TW202314043A - A low energy consumption iodide oxidation reaction system - Google Patents
A low energy consumption iodide oxidation reaction system Download PDFInfo
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本發明是一種低耗能產氫技術，特別是一種以電化學機制產氫同時產碘的高附加價值產物的系統。The invention is a technology for producing hydrogen with low energy consumption, in particular a system for producing hydrogen and iodine with high added value by an electrochemical mechanism.
一般傳統的產氫系統(Oxygen evolution reaction, OER)所使用的電解水技術可生成高純度的氫氣(H 2)和氧氣(O 2)，但面臨陽極氧析出反應的反應速率過慢造成的高能耗問題，同時這種OER系統也無法克服氧氣析出反應的熱力學限制，氧析出的反應電位大(＞1.23 V, SHE)，又所產生的氫氣與氧氣因氣體分子極小，會再穿透陰陽極隔離膜，造成氫氣的純度下降。 Generally, the electrolytic water technology used in the traditional hydrogen production system (Oxygen evolution reaction, OER) can generate high-purity hydrogen (H 2 ) and oxygen (O 2 ), but it faces the high energy At the same time, this OER system cannot overcome the thermodynamic limitation of oxygen evolution reaction. The reaction potential of oxygen evolution is large (>1.23 V, SHE), and the hydrogen and oxygen produced will penetrate through the cathode and anode because the gas molecules are extremely small. The isolation membrane causes the purity of hydrogen to decrease.
為了解決既有的電解水技術僅能產生氫氣與氧氣等較低經濟價值的產物，且反應速率慢又耗能的限制，本發明提供一種低耗能產氫與碘衍生物的系統，其包含： 一陽極反應區； 一陰極反應區與該陽極反應區電性連接；其中： 該陽極反應區與該陰極反應區相互以一液體相通，該液體中包含一觸媒，該陽極反應區與該陰極反應區間以該液體可通透之一通透間隔元件區隔； 該陽極反應區包含一陽極至少局部浸沒於一陽極反應液體中，該陽極反應液體中至少包含碘元素及/或碘離子，碘元素及/或碘離子無法通過該通透間隔元件；以及 該陰極反應區中包含一陰極至少局部浸沒於一陰極反應液體中，該陰極反應液體中至少包含氫氣與氫離子，並設有一產出物出口。 In order to solve the existing water electrolysis technology that can only produce products of low economic value such as hydrogen and oxygen, and has the limitation of slow reaction rate and energy consumption, the present invention provides a system for producing hydrogen and iodine derivatives with low energy consumption, which includes : an anode reaction zone; A cathode reaction zone is electrically connected to the anode reaction zone; wherein: The anode reaction zone and the cathode reaction zone communicate with each other through a liquid, the liquid contains a catalyst, and the anode reaction zone and the cathode reaction zone are separated by a permeable spacer element that is permeable to the liquid; The anode reaction zone includes an anode at least partially immersed in an anode reaction liquid, the anode reaction liquid contains at least iodine element and/or iodide ions, and the iodine element and/or iodide ions cannot pass through the permeable spacer; and The cathode reaction zone includes a cathode at least partially immersed in a cathode reaction liquid, the cathode reaction liquid contains at least hydrogen gas and hydrogen ions, and is provided with an output outlet.
其中，該液體包含0.01~ 2M的碘化鈉及/或0.01~ 2 M過氯酸；或0.01~ 2M的碘化鈉及/或0.01~ 2M氫氧化鈉水溶液。Wherein, the liquid comprises 0.01-2M sodium iodide and/or 0.01-2 M perchloric acid; or 0.01-2M sodium iodide and/or 0.01-2M sodium hydroxide aqueous solution.
其中，該通透間隔元件包含質子交換膜或陰離子交換膜。Wherein, the permeable spacer comprises a proton exchange membrane or an anion exchange membrane.
其中，該觸媒是一包含表面雙金屬成分的合金氧化物導電材料，由數個小尺寸的金屬原子以至少一原子層狀態附著於大尺寸的金屬氧化物表面所形成的合金氧化物導電材料。Among them, the catalyst is an alloy oxide conductive material containing a surface bimetallic composition, which is formed by the alloy oxide conductive material formed by several small-sized metal atoms attached to the surface of a large-sized metal oxide in at least one atomic layer state .
