CN114391052A - 制氢装置 - Google Patents
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- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 37
- 239000001257 hydrogen Substances 0.000 title claims abstract description 33
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 33
- 238000004519 manufacturing process Methods 0.000 title claims description 12
- 239000003011 anion exchange membrane Substances 0.000 claims abstract description 24
- 239000007788 liquid Substances 0.000 claims abstract description 20
- 239000012528 membrane Substances 0.000 claims abstract description 18
- 229920000554 ionomer Polymers 0.000 claims abstract description 14
- 239000011230 binding agent Substances 0.000 claims abstract description 13
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 11
- 239000001301 oxygen Substances 0.000 claims abstract description 11
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 11
- 239000003054 catalyst Substances 0.000 claims description 22
- 229920000642 polymer Polymers 0.000 claims description 16
- -1 transition metal sulfides Chemical class 0.000 claims description 15
- 238000006243 chemical reaction Methods 0.000 claims description 9
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- 229910052723 transition metal Inorganic materials 0.000 claims description 8
- 229910052799 carbon Inorganic materials 0.000 claims description 7
- 125000000524 functional group Chemical group 0.000 claims description 7
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 6
- 150000003624 transition metals Chemical class 0.000 claims description 6
- 238000004132 cross linking Methods 0.000 claims description 5
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- 229910052751 metal Inorganic materials 0.000 claims description 4
- 239000002184 metal Substances 0.000 claims description 4
- 125000006850 spacer group Chemical group 0.000 claims description 4
- 229910000314 transition metal oxide Inorganic materials 0.000 claims description 4
- 239000004693 Polybenzimidazole Substances 0.000 claims description 3
- 239000004698 Polyethylene Substances 0.000 claims description 3
- 239000004721 Polyphenylene oxide Substances 0.000 claims description 3
- 239000004793 Polystyrene Substances 0.000 claims description 3
- 150000004770 chalcogenides Chemical class 0.000 claims description 3
- 150000001875 compounds Chemical class 0.000 claims description 3
