CN105793474B - 配备有同轴电极对的电解槽 - Google Patents

配备有同轴电极对的电解槽 Download PDF

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CN105793474B
CN105793474B CN201480064850.6A CN201480064850A CN105793474B CN 105793474 B CN105793474 B CN 105793474B CN 201480064850 A CN201480064850 A CN 201480064850A CN 105793474 B CN105793474 B CN 105793474B
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CN105793474A (zh
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M·贝纳德托
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Industrie de Nora SpA
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Abstract

本发明涉及对于伴随周期性的极性反转而进行的电化学工艺特别有用的双极电解槽。该槽配备有一系列的同轴电极对，最内部的对和最外部的对与DC发生器的极连接并且中间对充当双极电极。以这样的方式布置和连接不同的电极对：使得在工艺的各个阶段，总的阴极面积等于阳极面积。

Description

配备有同轴电极对的电解槽
技术领域
本发明涉及双极型电化学槽并且涉及在其中进行电解工艺的方法。
背景技术
本发明涉及适合于伴随周期性的极性反转而进行的电化学工艺的双极电解槽。电化学槽的周期性极性反转(由此每个电极交替地作为阳极和作为阴极工作持续预设定的时间间隔)是本领域中已知的特别是用于防止在电极之一(通常为阴极)的表面上形成各种类型的结垢的措施。上述例如是用于电解稀释的碱性盐水以在阳极处制备活性氯的槽的典型情况(即，次氯酸盐和次氯酸与可能的痕量的溶解游离氯和平衡的其它物质的混合物)：特别是在由含有碳酸根离子和类似行为的其它阴离子的自来水获得盐水的情况下，阴极变成碳酸盐和其它不可溶性盐的优先沉积位点，这受到附近的过程诱发的碱化的支持。这样的沉积物不利地影响通过电极的电流输送，电极的电效率可最终不可逆地劣化。电流方向并且因此电极极性的周期性反转使得表面阴极性地工作半个循环以在反转时开始充当阳极，经受有利于先前形成的沉淀物的溶解的局部酸化。有时经受周期性电流反转的其它电解工艺例如为含有有机物质的废水的处理，在阳极处降解所述有机物质而在阴极处倾向于形成各种类型的沉积物；或者由电解浴阴极沉积金属并且同时阳极降解有机物，用于处理其中两种类型的物质作为杂质存在的水。在这样的情况下，阳极还经常经受污染膜的沉积，在这种情况下，该污染膜由有机残余物组成，该有机残余物倾向于在电极表面上低聚合，并且有时可通过随后的阴极循环中的初生氢的机械和化学作用被移除。为了保护操作的规则性和维持所需的工艺的操作参数恒定，指定交替作为阳极和作为阴极工作的安装在槽中电极，除了以恒定间隙隔开以外，还必须优选具有相同的尺寸，使得可以保持供应的电流和操作电压两者恒定(除了符号的变化)。这意味着用于这种类型的工艺的槽设计主要限于平坦型几何形状，换句话说考虑面向的平坦电极对的使用。然而，在许多情况下，这可构成不需要的限制，包括一些负面的结果。在许多情况下，事实上在小尺寸装置中进行这种类型的工艺，例如将要用于医院、旅馆或家庭领域的水的消毒或在珠宝废物中贵金属的回收的情况。对于这样类型的应用，尽可能多地限制体积，选择共轴同轴型的槽设计(例如具有外阴极壁和中央阳极的柱形槽)可为重要的。除了较好地利用可用体积以外，这还可具有改进电流输送最小化边缘效应的优点，已知该电流输送最小化边缘效应在平坦几何形状中较重并且在小尺寸的总体积电极面积的情况下是非常相关的。然而共轴同轴型的槽(圆柱形或棱柱形两者)的特征在于具有比内部电极大的尺寸的外部电极，使得采用周期性电流反转的操作更加困难。事实上保持一次循环和下一次循环之间的电流密度恒定并且因此制备所需的物质，相应的电极面积的变化会引起电流密度的相应变化以及因此工艺电压的相应变化；另一方面，应该决定在恒定电压下操作，电流密度以及因此生产率会在对应于两个不同电极面积的两个值之间振荡，几乎不与工业工艺的正常要求一致。
