胶的制备:在冷水浴和机械搅拌条件下,向步骤(1)中的混合液中加入抗坏血酸还原剂,丙烯酰胺,交联剂N,N-亚甲基双丙烯酰胺和过硫酸钾,上述原料与步骤(1)中氧化石墨烯质量比为1:5:0.1:0.02:2,搅拌120min的到混合溶液,后经80℃水热反应60min,即得到聚丙烯酰胺水凝胶。
(3)成型造粒的工艺条件:步骤(2)中的聚丙烯酰胺树脂的理论固含量,椰壳活性炭粉体,30wt%硅溶胶,羟甲基纤维素的质量比为1:8:2:0.05,制成直径4mm,长度6-12mm,圆柱形貌的颗粒,经70℃,6h干燥。
(4)煅烧条件:步骤(3)所得干燥颗粒经回转炉在N2惰性气体保护下经950℃煅烧3h,炉体出料端设置外加水冷的惰性气体保护容器中,进行隔氧强制降温,出料温度低于100℃且不复燃,经ASTM E11标准中规定的8目和12目直线振动筛筛分后,取筛上料为最终产品,可用于电催化氧化反应的粒子电极填料。
本实施例中的粒子电极电催化氧化反应原水,采用某垃圾渗沥液废水处理系统生化产水作为系统进水,添加相当于1000mg/L的NaCl和NaSO4电解质以提升电导率,其他水质指标参见附图2中表格,电催化氧化反应采用恒流供电模式,电流密度5mA/cm2,水力停留时间为2h,产水基本无色度,主要污染物去除率均大于80%,具体为COD<200mg/L,NH4-N<300mg/L和有机氯化物<20mg/L。
实施案例3:
(1)混合液的制备:氯化锡、硼酸钠,氯化物、氧化石墨烯和分散剂CTAB的投料质量比1:1:1:5:0.16,混合金属盐总量与溶剂(体积比1:4的水和二甲基乙酰胺)的质量比为1:4,在冷水浴下经超声分散15分钟,最终分散成的混合液即配即用,贮存时间(pot-life)不超过2h;
(2)聚酰亚胺水凝胶的制备:在冷水浴和机械搅拌条件下,二元胺3,3'-二氨基-4,4'-二羟基二苯砜和二元酸酐3,3',4,4'-联苯四羧酸二酐溶解于有机溶剂二甲基乙酰胺,在冷水浴条件下反应24h生成聚酰胺酸预聚体,将上述预聚体溶液在去离子水中沉析,并用过量去离子水冲洗2-3遍,收集抽滤后固体。所获得固体在去离子水和乙二醇2:1的混合溶剂中与有机胺三乙胺反应,经100℃,12h水热反应生成水溶性的聚酰胺酸盐水凝胶溶液。
(3)步骤(2)中反应单体二元胺和二元酸酐的摩尔比为1:1,反应单体与溶剂二甲基乙酰胺的质量比为1:10。聚酰胺酸预聚体、三乙胺和混合溶液的质量比为1:0.5:5。
(4)成型造粒的工艺条件:步骤(1)中的混合液,步骤(2)中的聚酰胺酸混合液,木质活性炭粉体,40wt%的铝溶胶,高粘度田菁粉的质量比为1:1:10:0.02,制成直径4mm,长度6-12mm,蝶形形貌的颗粒,经70℃,6h干燥。
(5)煅烧条件:步骤(3)所得干燥颗粒经回转炉在N2惰性气体保护下经950℃煅烧3h,炉体出料端设置外加水冷的惰性气体保护容器中,进行隔氧强制降温,出料温度低于100℃且不复燃,经ASTM E11标准中规定的8目和12目直线振动筛筛分后,取筛上料为最终产品,可用于电催化氧化反应的粒子电极填料。
本实施例中的粒子电极电催化氧化反应原水,采用某脱硫脱硝废水水处理膜系统进水,水质特征为COD、氨氮含量均较高,其他水质指标参见附图2中表格,电催化氧化反应采用恒流供电模式,电流密度20mA/cm2,水力停留时间为3h,产水基本无色度,主要污染物去除率均大于70%,具体为COD<1000mg/L,NH4-N<100mg/L和有机氯化物<100mg/L。
尽管已经示出和描述了本发明的实施例,对于本领域的普通技术人员而言,可以理解在不脱离本发明的原理和精神的情况下可以对这些实施例进行多种变化、修改、替换和变型,本发明的范围由所附权利要求及其等同物限定。
Claims (10)
1.一种粒子电极电催化填料制备方法,其特征在于,包括以下步骤:
步骤一:配置一定浓度的多组分金属盐溶液,并向该溶液中投加氧化石墨烯、分散助剂和溶剂,并分散成混合液;