其中，該質子交換膜包含全氟磺酸膜；以及該陰離子交換膜包含鹼性高分子電解質膜。Wherein, the proton exchange membrane includes a perfluorosulfonic acid membrane; and the anion exchange membrane includes an alkaline polymer electrolyte membrane.
其中，該雙金屬成分的合金氧化物材料中，該小尺寸金屬包含釕、鐵、鈷、銠、銥、鎳、鈀、銅、銀、金或鉑；以及該金屬氧化物材料包含氧化錫、氧化鈦、氧化釕、氧化銦、氧化鋅、氧化鐵、氧化鈷、氧化鎢、氧化鉬、氧化鎳的其一或組合。Wherein, in the alloy oxide material of the bimetallic composition, the small-sized metal comprises ruthenium, iron, cobalt, rhodium, iridium, nickel, palladium, copper, silver, gold or platinum; and the metal oxide material comprises tin oxide, One or a combination of titanium oxide, ruthenium oxide, indium oxide, zinc oxide, iron oxide, cobalt oxide, tungsten oxide, molybdenum oxide, and nickel oxide.
其中，如請求項1所述之低耗能產氫與碘衍生物的系統，其中：該陽極反應區產生I
3 -(aq) + I
-(aq) → I
2(s)的反應；以及該陰極反應區產生H
+(aq) → H
2(g)的反應。
Wherein, the system for producing hydrogen and iodine derivatives with low energy consumption as described in
其中，該陰極反應區產生之氫氣自一產出物出口排出。Wherein, the hydrogen gas generated in the cathode reaction zone is discharged from an output outlet.
藉由上述說明可知， 本發明提供一種新型電解方法，利用碘化物氧化反應作為取代氧氣析出反應，因為碘化物氧化反應電位(＞0.54 V, SHE)，因此可有效節省30~40% 電能，所生成的碘(Iodine)不會再穿透隔離膜降低氫氣濃度，此高附加價值的碘具有可觀的商業價值，可運用在醫學影像顯影劑、醫藥、LCD偏光膜、食品、化學品等。本發明的優勢在於相對於既有的電解方法降低大量能耗，也可產出具商業價值的碘之高值化產氫技術。From the above description, it can be seen that the present invention provides a new type of electrolysis method, which uses the iodide oxidation reaction to replace the oxygen evolution reaction. Because the iodide oxidation reaction potential (>0.54 V, SHE), it can effectively save 30~40% of electric energy, so The generated iodine (Iodine) will no longer penetrate the isolation film to reduce the hydrogen concentration. This high-value-added iodine has considerable commercial value and can be used in medical image developers, medicines, LCD polarizing films, food, chemicals, etc. The advantage of the present invention is that compared with the existing electrolysis method, a large amount of energy consumption is reduced, and a high-value hydrogen production technology that can also produce commercially valuable iodine.
爲了更清楚地說明本發明實施例的技術方案，下面將對實施例描述中所需要使用的附圖作簡單的介紹。顯而易見地，下面描述中的附圖僅僅是本發明的一些示例或實施例，對於本領域的普通技術人員來講，在不付出創造性勞動的前提下，還可以根據這些附圖將本發明應用於其它類似情景。除非從語言環境中顯而易見或另做說明，圖中相同標號代表相同結構或操作。In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the following briefly introduces the drawings that need to be used in the description of the embodiments. Obviously, the accompanying drawings in the following description are only some examples or embodiments of the present invention, and those skilled in the art can also apply the present invention to other similar scenarios. Unless otherwise apparent from context or otherwise indicated, like reference numerals in the figures represent like structures or operations.
應當理解，本文使用的“系統”、“裝置”、“單元”和/或“模組”是用於區分不同級別的不同組件、元件、部件、部分或裝配的一種方法。然而，如果其他詞語可實現相同的目的，則可通過其他表達來替換所述詞語。It should be understood that "system", "device", "unit" and/or "module" as used herein is a method for distinguishing different components, elements, components, parts or assemblies of different levels. However, the words may be replaced by other expressions if other words can achieve the same purpose.
