CN106536790B - 二氧化氯的催化或电催化产生 - Google Patents
二氧化氯的催化或电催化产生 Download PDFInfo
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- OSVXSBDYLRYLIG-UHFFFAOYSA-N dioxidochlorine(.) Chemical compound O=Cl=O OSVXSBDYLRYLIG-UHFFFAOYSA-N 0.000 title claims abstract description 37
- 239000004155 Chlorine dioxide Substances 0.000 title claims abstract description 16
- 235000019398 chlorine dioxide Nutrition 0.000 title claims abstract description 16
- 230000003197 catalytic effect Effects 0.000 title description 4
- 239000003054 catalyst Substances 0.000 claims abstract description 44
- XTEGARKTQYYJKE-UHFFFAOYSA-M Chlorate Chemical compound [O-]Cl(=O)=O XTEGARKTQYYJKE-UHFFFAOYSA-M 0.000 claims abstract description 18
- 238000000034 method Methods 0.000 claims abstract description 10
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- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims abstract description 6
- 239000001301 oxygen Substances 0.000 claims abstract description 6
- 229910052760 oxygen Inorganic materials 0.000 claims abstract description 6
- 239000007864 aqueous solution Substances 0.000 claims abstract description 4
- 229910052751 metal Inorganic materials 0.000 claims abstract description 4
- 239000002184 metal Substances 0.000 claims abstract description 4
- 230000002378 acidificating effect Effects 0.000 claims abstract description 3
- 230000010287 polarization Effects 0.000 claims abstract description 3
- 150000004706 metal oxides Chemical class 0.000 claims description 7
- 239000000203 mixture Substances 0.000 claims description 6
- 239000000919 ceramic Substances 0.000 claims description 5
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- HTXDPTMKBJXEOW-UHFFFAOYSA-N dioxoiridium Chemical compound O=[Ir]=O HTXDPTMKBJXEOW-UHFFFAOYSA-N 0.000 claims description 3
- 229910000457 iridium oxide Inorganic materials 0.000 claims description 3
- HBEQXAKJSGXAIQ-UHFFFAOYSA-N oxopalladium Chemical compound [Pd]=O HBEQXAKJSGXAIQ-UHFFFAOYSA-N 0.000 claims description 3
- MUMZUERVLWJKNR-UHFFFAOYSA-N oxoplatinum Chemical compound [Pt]=O MUMZUERVLWJKNR-UHFFFAOYSA-N 0.000 claims description 3
- SJLOMQIUPFZJAN-UHFFFAOYSA-N oxorhodium Chemical compound [Rh]=O SJLOMQIUPFZJAN-UHFFFAOYSA-N 0.000 claims description 3
- 229910003445 palladium oxide Inorganic materials 0.000 claims description 3
- 229910003446 platinum oxide Inorganic materials 0.000 claims description 3
- 229910003450 rhodium oxide Inorganic materials 0.000 claims description 3
- 229910001925 ruthenium oxide Inorganic materials 0.000 claims description 3
- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(iv) oxide Chemical compound O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 claims description 3
- 229910044991 metal oxide Inorganic materials 0.000 claims description 2
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- 239000002253 acid Substances 0.000 description 9
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- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 4
- 239000003638 chemical reducing agent Substances 0.000 description 4
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 3
- 238000006243 chemical reaction Methods 0.000 description 3
- QBWCMBCROVPCKQ-UHFFFAOYSA-N chlorous acid Chemical compound OCl=O QBWCMBCROVPCKQ-UHFFFAOYSA-N 0.000 description 3
- 239000002994 raw material Substances 0.000 description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 2
- 239000012267 brine Substances 0.000 description 2
- 238000010531 catalytic reduction reaction Methods 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- SUKJFIGYRHOWBL-UHFFFAOYSA-N sodium hypochlorite Chemical compound [Na+].Cl[O-] SUKJFIGYRHOWBL-UHFFFAOYSA-N 0.000 description 2
- HPALAKNZSZLMCH-UHFFFAOYSA-M sodium;chloride;hydrate Chemical compound O.[Na+].[Cl-] HPALAKNZSZLMCH-UHFFFAOYSA-M 0.000 description 2
- 125000006850 spacer group Chemical group 0.000 description 2
- BZSXEZOLBIJVQK-UHFFFAOYSA-N 2-methylsulfonylbenzoic acid Chemical compound CS(=O)(=O)C1=CC=CC=C1C(O)=O BZSXEZOLBIJVQK-UHFFFAOYSA-N 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 1
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 1
- 229910019834 RhO2 Inorganic materials 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 229910052783 alkali metal Inorganic materials 0.000 description 1
- 150000001340 alkali metals Chemical class 0.000 description 1
- 239000002585 base Substances 0.000 description 1
- XTEGARKTQYYJKE-UHFFFAOYSA-N chloric acid Chemical compound OCl(=O)=O XTEGARKTQYYJKE-UHFFFAOYSA-N 0.000 description 1
- 238000004821 distillation Methods 0.000 description 1
- 238000010292 electrical insulation Methods 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- -1 halide salts Chemical class 0.000 description 1
- 229910052500 inorganic mineral Inorganic materials 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- 239000011707 mineral Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- YZHUMGUJCQRKBT-UHFFFAOYSA-M sodium chlorate Chemical compound [Na+].[O-]Cl(=O)=O YZHUMGUJCQRKBT-UHFFFAOYSA-M 0.000 description 1