步骤二:向步骤一中的混合液中加入形成水凝胶的反应单体,经水热反应陈化为复合水凝胶粘结剂;
步骤三:将步骤二中复合水凝胶粘结剂和载体材料、辅助粘结剂和增粘剂等按比例造粒成型,所得颗粒依次经过干燥,惰性气体保护下的煅烧碳化,最终制得用于电催化氧化反应的粒子电极电催化填料。
2.根据权利要求1所述一种粒子电极电催化填料制备方法,其特征在于:步骤一中,所述多组分金属盐溶液使用金属钨、钒、锡、镉和锑的硫酸盐,盐酸盐,硝酸盐和酒石酸盐中至少一种,所述溶剂为去离子水,金属盐的固含量为5-30wt%,所述混合液的配置方法是向多组分金属盐溶液加入氧化石墨烯的粉体、质量分数为10-30%的溶液其中一种。
3.根据权利要求2所述一种粒子电极电催化填料制备方法,其特征在于:所述质量分数为10-30%的溶液的溶剂为去离子水,无水乙醇,丙醇、丙酮、聚乙烯醇中的一种或几种的混合物。
4.根据权利要求1所述一种粒子电极电催化填料制备方法,其特征在于:所述步骤一中混合液的分散助剂为阴离子、阳离子、非离子表面活性剂其中一种。
5.根据权利要求1所述一种粒子电极电催化填料制备方法,其特征在于:所述步骤二中的水凝胶为有机水凝胶,具体为水溶性酚醛树脂,聚丙烯酰胺和聚酰亚胺中的一种。
6.根据权利要求5所述一种粒子电极电催化填料制备方法,其特征在于:所述水溶性酚醛树脂,其反应体系为苯酚、间苯二酚、2氯-间苯三酚,儿茶酚单体,在碱性和有机酸其中一种催化剂的作用下,与甲醛和糠醛在室温至120℃条件下,老化6-48h,最终得到复合酚醛树脂水凝胶粘结剂。
7.根据权利要求5所述一种粒子电极电催化填料制备方法,其特征在于:所述聚丙烯酰胺水凝胶,其反应体系为氧化石墨烯还原剂水合肼,硼氢化钠,抗坏血酸中的一种,反应单体丙烯酰胺,交联剂甲叉双丙烯酰胺和N,N-亚甲基双丙烯酰胺中的一种,在催化剂N,N,N',N'-四甲基乙二胺和过硫酸钾作用下,经30-120℃条件水热反应3-24h,最终得到复合聚丙烯酰胺水凝胶。
8.根据权利要求5所述一种粒子电极电催化填料制备方法,其特征在于:所述的聚酰亚胺水凝胶,其反应体系为二元胺单体、与二元酸酐,在极性溶剂中和冰水浴条件下反应生成聚酰胺酸预聚体,预聚体溶液在水中沉析得到固体,再在去离子或混合溶液中与有机胺或吡啶反应,经70-100℃条件下进行1-12h的溶胶-凝胶反应生成水溶性聚酰胺酸盐水凝胶,即聚酰亚胺水凝胶的预聚体,经后续干燥和煅烧工艺完成亚胺化处理过程。
9.根据权利要求1所述一种粒子电极电催化填料制备方法,其特征在于:所述步骤三中,载体材料为300目以上、碘值1200以上,灰分在8%以下的椰壳、果壳或经深度酸洗的煤制活性炭粉末,所述辅助粘结材料为铝溶胶、硅溶胶、高岭土膨润土中的一种,以及羟甲基纤维素和田菁粉增粘剂中的一种,辅助粘结剂和增粘剂的添加量为固体总量的10-20%和1-4%,所述成型造粒方法为液压挤出、螺杆挤出或液压压片造粒方法中的一种,成型后干燥条件为80-120℃,120-240分钟,干燥后颗粒的煅烧条件为N2、CO2气氛保护,或水蒸气活化的条件下,经750-950℃条件下碳化处理120-240分钟;冷却后最终得到粒子电极。
10.根据权利要求1所述一种粒子电极电催化填料使用方法,其特征在于:将权利要求1-9任意一项所述的电极电催化填料辅以15-30%体积的惰性颗粒,组成复性填料装填在二维平板电极板之间,形成三维形稳粒子电极,装填量为极板高度的50-70%,电催化氧化反应使用恒流的供电方式,电流密度为10-30mA/cm2,采用从下至上的溢流进水方式,采用垂直于二维电极板的过流接触方式,反应时间为30-240min,适用于COD>2000mg/L,NH4-N<1500mg/L,有机氯化物<1000mg/L和电导率1-10ms/cm的废水。
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