如本發明和請求項書中所示，除非上下文明確提示例外情形，“一”、“一個”、“一種”和/或“該”等詞並非特指單數，也可包括複數。一般說來，術語“包括”與“包含”僅提示包括已明確標識的步驟和元素，而這些步驟和元素不構成一個排它性的羅列，方法或者設備也可能包含其它的步驟或元素。As shown in the present application and claims, words such as "a", "an", "an" and/or "the" are not specific to the singular and may also include the plural, unless the context clearly indicates an exception. Generally speaking, the terms "comprising" and "comprising" only suggest the inclusion of clearly identified steps and elements, and these steps and elements do not constitute an exclusive list, and the method or device may also contain other steps or elements.
本發明中使用了流程圖用來說明根據本發明的實施例的系統所執行的操作。應當理解的是，前面或後面操作不一定按照順序來精確地執行。相反，可以按照倒序或同時處理各個步驟。同時，也可以將其他操作添加到這些過程中，或從這些過程移除某一步或數步操作。The flow chart is used in the present invention to illustrate the operations performed by the system according to the embodiment of the present invention. It should be understood that the preceding or following operations are not necessarily performed in the exact order. Instead, various steps may be processed in reverse order or simultaneously. At the same time, other operations can be added to these procedures, or a certain step or steps can be removed from these procedures.
＜較佳實施例＞<Preferred Embodiment>
請參考圖1，本發明所提供的一種低耗能產氫與碘衍生物的系統100，其包含：一陽極反應區101以及一陰極反應區103，該陽極反應區101與該陰極反應區103相互以一液體105相通，該陽極反應區101與該陰極反應區103間又以該液體105可通透之一通透間隔元件107區隔。該液體105一較佳實施例包含0.01M～2M的碘化鈉(NaI)及/或0.1 M～2M過氯酸(HClO
4)，另一較佳實施例該液體105一較佳實施例包含0.01~ 2M的碘化鈉及/或0.01~ 2M氫氧化鈉水溶液。
Please refer to FIG. 1 , a
其中，該陽極反應區101在本實施例中較佳包含一陽極1011至少局部浸沒於一陽極反應液體1013中。該陽極反應液體1013中至少包含碘元素(I
2)及/或碘離子，該碘離子包含I
-與I
3-(三碘離子)。碘元素及/或碘離子無法通過該通透間隔元件107，僅會留滯於該陽極反應區101中反應，該通透間隔元件107一較佳實施例可以是質子交換膜，例如全氟磺酸膜(Nafion
®)，或陰離子交換膜(適用於鹼性系統)，例如鹼性高分子電解質膜。
Wherein, the
該陰極反應區103中包含一陰極1031至少局部浸沒於一陰極反應液體1033中。該陰極1031與該陽極1011電性連接。該陰極反應液體1033中至少包含氫氣(H
2)與氫離子(H
+)。該陰極反應區103中設有一產出物出口1035。
The
進一步地，當本發明所提供的系統執行時，該陽極反應區101與該陰極反應區103分別產生的反應如下。Further, when the system provided by the present invention is implemented, the reactions generated in the
該陽極反應區101：I 3 -(aq) + I -(aq) → I 2(s) The anode reaction zone 101: I 3 - (aq) + I - (aq) → I 2 (s)
該陰極反應區103：H +(aq) → H 2(g) The cathode reaction zone 103: H + (aq) → H 2 (g)
其中，本發明於該陰極反應區103反應所產生的氫氣將自該產出物出口1035排出並收集。Wherein, the hydrogen gas produced by the reaction in the
進一步地，本發明所提供的該液體105中較佳包含一觸媒C，該催化劑C是一種包含雙金屬成分的合金氧化物導電材料，特別是一種表面合金氧化物材料(Surface Alloy Oxide)。所謂的表面合金材料是指取兩種尺寸大小相異的金屬原子與金屬氧化物，將數個小尺寸的其一金屬原子附著於大尺寸的金屬氧化物表面所形成的合金氧化物，較佳的小尺寸金屬是具有催化功能，以至少單一原子層與大尺寸金屬原子形成表面合金氧化物，更佳是以1-3層原子層形成表面合金氧化物。該觸媒C一較佳實施例為釕(Ruthenium, Ru)- 錫(Tin, Sn)表面合金氧化物材料，釕原子在錫氧化物(SnO 2)粒子表面，以3層形成表面合金氧化物。該小尺寸金屬其它較佳實施例包含釕(Ru)、鐵(Fe)、鈷(Co)、銠(Rh)、銥(Ir)、鎳(Ni)、鈀(Pd)、銅(Cu)、銀(Ag)、金(Au)或鉑(Pt)。該金屬氧化物材料選擇包含氧化錫、氧化鈦、氧化釕、氧化銦、氧化鋅、氧化鐵、氧化鈷、氧化鎢、氧化鉬或氧化鎳的其一或混合搭配形成表面合金金屬氧化物材料。 