因此确定了对于提供同轴电极几何形状的电解槽的需求，该电解槽具有恒定的电极间间隙并且具有与阳极面积相同的阴极面积。
发明内容
在一个方面，本发明涉及双极电解槽，该双极电解槽由外部体壳体限定，在其内部具有：
－划分成两个电极的外部电极对，该两个电极通过隔离元件在边缘处分隔，指定以交替地操作一个电极作为阴极并且另一个电极作为阳极，并且反之亦然；
－与其同轴的至少一个中间电极对，从而在其间限定大体上恒定的宽度的第一间隙，该至少一个中间电极对也划分成两个电极，两个电极通过隔离元件在边缘处分隔，不直接供应电流并且旨在作为双极元件操作；
－与前两者同轴的内部电极对，从而限定与该中间电极对的大体上恒定的宽度的第二间隙；该内部电极对也划分成两个电极，两个电极通过隔离元件在边缘处分离，指定以交替操作一个电极作为阴极并且另一个电极作为阳极，并且反之亦然，该对的两个电极的每个面向该中间对的两个电极之一；
－将该外部对的电极之一和不面向该中间对的电极的进而面向其的该内部对的相应电极与槽极之一电连接的装置；
－将两个内部和外部对的剩余电极与槽的另一个极电连接的装置。
在一个实施方案中，外部槽体具有狭长形形状并且电极对具有棱柱形或圆柱形形状。
在另一个实施方案中，外部槽体和该电极对具有类球形形状。
在一个实施方案中，存在适应于作为双极元件操作的更多的中间电极对，以便增加槽的产率。
在以这样的方式构造的槽中，阳极面积和阴极面积对应于外部电极对的一半和内部电极对的一半的面积总和：通过使电极极性反转，阳极和阴极面积的值没有改变。
在一个实施方案中，槽体和电极对均具有棱柱形或圆柱形形状。例如将圆柱形槽体与也是圆柱形的电极对结合以使没有参与电解反应的槽体积最小化。在一个实施方案中，两个同轴电极对与槽体共轴。这还可具有使没有参与电解反应的槽体积最小化的优点。在一个实施方案中，槽的所有电极均由钛或其它阀金属制成，所述钛或其它阀金属涂覆有含有一种或多种选自铂组的组分例如铂金属或铂、钌或铱的氧化物的催化组合物。在一个实施方案中，上面的催化组合物还包含能够有利于紧密和保护性的膜的生长的氧化物，例如钛、钽、铌或锡的氧化物。在本申请文件的上下文中，术语由钛或阀金属制成的电极用于表明从要么纯的要么不同合金化的钛或其它阀金属(例如铌、钽或锆)的基材开始而获得的电极。
在一个替代性的实施方案中，槽的所有电极均由要么处于块体形式要么承载于合适的传导基材(例如铌或其它阀金属)上的传导金刚石(例如硼掺杂的金刚石)制成。
对于绝大多数已知的阳极应用而言，指定的材料具有以优化的方式工作的优点，包括阳极产物例如氯、氧、臭氧或过氧化物的析出，与此同时保证还作为阴极的恰当功能化。
在一个实施方案中，如对于本领域技术人员将清楚的是，取决于每个工艺的需要，第一间隙和第二间隙具有独立地在1和20mm之间的大体上恒定的宽度。
在另一方面，本发明涉及执行电解工艺的方法，包括在如上文所述的电解槽的间隙内供给工艺电解质并且向槽极供应直流电流，以预设定的时间间隔、例如每1－120分钟改变所施加的电流的方向。在一个实施方案中，根据本发明的电解工艺由电解盐溶液与制备活性氯构成。在一个替代性的实施方案中，根据本发明的电解工艺由降解有机物质的废水处理构成。在又一个实施方案中，根据本发明的电解工艺由通过阴极电沉积回收金属并且任选地同时降解有机物质构成。
现在将参考附图描述例示本发明的一些实施方式，其仅具有说明不同元件相对于本发明的所述具体实施方式的相互布置的目的；特别地，附图不必按比例绘制。