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- 150000004714 phosphonium salts Chemical class 0.000 claims description 3
- 229920002480 polybenzimidazole Polymers 0.000 claims description 3
- 229920000573 polyethylene Polymers 0.000 claims description 3
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- QGZKDVFQNNGYKY-UHFFFAOYSA-O Ammonium Chemical compound [NH4+] QGZKDVFQNNGYKY-UHFFFAOYSA-O 0.000 claims 1
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical group [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims 1
- RWSOTUBLDIXVET-UHFFFAOYSA-O sulfonium Chemical compound [SH3+] RWSOTUBLDIXVET-UHFFFAOYSA-O 0.000 claims 1
- 238000005868 electrolysis reaction Methods 0.000 abstract description 7
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 20
- 230000003204 osmotic effect Effects 0.000 description 5
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 4
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- WMFOQBRAJBCJND-UHFFFAOYSA-M Lithium hydroxide Chemical compound [Li+].[OH-] WMFOQBRAJBCJND-UHFFFAOYSA-M 0.000 description 2
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- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical class S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 1
- 125000001931 aliphatic group Chemical group 0.000 description 1
- 150000001447 alkali salts Chemical class 0.000 description 1
- 125000003118 aryl group Chemical group 0.000 description 1
- 150000005323 carbonate salts Chemical class 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
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- 239000003337 fertilizer Substances 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 239000011256 inorganic filler Substances 0.000 description 1
- MRELNEQAGSRDBK-UHFFFAOYSA-N lanthanum oxide Inorganic materials [O-2].[O-2].[O-2].[La+3].[La+3] MRELNEQAGSRDBK-UHFFFAOYSA-N 0.000 description 1
- 239000011244 liquid electrolyte Substances 0.000 description 1
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- 235000020679 tap water Nutrition 0.000 description 1
- 230000007704 transition Effects 0.000 description 1
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Abstract
本发明涉及一种由含水液体电解制氢和氧的装置,该装置包括:一阳极半电池(3)和一阴极半电池(4)以及位于两个半电池之间的一阴离子交换膜(9),其包含阳极电极,半电池(3,4)的电极(7,8)与阴离子交换膜(9)形成膜电极组件(MEA)。还包含用于将含水液体仅供给至阳极半电池(3)和阴极半电池(4)中的一个的装置(2),其中,另一个基本上干燥的半电池中的电极不含离聚物和/或不含粘合剂。
Description
技术领域
本发明涉及一种制氢装置,尤其是但并不限于利用可再生能源的电解槽。
背景技术
从能量存储到肥料生产,氢有广泛的用途。氢可以从许多来源获得。由于显而易见的原因,其中一些来源,例如化石燃料,是不期望的。因此,需要能够以可靠和可持续的方式制氢。