- 239000011780 sodium chloride Substances 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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- C—CHEMISTRY; METALLURGY
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- C25B1/00—Electrolytic production of inorganic compounds or non-metals
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- C25B1/26—Chlorine; Compounds thereof
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Abstract
本发明关注电极元件，包含：阀金属基材；施加至所述基材的第一催化剂组分，所述第一催化剂组分适合于在阳极极化下由水溶液析出氧；第二催化剂组分，其适合于在酸性环境中由氯酸盐溶液产生二氧化氯，所述第一和第二催化剂组分彼此电绝缘。本发明还关注包含这样的电极元件的电解池和用于在催化剂组分上产生二氧化氯的工艺，电化学电池包含这样的电极元件。
Description
发明领域
本发明涉及二氧化氯(ClO2)的生产并且特别地涉及用于生产二氧化氯的催化工艺以及合适的电极元件。
发明背景
历史上，通过水溶液中的金属氯酸盐(例如氯酸钠(NaClO3))和相对强的酸(例如硫酸、磷酸或氢氯酸)之间的反应商业制备ClO2。
通常，用于产生ClO2的工艺利用含碱性氯酸盐的原料(经常是NaClO3)，其还包括碱金属的卤化物盐或其他还原剂。典型地通过以任何众所周知的手段电解氯化钠盐水产生用于这样的ClO2生产工艺的氯酸钠原料。当使用氯化物作为还原剂时，将盐水和氯酸盐的混合物直接加料至一个或多个反应器，其中原料接触所需要的酸并且反应形成ClO2。由于所需要的高酸度量，例如5-10N酸，加上对于还原剂的需求，没有实践由NaClO3小规模生产ClO2。例如在US4501824,US426263,US4381290和US4362707中报道了凭借氯酸钠在强酸中电化学或催化还原的ClO2产生工艺的实例。这些现有技术的教导允许省去对于单独的还原剂的需求，然而在工艺中仍然需要酸的化学供应。
发明概述
在所附的权利要求中阐述本发明的各个方面。
在一个方面，本发明涉及电极元件，包含：阀金属基材；施加至所述基材的第一催化剂组分，所述第一催化剂组分适合于在阳极极化下由水溶液析出氧；第二催化剂组分，其适合于在酸性环境中由氯酸盐溶液产生二氧化氯；所述第一和第二催化剂组分彼此电绝缘。
由于上面的布置，氧的阳极析出与因而引起的质子产生导致了在第二催化剂组分的表面处溶液局部pH的降低。换言之，在不需要任何外部酸添加的情况下，电化学阳极反应产生适合于实施氯酸盐至二氧化氯的催化还原的酸浓度。然后本发明的电极元件适合于仅由水和氯酸盐溶液开始产生二氧化氯，因此避免强无机酸例如硫酸的处置。
关于电极元件，在此预期包含布置在单个的独立件中的两种有区别的催化剂组分的整体电极，该两种催化剂组分或由合适的绝缘间隔体隔开，或密切接触但是彼此电绝缘。
在一个实施方案中，电极元件的第二催化剂组分负载在陶瓷载体上。该陶瓷载体，例如能够为分立的陶瓷介质形式，例如蒸馏支架。
在另一个实施方案中，电极元件的第二催化剂组分负载在金属性载体上。
能够任选地使此第二催化剂组分极化至较低的电势以增强二氧化氯的生产。
在一个实施方案中，电极元件的第二催化剂组分连接至电源。
在一个实施方案中，电极元件的第一催化剂组分包含贵金属氧化物。
在一个实施方案中，在根据本发明的电极元件中，该第二催化剂组分是选自由氧化钌、氧化铱、氧化钯、氧化铑和氧化铂组成的组的贵金属氧化物的混合物。任选地，该第二催化剂组分还包含阀金属氧化物。
在一个实施方案中，电极元件的第二催化剂组分是陶瓷的或金属性的片材或网状物的形式，或多孔材料的形式。
在另一个方面，本发明涉及电解池，其包含至少一个如上面述描述的电极元件。
在一个实施方案中，该电解池配备有电极元件，其设置为第二催化剂组分和施加至基材的插入的第一催化剂组分的排列，该第一和第二催化剂组分相互地绝缘。
在又一个方面，本发明涉及用于在催化剂组分上产生二氧化氯的工艺，其包含以下步骤：
-提供包含至少一个阴极和至少一个如权利要求1中描述的电极元件作为阳极的电化学电池；
-用含氯酸盐溶液的含水原料供应所述电池；
-通过使电流在阴极和阳极之间通过来电解所述原料从而在所述第一催化剂组分的表面上形成氧和酸度并且将酸度供应至所述第二催化剂层的表面的周围；
-分离(strip)和回收在催化层上产生的二氧化氯。
优选地，在40℃至90℃的温度下电解该溶液。
包括下列实施例来证明本发明的特别的实施方案，在要求保护的数值范围内已经大量验证了其可行性。本领域技术人员应该领会，在以下实施例中公开的组成和技术代表由本发明人探索的在本发明的实践中良好作用的组成和技术；然而，鉴于本公开，本领域技术人员应该领会在所公开的具体实施方案中能够做出许多改变，并且仍然获得类似的或相似的结果，而不脱离本发明的范围。
实施例
制备包含0.5厘米直径涂覆钛棒作为阳极的电化学电池。阳极的涂层由10g/m2的2：1摩尔比的铱和钽的混合氧化物组成。使充当用于第二催化剂元件的载体的涂覆的钛膨胀网缠绕该棒，且在其间布置间隔体以提供电绝缘。钛网的涂层由10g/m2的1：2摩尔比的RuO2/RhO2组成。供应2M NaClO3溶液作为电解质原料。在61℃的温度下和在50mA/cm2的阳极电流密度下进行反应。
试验运行持续5小时。每一小时提取样品并且在UV/VIS分光光度计(Hach DR5000)中表征。图显示作为时间的函数的二氧化氯浓度的增加。