Further, the liquid 105 provided by the present invention preferably includes a catalyst C, the catalyst C is an alloy oxide conductive material containing a bimetallic component, especially a surface alloy oxide material (Surface Alloy Oxide). The so-called surface alloy material refers to the alloy oxide formed by taking two metal atoms and metal oxides of different sizes, and attaching several small-sized metal atoms to the surface of a large-sized metal oxide. The small-sized metal has a catalytic function, and forms a surface alloy oxide with at least a single atomic layer and a large-sized metal atom, and more preferably forms a surface alloy oxide with 1-3 atomic layers. A preferred embodiment of the catalyst C is ruthenium (Ruthenium, Ru)-tin (Tin, Sn) surface alloy oxide material, and ruthenium atoms are on the surface of tin oxide (SnO 2 ) particles to form a surface alloy oxide in three layers . Other preferred embodiments of the small-sized metal include ruthenium (Ru), iron (Fe), cobalt (Co), rhodium (Rh), iridium (Ir), nickel (Ni), palladium (Pd), copper (Cu), Silver (Ag), Gold (Au) or Platinum (Pt). The metal oxide material is selected to include one of tin oxide, titanium oxide, ruthenium oxide, indium oxide, zinc oxide, iron oxide, cobalt oxide, tungsten oxide, molybdenum oxide or nickel oxide or a mixture thereof to form a surface alloy metal oxide material.
進一步地，前述釕(Ruthenium, Ru)- 錫(Tin, Sn)表面合金氧化物材料的製造方法較佳實施例包含：Further, preferred embodiments of the aforementioned ruthenium (Ruthenium, Ru)-tin (Tin, Sn) surface alloy oxide material manufacturing method include:
準備一乙醇水溶液(EtOH: DI H 2O)，將錫前驅物(Sn precursor)與尿素(Urea)加入於該乙醇水溶液中，以溫度150 OC水熱法反應24小時，形成錫氧化物(SnO 2)； Prepare an ethanol aqueous solution (EtOH: DI H 2 O), add the tin precursor (Sn precursor) and urea (Urea) to the ethanol aqueous solution, and react at a temperature of 150 OC for 24 hours by hydrothermal method to form tin oxide ( SnO 2 );
將釕前驅物(Ru precursor)與乙二醇(Ethylene Glycol)添加進錫氧化物的混合物中，以溫度180 OC水熱法反應12小時後得到釕(Ruthenium, Ru)- 錫(Tin, Sn)表面合金氧化物材料。 Add the ruthenium precursor (Ru precursor) and ethylene glycol (Ethylene Glycol) to the mixture of tin oxides, and react at a temperature of 180 OC for 12 hours to obtain ruthenium (Ruthenium, Ru)-tin (Tin, Sn ) surface alloy oxide material.
＜確效性測試＞以下將以含有前述該釕(Ruthenium, Ru)- 錫(Tin, Sn)表面合金氧化物材料作為該觸媒C的實施例進行確效性測試。<Validity Test> The validation test will be carried out below using the embodiment containing the aforementioned ruthenium (Ruthenium, Ru)-tin (Tin, Sn) surface alloy oxide material as the catalyst C.
請參考圖2，於相同觸媒比較不同反應，使用線性伏安法(Linear sweep voltammetry, LSV) 比較能耗情況，在相同的電流密度 10 mA/cm 2，本發明的反應僅需耗費1.07 伏(V)的電壓，而一般傳統的產氫系統(Oxygen evolution reaction, OER)則須1.58 V，能量可節省510mV。 Please refer to Figure 2 to compare different reactions on the same catalyst, and use linear sweep voltammetry (LSV) to compare energy consumption. At the same current density of 10 mA/cm 2 , the reaction of the present invention only consumes 1.07 volts (V) voltage, while the general traditional hydrogen production system (Oxygen evolution reaction, OER) requires 1.58 V, and the energy can be saved by 510mV.