电解槽是用于通过分解水产生氢气和氧气的装置。例如,可以使用富余的可再生能源为此类设备供能,使用氢作为能量存储手段而不是电池。
电解槽通常采用目前可用的三种主要技术之一,即阴离子交换膜(AEM,anionexchange membrane)、质子交换膜(PEM,proton exchange membrane)和液体碱性系统(liquid alkaline systems)。液体碱性系统是最成熟的技术,PEM在某种程度上已经成熟。AEM电解槽是一项相对较新的技术。其他技术,例如固体氧化物电解也具有可行性。
AEM和PEM电解槽依赖于将离子从一个半电池(half-cell)转移到另一个以产生氢气。AEM系统依赖于氢氧根离子OH-的运动,而PEM系统依赖于氢离子H+的运动。
AEM电解槽中的半反应(half-reactions)如下:
阳极:4OH- → 2H2O + 4e- + O2
阴极:4H2O + 4e- → 2H2 +4OH-。
AEM和PEM系统的膜分别包含阳离子和阴离子,以促进OH-或H+的移动。通常,膜电极组件(MEA,membrane electrode assembly)包含离聚物(ionomer)和/或粘合剂以改善组件的性能,例如导电性、机械强度和热稳定性。粘合剂的添加可用于保持电极组件的完整性,而离聚物有助于在没有液体电解质的情况下,增加作为固体电解质工作的可用的催化剂层厚度,并通过形成基材、离聚物和电催化剂的聚集体帮助创建三相边界点。离聚物和/或粘合剂的添加会增加成本,并且可能导致性能降低,例如,在某些情况下,离聚物可能会降低耐久性,而粘合剂会影响导电性。
发明内容
本发明的目的是提供一种改进的制氢装置。
根据本发明,提供了一种由含水液体电解制氢和氧的装置,该装置包括:
一阳极半电池,其包含阳极电极,
一阴极半电池,其包含阴极电极,
一阴离子交换膜(AEM),其位于两个半电池之间,其中,
- 阳极电极、阴极电极和阴离子交换膜形成MEA,
- 包含用于将含水液体仅供给至阳极半电池和阴极半电池中的一个的装置,其中,
至少另一个基本上干燥的半电池中的电极不含离聚物和/或不含粘合剂。
如本文中所采用的,含水液体可以是任何含有水分子的溶液。由于采用AEM系统,因此溶液通常至少为轻微碱性,更优选为弱碱性至强碱性。可以通过任何合适的化合物(例如强碱、缓冲溶液……)来实现碱性。然而,在优选实施例中使用KOH。含水液体还可以包括自来水、海水,更优选为蒸馏水或去离子水。
AEM电解槽的优点之一是能够使用具有较低腐蚀性的电解液。可以设置KOH或合适的替代物的含量在1%-30%的范围内,更优选在0.1%到10%之间。更优选地,KOH为大约0.1%至5%,并且最优选地在0.2%到2%之间。虽然KOH是优选的,因为它的溶解度和其碳酸盐的溶解度可以减少与沉淀相关的问题,但也可以采用替代品,包括NaOH和LiOH。
如本文中所采用的,所指“干”半电池或基本上干的半电池是指没有直接供给液体的那个半电池。这清楚地显示在附图中。对于干阴极的情况,应该承认渗透牵引(osmoticdrag)可能会导致干半电池中暂时存在一些水,但是,正如发生的反应所示,干半电池中存在的任何水都将分解为氢和氢氧根离子。氢氧根离子迁移回阳极,同时通过电渗牵引(electroosmotic drag)带来溶剂水。
对于干阳极的情况,电渗牵引可能会移动干半电池中的氢氧根离子,产生氧气和水。形成的水通过渗透牵引迁移回阴极。在这两种情况下,暂时存在的水都不足以使该半电池不干燥。
本领域普通技术人员均熟悉电解槽的其余配套装置(BOP,balance of plant),因此,本文不对BOP进行任何深入讨论。
在优选实施例中,含水液体的pH值为7,或大于7。通常,pH值在12到14的范围内。优选地,pH范围在12.5和13.5之间,特别是pH在13和13.5之间,例如pH可以是13.25。或者,作为可能且优选的方式,可以预料该系统可使用pH为7的基本中性的液体。
根据本发明的电解槽虽然可以在很宽的温度范围内运行,但可以设置温度在40℃至80℃的范围内。更优选地在50℃到70℃的范围内,并且更优选地仍然基本上在55℃到60℃的范围内。
优选地,电解槽由可再生能源提供电源,包括但不限于太阳能、风能、水力、地热或它们的组合。也就是说,市电(mains electricity)可用于为电解槽供电。无论是由于市电价格的波动,还是由于可再生能源提供了超出电解槽用户当前负载的过剩能源,电解槽都适合以间歇方式运行。
粘合剂用于改善MEA的机械稳定性等。另一方面,没有粘合剂意味着必须确保催化层的稳定性,防止其从膜上分层并确保催化剂和膜之间的紧密接触。可以采用多种制造方法来实现这一点,包括但不限于:膜的聚合物主链(polymeric backbone)的交联(crosslinking)、使用更厚的膜、提高聚合物和催化剂之间的分子间结合力、或这些手段的组合。然而,此类措施可能会降低MEA的导电性从而影响效率。
优选地,含水液体被供给到阳极,使得阴极干燥并且产生的氢基本上干燥且不含电解质。或者,也可以将含水液体供给到电池的阴极侧,使得阳极是干燥的并且产生的氧基本上是干燥的并且没有阳极半电池电解质。
氢气通常需要在高压下提供。相应地,制氢装置可包括允许在各种升高的输出压力下产生氢气的装置。虽然氢气的输出压可以是1巴(bar),但优选地,氢气将在1巴以上的环境下制得,例如在5到50巴的范围内,更优选为30到40巴,通常在35巴,除非当地法规另有规定,例如在日本是8巴。对于车辆或其他应用,可能需要超过700巴的更高压力。在这种情况下将需要用于增加压力的压缩机或其他装置。