之前的说明不应当意图为限制本发明，在没有脱离其范围的情况下其可以根据不同的实施方案使用，并且本发明的范围的程度仅由所附的权利要求限定。
贯穿本申请的说明书和权利要求书，术语“包含”及其变型例如“包括”和“包含有”不意图排除其他元件、组分或额外的工艺步骤的存在。
此申请文件中包括文献、法案、材料、装置、制品及类似物的讨论仅仅是出于为本发明提供上下文的目的。不表明或代表这些内容的任何或全部形成部分的现有技术基础或是在此申请的每个权利要求的优先权日之前与本发明相关的领域内的公知常识。
Claims (11)
1.电极元件，由包含布置在单个的独立件中的两种有区别的催化剂组分的整体电极组成，并包含：
-阀金属基材；
-施加至所述基材的第一催化剂组分，所述第一催化剂组分适合于在阳极极化下由水溶液析出氧；
-第二催化剂组分，其适合于在酸性环境中由氯酸盐溶液产生二氧化氯；
所述第一和第二催化剂组分密切接触但是彼此电绝缘。
2.根据权利要求1的电极元件，其中所述第二催化剂组分负载在陶瓷载体上。
3.根据权利要求1的电极元件，其中所述第二催化剂组分负载在金属性载体上。
4.根据权利要求1的电极元件，其中所述第一催化剂组分包含贵金属氧化物。
5.根据权利要求1的电极元件，其中所述第二催化剂组分是选自由氧化钌、氧化铱、氧化钯、氧化铑和氧化铂组成的组的贵金属氧化物的混合物。
6.根据权利要求1的电极元件，其中所述第二催化剂组分是选自由氧化钌、氧化铱、氧化钯、氧化铑和氧化铂组成的组的贵金属氧化物的混合物，并且还包含阀金属氧化物。
7.根据权利要求1的电极元件，其中所述第二催化剂组分是片材、网状物或多孔材料的形式。
8.电解池，其包含至少一个如权利要求1中描述的电极元件。
9.根据权利要求8的电解池，其中通过彼此绝缘的第二催化剂组分和施加至基材的插入的第一催化剂组分的排列来设置电极元件。
10.电解池，其包含至少一个如权利要求3中描述的电极元件以及电源，其中所述第二催化剂组分连接至所述电源。
11.用于在催化剂组分上产生二氧化氯的工艺，其包含以下步骤：
-提供包含至少一个阴极和至少一个如权利要求1中描述的电极元件作为阳极的电化学电池；
-用含氯酸盐溶液的含水原料填充所述电池；
-通过使电流在阴极和阳极之间通过来电解所述原料，从而在所述第一催化剂组分表面上形成氧和酸度并且从而形成与所述第二催化剂组分的表面紧密接触的酸度；
-分离和回收在所述第二催化剂组分上产生的二氧化氯。
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| US201462025557P | 2014-07-17 | 2014-07-17 | |
| US62/025,557 | 2014-07-17 | ||
| PCT/EP2015/066378 WO2016009031A1 (en) | 2014-07-17 | 2015-07-17 | Catalytic or electrocatalytic generation of chlorine dioxide |
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| Publication number | Publication date |
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| JP2017522456A (ja) | 2017-08-10 |
| PH12016502566A1 (en) | 2017-04-17 |
| RU2017104923A (ru) | 2018-08-17 |
| US20170211194A1 (en) | 2017-07-27 |
| RU2674688C2 (ru) | 2018-12-12 |
| AU2015289095B2 (en) | 2019-04-04 |
| MY175177A (en) | 2020-06-12 |
| BR112017000889A2 (pt) | 2017-11-21 |
| CN106536790A (zh) | 2017-03-22 |
| US10590546B2 (en) | 2020-03-17 |
| RU2017104923A3 (zh) | 2018-11-13 |
| ZA201608309B (en) | 2018-11-28 |
| PH12016502566B1 (en) | 2017-04-17 |
| MX2017000725A (es) | 2017-04-27 |
| TR201811290T4 (tr) | 2018-08-27 |
| CA2951002C (en) | 2023-07-04 |
| EP3169829B1 (en) | 2018-05-23 |
| KR20170035901A (ko) | 2017-03-31 |
| JP7037937B2 (ja) | 2022-03-17 |
| IL249542A0 (en) | 2017-02-28 |
| SG11201610299QA (en) | 2017-01-27 |
| EP3169829A1 (en) | 2017-05-24 |
| AU2015289095A1 (en) | 2016-12-22 |
| ES2676493T3 (es) | 2018-07-20 |
| KR102405372B1 (ko) | 2022-06-07 |
| WO2016009031A1 (en) | 2016-01-21 |
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| IL249542B (en) | 2018-12-31 |
| CA2951002A1 (en) | 2016-01-21 |
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