附图简要说明
图1示出了根据本发明的一个实施方案的包含圆柱体和棱柱形电极对的槽的截面的俯视图。
图2示出了根据本发明的一个实施方案的包含圆柱体和圆柱形电极对的槽的截面的俯视图。
附图详细描述
图1显示了由圆柱体100限定的槽构成的本发明的一个实施方案的截面的俯视图，在该槽内部放置三个平行六面体形电极对，即：由通过隔离元件101在边缘处分隔的电极301和401构成的内部对，由电极501和502构成的中间对，和由电极302和402构成的与内部对共轴的外部对；还通过等同的隔离元件101在边缘处分隔中间对的电极和外部对的电极。隔离元件101保持电极在固定位置，防止其短路：除了进行这些功能以外，元件101还避免电流集中在每个电极对的面向边缘处。出于这样的原因，必须适当地定制元件101的尺寸：发明人发现，对于大多数所测试的应用，定制元件101的尺寸使得每个电极对的面向边缘之间的距离至少等于各自的间隙102和112的宽度。电极402和501彼此面向，正如电极302和502一样，从而定义第一间隙102，除了拐角区域外，该第一间隙102具有大体上恒定的宽度。
类似地，电极301和501彼此面向，正如电极401和502一样，从而定义第一间隙112，除了拐角区域外，该第二间隙112具有大体上恒定的宽度。
内部对的电极301和外部对的没有面向双极电极501、进而面向相同的电极301的电极302与直流电源200的一个极300连接，该直流电源200设有用于以预设定的时间间隔使电流的方向反转的装置；类似地，内部对的另一个电极401和外部对的另一个电极402与直流电源200的另一个极400连接。槽体的两个相邻的间隙102和112之外的区域103和104填充有隔离材料，从而限制工艺电解质在构成反应区的所述间隙内。可从在相对位置上具有出口的槽体100的终端部分对槽进行供给，并且槽可任选地以采用单一道次的电解质的连续模式或者以分批模式进行工作。
图2显示了本发明的类似实施方案的截面的俯视图，其与前一个的不同之处在于电极对的圆柱形形状。除了使活性电极表面与总的槽体积之比最大化以外，这还具有保持间隙102和112的宽度恒定、消除拐角区域的优点。
在以下实施例中说明了由发明人获得的一些最显著的结果，其不旨在限制本发明的范围。
实施例
采用由含有19g/l NaCl的自来水制备的盐水溶液由相对间隙对与图2的实施方案对应的槽(不同之处在于配备有双极电极的两个中间对)进行供给。该槽配备有60mm直径外部电极对、30mm直径内部电极对和分别为50mm和40mm直径的中间双极电极对(定义宽度约4mm的间隙)。所有的电极对具有50mm的高度。各个对的所有电极由钛片材构成，该钛片材在面向间隙的一侧上采用钌、钯和钛的氧化物的混合物进行活化(根据现有技术)。对应于两个间隙的体积的总反应体积为32.5ml。在施加5A的总电流(对应于在内电极组合上约1kA/m2和在外电极组合上0.5kA/m2的电流密度)时，和在每180秒使电流流动的方向反转时，可以在一系列的分批循环(每次持续60分钟)的过程中以66％的恒定效率制备2700ppm的活性氯。
重复该测试，施加10A的总电流，总是采用每180秒的电流反转在60分钟的分批循环中操作，导致了以68％的恒定效率制备5530ppm的活性氯。在该第二测试期间，观察到pH从初始的中性增加到高达9.6的值。
上述描述不应该旨在限制本发明，可以根据不同的实施方案来使用本发明而不脱离其范围，并且其程度仅由所附权利要求书限定。
贯穿本申请的说明书和权利要求书，术语"包含(comprise)"以及其变体例如"含有(comprising)"和"包括(comprises)"并非旨在排除其它元件、组分或者附加的工艺步骤的存在。
在本申请文件中包括对文件、法案、材料、装置、制品以及类似物的讨论仅是出于为本发明提供上下文的目的。并不暗示或者表示这些物件中的任何或者全部在本申请的每一项权利要求的优先权日期之前形成了现有技术基础的一部分或者是与本发明相关的领域中的公知常识。