可以以多种方式管理氢气的预定输出压。电解槽可以有不同的氢气生产速度,但出于显而易见的原因,无论电解槽运行在何种容量下,都希望保持恒压输出。压力控制阀或等效装置在使用过程中或在电解槽不工作时是可调节的。
实际上,可以提供对输出压的限制以符合对相关地区对生产方面的限制,或者使其固定以确保符合所应用的地区对最大压强的规定。此处不讨论BOP。
虽然电解槽可工作于包括一个MEA的单个电池,但也可以使用多个电池。通常可包括10到30个电池;在优选实施例中,在一个宽度为48厘米(19英寸)的机壳中有23个电池,因此每个电池的宽度约为2厘米。也就是说,一个组合可以由两个或多个电池组装在一起构成。
阳极电极和阴极电极都可以通过多种工艺制造,例如但不限于:催化剂涂覆膜(CCM,catalyst coated membrane)、催化剂涂覆基底(CCS,catalyst coated substrate)或直接沉积(DD,direct deposition)。对于上述任何一种,都能够获得至少一种不含离聚物和/或不含粘合剂的半电池。
为了使氢气适用于高等级应用,可能需要在压缩、储存或其他用途之前对电解槽制备的氢气进行干燥。可以使用任何合适的干燥手段。
为了免除对离聚物和/或粘合剂的需要,可以将催化剂包含在DD或CCM中。可以使用催化剂涂覆基底,例如但不限于:碳基布、纸或毡、不锈钢泡沫或镍基泡沫。优选在阴极上使用碳布或纸,在阳极上使用镍泡沫或毡。基底还可以用作气体扩散层,以允许气体,即分别在阴极和阳极产生的氢气和氧气,流出。在这样的实施例中,基底应该是足够多孔的以允许含水液体和化合物在释放氢和释放氧的半反应中进行所需的扩散。
电解槽可适用于由能量监控系统,例如软件,进行监测和/或控制,从而减少对用户干预的要求。该监控系统旨在允许远程监控和控制电解槽的运行操作参数。
AEM的优点之一是能够使用不含铂族金属(PGM,platinum group metals)的催化剂。优选不使用PGM或其他稀土金属作为催化剂。与更丰富的替代品,例如过渡族金属,相比,铂族金属本质上更不可持续且成本更高。
在阳极,可以选择非化学计量的过渡金属氧化物作为合适的催化剂。阳极处的催化剂的例子包括CuCoOx。
阴极处的用于析出氢气的反应的催化剂的示例包括Ni/CeO2-La2O3/C。可以使用其他合适的非PGM阴极催化剂,包括硫属化物(chalcogenides)和烟碱类化合物(pnictogenides),例如过渡金属硫化物、过渡金属磷化物或分散在导电基材中的过渡金属,例如氮掺杂的碳或适配于具有大表面积的碳,或具有尖晶石(spinel)或钙钛矿(perovskitic)结构或过渡金属配合物的其他非化学计量的过渡金属氧化物。
所使用的任何膜需要具有这行方面的特性:机械强度、热稳定性、化学稳定性、离子导电性以及防止电子和产生的气体在半电池隔室之间穿过。
优选地,AEM由聚合物主链与适于传输阴离子,即氢氧根离子,的功能基团结合形成。聚合物包括但不限于:聚苯乙烯(polystyrene)、聚砜(polysulfone)、聚苯并咪唑(polybenzimidazole)、聚苯醚(polyphenylene oxide)、苯乙烯-丁二烯嵌段共聚物(styrene-butadiene block copolymer)、聚乙烯(polyethylene)等。聚合物主链中的交联提供了机械稳定性。下面进一步讨论功能基团。它们可以直接连接到聚合物主链上或通过作为间隔基的脂肪族或芳香族短链分隔,以促进离子导电域和主链域之间更好的相分离。聚合物主链、间隔基或离子交换基团中的交联提供了更高的机械稳定性,也有助于提高化学和热稳定性。
为了促进离子的转移,需要存在离子交换基团。合适的离子包括但不限于:铵盐(ammonium salt)、锍盐(sulfonium salt)或鏻盐(phosphonium salt)。膜的强度和热稳定性可归因于聚合物主链,而功能基团则提供离子导电性。为了本发明的目的,膜对阴离子是传导性的。
附图说明
为了帮助理解本发明,现在将通过示例并参考附图来描述其具体实施例,其中:
图1A示出了具有干阴极的AEM系统;和
图1B示出了具有干阳极的AEM系统。
具体实施方式
图1A和图1B属于本发明采用AEM的实施例。图1A显示了本发明的一个实施方案,其中水溶液基本引入到阳极侧。在此描述该实施例的典型内容。
如图1A所示,可以看到电解槽的电池1a,该电池包括阳极半电池3和阴极半电池4以及MEA 10。水溶液通过入口2被引入阳极半电池。可以是KOH的稀水溶液,也可以使用替代的碱性盐,或者,可能是纯水。向电池供电的装置是众所周知的,因此未示出;所有实施例均如此。
MEA 10包括阳极电极(或阳极)7、阴极电极(或阴极)8和阴离子交换膜9。在本发明的这个实施例中,由于入口2是通到包含阳极半电池3的隔室,不含离聚物和/或粘合剂的是阴极8。
在电池阳极侧产生的氧气通过出口5离开电池。虽然氧气可以被处理以作他用,但通常其被排出。在阴极产生的氢气通过出口6离开电池。由于渗透牵引,氢气流可能包含痕量的水,因此该气流可在压缩以储存之前经过一干燥器。在具有干阴极的实施例中,改变电流密度将影响产生的氢气的纯度。增加电流密度会增加产氢率,这意味着阴极上存在的水更少。
由于氢氧根离子迁移回阳极,同时通过电渗牵引带走溶剂水,水被进一步从阴极去除。
每个半电池中的反应如下:
阳极:4OH- → 2H2O + 4e- + O2
阴极:4H2O + 4e- → 2H2 +4OH-。
由于阴极侧没有电解液/水这一事实,产生的氢气基本上是干燥的。众所周知,由于渗透牵引,一些水可能会穿过膜,但是可以理解这是很少量的,并且不被认为会使阴极不干燥。