請參考圖3的電壓(Voltage, V)與電流密度(Current Density, J, mAcm -2)關係，結果顯示在不同電流密度，本發明的能耗均比OER有顯著的降低。 Please refer to the relationship between voltage (Voltage, V) and current density (Current Density, J, mAcm -2 ) in Figure 3. The results show that the energy consumption of the present invention is significantly lower than that of OER at different current densities.
請參考圖4A與4B的產物生成效率，計算本發明產氫技術之氫氣與碘生成效率，圖之縱軸為實驗量測值 (氫氣以氣相層析儀量測；液態碘以滴定方式量測)；橫軸為理論計算值，縱軸數值/橫軸數值=生成效率。其中，本發明實施例的H 2生成效率: ~100% (以氣相層析儀量測)，I2生成效率: ~92% (以滴定方式量測)。 Please refer to the product generation efficiency in Figures 4A and 4B to calculate the hydrogen and iodine generation efficiency of the hydrogen production technology of the present invention. The vertical axis of the figure is the experimental measurement value (hydrogen is measured by gas chromatography; liquid iodine is measured by titration) measured); the horizontal axis is the theoretical calculation value, and the vertical axis value/horizontal axis value = generation efficiency. Wherein, the H2 generation efficiency of the embodiment of the present invention: ~100% (measured by gas chromatography), and the I2 generation efficiency: ~92% (measured by titration).
請參考圖5A與5B，於相同反應比較不同觸媒，以產生10mA/cm 2電流密度，RuSnO 2觸媒所需的電壓明顯小於測試之其它觸媒(以Pt/C為對比例) 以及標準品 氧化錫(SnO 2) 與氧化釕 (RuO 2)。 Please refer to Figure 5A and 5B, comparing different catalysts in the same reaction, in order to generate a current density of 10mA/cm 2 , the voltage required for the RuSnO 2 catalyst is significantly lower than that of other catalysts tested (Pt/C as a comparison) and the standard Products tin oxide (SnO 2 ) and ruthenium oxide (RuO 2 ).
此外，除非請求項中明確說明，本發明所述處理元素和序列的順序、數字字母的使用、或其他名稱的使用，並非用於限定本發明流程和方法的順序。儘管上述揭露中通過各種示例討論了一些目前認爲有用的發明實施例，但應當理解的是，該類細節僅起到說明的目的，附加的請求項並不僅限於披露的實施例，相反，請求項旨在覆蓋所有符合本發明實施例實質和範圍的修正和等價組合。In addition, unless explicitly stated in the claim, the sequence of processing elements and sequences, the use of numbers and letters, or the use of other names in the present invention are not used to limit the sequence of the flow and method of the present invention. While the foregoing disclosure discusses, by way of various examples, some embodiments of the invention that are presently believed to be useful, it should be understood that such details are for illustrative purposes only and that the appended claims are not limited to the disclosed embodiments, but instead claim The items are intended to cover all modifications and equivalent combinations consistent with the spirit and scope of the embodiments of the present invention.
同理，應當注意的是，爲了簡化本發明揭露技術的表述，從而幫助對一個或多個發明實施例的理解，前文對本發明實施例的描述中，有時會將多種特徵歸並至一個實施例、附圖或對其的描述中。但是，這種揭露方法並不意味著本發明所欲宣稱的保護對象所需要的特徵比實施例中提及的特徵多。實際上，在不損及本發明功效的情況下，請求項中的特徵可能要少於上述揭露的單個實施例的全部特徵。In the same way, it should be noted that in order to simplify the description of the technology disclosed in the present invention so as to help the understanding of one or more embodiments of the invention, in the description of the embodiments of the present invention above, sometimes multiple features are combined into one implementation examples, drawings or descriptions thereof. However, this method of disclosure does not mean that the claimed object of the present invention requires more features than those mentioned in the examples. Indeed, claimed features may be less than all features of a single foregoing disclosed embodiment without prejudice to the efficacy of the invention.