Claims (10)

1.双极电解槽，该双极电解槽由狭长形或类球形形状壳体的外部体限定，在其内部具有：
－外部电极对；
－内部电极对；
－至少一个中间电极对，
所述外部电极对划分成通过第一隔离元件在边缘处分隔的相同尺寸的第一外部电极和第二外部电极，所述内部电极对划分成通过第二隔离元件在边缘处分隔的相同尺寸的第一内部电极和第二内部电极，所述至少一个中间电极对划分成通过第三隔离元件在边缘处隔离的相同尺寸的第一中间电极和第二中间电极，所述内部电极对、外部电极对和中间电极对同轴设置，且所述第一外部电极和所述第一中间电极的表面以及所述第二外部电极和所述第二中间电极的表面面向彼此从而限定第一间隙，所述第一中间电极和所述第一内部电极的表面以及所述第二中间电极和所述第二内部电极的表面面向彼此从而限定至少一个第二间隙，所述第一外部电极和所述第二内部电极与该槽的一个极连接，所述第二外部电极和所述第一内部电极与该槽的相对极连接。
2.根据权利要求1的槽，其中所述外部电极对、中间电极对和内部电极对是置于狭长形形状的体内部中的圆柱形或棱柱形形状的电极对或者置于类球形体的内部中的类球形形状的电极对。
3.根据权利要求2的槽，其中所述外部电极对、所述至少一个中间电极对和所述内部电极对与槽体共轴。
4.根据前述权利要求中任一项的槽，其中所述第一外部电极和第二外部电极、所述第一中间电极和第二中间电极以及所述第一内部电极和第二内部电极由块体或承载形式的传导金刚石制成或者由涂覆有含有铂族的一种或多种元素的催化组合物的钛制成。
5.根据权利要求4的槽，其中所述催化组合物包含选自金属性铂、氧化铂、氧化钌和氧化铱的至少一种组分，和选自钛、钽、铌和锡的元素的至少一种氧化物。
6.根据权利要求1-3和5中任一项的槽，其中所述第一间隙和所述第二间隙具有独立地从1至20mm的恒定宽度。
7.根据权利要求4的槽，其中所述第一间隙和所述第二间隙具有独立地从1至20mm的恒定宽度。
8.在根据权利要求1至7中任一项的槽中执行电解工艺的方法，包括在所述第一间隙和所述至少一个第二间隙内供给工艺电解质并且向槽极供应直流电流，以预设定的时间间隔改变所述直流电流的方向。
9.根据权利要求8的方法，其中所述电解工艺选自：电解盐溶液与制备活性氯，通过电解废水来降解有机物质，和通过阴极电沉积来回收金属并且任选同时降解有机物质。
10.根据权利要求8或9的方法，其中所述预设定时间间隔具有1至120分钟的持续时间。
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KR20160093650A (ko) 2016-08-08
BR112016009720B1 (pt) 2021-10-13
EA201691158A1 (ru) 2016-09-30
AU2014359318B2 (en) 2018-08-02
EP3077577A1 (en) 2016-10-12
HK1221268A1 (zh) 2017-05-26
US10023966B2 (en) 2018-07-17
EP3077577B1 (en) 2018-02-07
ES2663499T3 (es) 2018-04-13
JP6511053B2 (ja) 2019-05-08
EA030848B1 (ru) 2018-10-31
JP2017503916A (ja) 2017-02-02
WO2015082527A1 (en) 2015-06-11
BR112016009720A2 (zh) 2017-08-01
MX2016005653A (es) 2016-08-11
TW201522715A (zh) 2015-06-16
US20160251763A1 (en) 2016-09-01
IL245083B (en) 2019-01-31
KR102277620B1 (ko) 2021-07-19
ITMI20132015A1 (it) 2015-06-04
IL245083A0 (en) 2016-06-30
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MX357177B (es) 2018-06-28

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