现在参考图1B,可以看出图1B的实施例在很大程度上类似于图1A的实施例。不同之处在于入口2通向包含阴极半电池4而不是阳极半电池3的隔室。每个半电池中的反应与上述相同。可以看出,水在阴极8处被消耗,因此该实施例不受水从阳极7到阴极8的移动的限制。然而,这种操作模式导致产生湿氢,而干燥的氢通常是更优选的。因此,会使用干燥器(未图示)来净化氢气。这个阶段通常在产生的氢被压缩(未图示)之前进行。
在图1A中,由于阴极8是干燥的因此至少阴极8不含离聚物和/或粘合剂。在图1B中,由于阳极7是干燥的,因此至少阳极7不含离聚物和/或粘合剂。
在优选的实施方案中,阳极和阴极均不含离聚物和/或粘合剂。这意味着阳极或阴极中没有离聚物,和/或,阳极或阴极中没有粘合剂,或它们的组合。
本发明不旨在被限定于AEM或除此之外的任何特定膜。可以使用表现出所需特性的任何膜,该膜允许离子从一个半电池传输到另一个半电池。
此外,功能性基团和聚合物主链均不限于任何指定的实例,并且可以使用包含任何离子交换基团的任何合适的聚合物主链,或者任何无机或有机填料或增强剂可以被添加到其组成中。
本发明不限于所使用的催化剂。只要显示出合适的特性,就可以使用任何合适的催化剂或膜。
此外,可以改变MEA的结构和/或组成以能够利用去离子水或具有基本中性pH值的其他溶液。也可以使用缓冲溶液。在任何一种情况下,这些修改都不会超出本发明的范围。
Claims (16)
1.一种由含水液体电解制氢和氧的装置,其特征在于,所述装置包括:
一阳极半电池,其包含阳极电极,
一阴极半电池,其包含阴极电极,
一阴离子交换膜(AEM),其位于两个半电池之间,其中,
- 所述阳极电极、所述阴极电极和所述阴离子交换膜形成膜电极组件MEA,
- 包含用于将含水液体仅供给至所述阳极半电池和所述阴极半电池中的一个的装置,其中,
至少另一个基本上干燥的半电池中的电极不含离聚物和/或不含粘合剂。
2.如权利要求1所述的装置,其特征在于,在使用期间,所述含水液体的pH值为7或更高。
3.如权利要求1所述的装置,其特征在于,在使用期间,所述含水液体的pH值在12到14之间。
4.如权利要求1至3中任一项所述的装置,其特征在于,所述含水液体还包括0.1%至10%的KOH。
5.如权利要求1所述的装置,其特征在于,装置的温度在40℃到80℃的范围内。
6.如权利要求1至5中任一项所述的装置,其特征在于,所述阴极和阳极电极与一由可再生能源供能的电源连接。
7.如权利要求1至6中任一项所述的装置,其特征在于,所述MEA通过以下一种或多种方式提供稳定性:
- 膜的聚合物主链、间隔基或离子交换基团的交联,
- 提高聚合物和催化剂之间的分子间结合力,
- 更厚的膜,
- 以上的任意组合。
8.如权利要求1至7中任一项所述的装置,其特征在于,所述装置用于在1巴以上的高压下制氢。
9.如权利要求1至8中任一项所述的装置,其特征在于,所述阳极电极或阴极电极中的任意一个采用:
- 催化剂涂覆膜,或者
- 催化剂涂覆基底,或者
- 直接膜沉积。
10.如权利要求9所述的装置,其特征在于,所述催化剂涂覆基底是下述任意一种:
- 碳基布
- 碳基纸
- 碳基毡
- 不锈钢泡沫
- 镍基泡沫。
11.如权利要求1至10中任一项所述的装置,其特征在于,至少一种催化剂由非铂族金属制成。
12.如权利要求1至11中任一项所述的装置,其特征在于,所述阳极采用的用于析出氧气的反应的催化剂包括非化学计量的过渡金属氧化物。
13.如权利要求1至12中任一项所述的装置,其特征在于,所述阴极采用的用于析出氢气的反应的催化剂选自:硫属化物、烟碱类化合物、过渡金属硫化物、过渡金属磷化物、分散在导电基材中的过渡金属、或具有尖晶石或钙钛矿结构或过渡金属配合物的其他非化学计量的过渡金属氧化物。
14.如权利要求1至13中任一项所述的装置,其特征在于,所述AEM由聚合物主链与适于传输阴离子的功能基团结合形成,所述聚合物选自如下任意一种:聚苯乙烯、聚砜、聚苯并咪唑、聚苯醚、苯乙烯-丁二烯嵌段共聚物、聚乙烯。
15.如权利要求14所述的装置,其特征在于,所述聚合物主链与功能基团之间具有间隔基。
16.如权利要求1至15中任一项所述的装置,其特征在于,所述功能基团选自如下任意一种或多种:铵盐、锍盐或鏻盐。
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- 2020-06-24 CN CN202080046475.8A patent/CN114391052A/zh active Pending
- 2020-06-24 US US17/621,678 patent/US20220341046A1/en active Pending
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JP2022541385A (ja) | 2022-09-26 |
US20220341046A1 (en) | 2022-10-27 |
GB2589535A (en) | 2021-06-09 |
GB201909232D0 (en) | 2019-08-14 |
EA202193292A1 (ru) | 2022-03-25 |
AU2020306696A1 (en) | 2022-01-27 |
WO2020260370A1 (en) | 2020-12-30 |
KR20220051161A (ko) | 2022-04-26 |
GB2589535B (en) | 2024-01-31 |
JP7475072B2 (ja) | 2024-04-26 |
EP3990682A1 (en) | 2022-05-04 |
CA3143893A1 (en) | 2020-12-30 |
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