一些實施例中使用了描述成分、屬性數量的數字，應當理解的是，此類用於實施例描述的數字，在一些示例中使用了修飾詞“大約”、“近似”或“大體上”來修飾。除非另外說明，“大約”、“近似”或“大體上”表明所述數字允許有±20%的變化。相應地，在一些實施例中，說明書和請求項中使用的數值參數均爲近似值，該近似值根據個別實施例所需特點可以發生改變。在一些實施例中，數值參數應考慮規定的有效數位並采用一般位數保留的方法。儘管本發明一些實施例中用於確認其範圍廣度的數值域和參數爲近似值，在具體實施例中，此類數值的設定在可行範圍內盡可能精確。In some embodiments, numbers describing the quantity of components and attributes are used. It should be understood that such numbers used in the description of the embodiments use the modifiers "about", "approximately" or "substantially" in some examples. grooming. Unless otherwise stated, "about", "approximately" or "substantially" indicates that the stated figure allows for a variation of ±20%. Accordingly, in some embodiments, the numerical parameters used in the specification and claims are approximations that may vary depending upon the desired characteristics of individual embodiments. In some embodiments, numerical parameters should take into account the specified significant digits and adopt the general digit reservation method. Although the numerical ranges and parameters used to demonstrate the breadth of scope in some embodiments of the invention are approximations, in specific embodiments such numerical values are set as precisely as practicable.
最後，應當理解的是，本發明中所述實施例僅用以說明本發明實施例的原則。其他的變形也可能屬本發明的範圍。因此，作爲示例而非限制，本發明實施例的替代配置可視爲與本發明的教導一致。相應地，本發明的實施例不僅限於本發明明確介紹和描述的實施例。Finally, it should be understood that the embodiments described in the present invention are only used to illustrate the principles of the embodiments of the present invention. Other variations are also possible within the scope of the present invention. Accordingly, by way of illustration and not limitation, alternative configurations of the embodiments of the present invention may be considered consistent with the teachings of the present invention. Accordingly, the embodiments of the present invention are not limited to the embodiments of the present invention explicitly shown and described.
100:低耗能產氫與碘衍生物的系統 101:陽極反應區 1011:陽極 1013:陽極反應液體 103:陰極反應區 1031:陰極 1033:陰極反應液體 1035:產出物出口 105:液體 107:通透間隔元件 C:觸媒 100: A system for producing hydrogen and iodine derivatives with low energy consumption 101: Anode reaction area 1011: anode 1013: anode reaction liquid 103: Cathode reaction area 1031: Cathode 1033: cathode reaction liquid 1035: Output export 105: liquid 107: transparent spacer element C: Catalyst
本發明將以示例性實施例的方式進一步說明，這些示例性實施例將通過附圖進行詳細描述。這些實施例並非限制性的，在這些實施例中，相同的編號表示相同的結構，其中： 圖1為本發明較佳實施例之系統示意圖。 圖2為本發明與對比例的電流密度與電壓關係示意圖。 圖3為本發明與對比例的電壓與電流密度關係示意圖。 圖4A與圖4B分別為本發明氫氣與碘產物生成效率示意圖。 圖5A與圖5B分別為本發明與對比例電流密度與標準電勢，以及標準電勢與電流密度的關係示意圖。 The invention will be further illustrated by way of exemplary embodiments which will be described in detail by means of the accompanying drawings. These examples are non-limiting, and in these examples, the same number indicates the same structure, wherein: Fig. 1 is a system diagram of a preferred embodiment of the present invention. Fig. 2 is a schematic diagram of the relationship between current density and voltage of the present invention and comparative examples. Fig. 3 is a schematic diagram of the relationship between voltage and current density of the present invention and comparative examples. 4A and 4B are schematic diagrams of the production efficiency of hydrogen and iodine products in the present invention, respectively. 5A and 5B are schematic diagrams showing the relationship between current density and standard potential, and standard potential and current density in the present invention and comparative examples, respectively.
100:低耗能產氫與碘衍生物的系統 100: A system for producing hydrogen and iodine derivatives with low energy consumption
101:陽極反應區 101: Anode reaction area
1011:陽極 1011: anode
1013:陽極反應液體 1013: anode reaction liquid
103:陰極反應區 103: Cathode reaction area
1031:陰極 1031: Cathode
1033:陰極反應液體 1033: cathode reaction liquid
1035:產出物出口 1035: Output export
105:液體 105: liquid
107:通透間隔元件 107: transparent spacer element
C:觸媒 C: Catalyst
Claims (8)
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