CN106602116A - Application of inorganic acids as additives for improving battery efficiency of vanadium battery - Google Patents
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- 229910052720 vanadium Inorganic materials 0.000 title claims abstract description 58
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 title claims abstract description 57
- 239000000654 additive Substances 0.000 title claims abstract description 29
- 150000007522 mineralic acids Chemical class 0.000 title abstract description 27
- 239000003792 electrolyte Substances 0.000 claims abstract description 55
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims abstract description 20
- 229910001456 vanadium ion Inorganic materials 0.000 claims abstract description 17
- 239000002994 raw material Substances 0.000 claims abstract description 14
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 claims abstract description 12
- 229910000147 aluminium phosphate Inorganic materials 0.000 claims abstract description 5
- XMBWDFGMSWQBCA-UHFFFAOYSA-N hydrogen iodide Chemical compound I XMBWDFGMSWQBCA-UHFFFAOYSA-N 0.000 claims abstract description 4
- 229940071870 hydroiodic acid Drugs 0.000 claims abstract description 4
- 230000000996 additive effect Effects 0.000 claims description 22
- 239000000203 mixture Substances 0.000 claims description 9
- 239000002253 acid Substances 0.000 claims 14
- 229910052500 inorganic mineral Inorganic materials 0.000 claims 14
- 239000011707 mineral Substances 0.000 claims 14
- 239000001117 sulphuric acid Substances 0.000 claims 2
- 235000011149 sulphuric acid Nutrition 0.000 claims 2
- 150000007513 acids Chemical class 0.000 claims 1
- 238000000034 method Methods 0.000 abstract description 6
- 238000004146 energy storage Methods 0.000 abstract description 5
- 238000004519 manufacturing process Methods 0.000 abstract description 2
- 230000001351 cycling effect Effects 0.000 abstract 1
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical group [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 12
- 238000003756 stirring Methods 0.000 description 5
- 229920000557 Nafion® Polymers 0.000 description 4
- 238000005562 fading Methods 0.000 description 4
- 229910002804 graphite Inorganic materials 0.000 description 4
- 239000010439 graphite Substances 0.000 description 4
- 230000010287 polarization Effects 0.000 description 4
- 238000007599 discharging Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 239000008151 electrolyte solution Substances 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000011263 electroactive material Substances 0.000 description 1
- 238000012983 electrochemical energy storage Methods 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- QFWPJPIVLCBXFJ-UHFFFAOYSA-N glymidine Chemical compound N1=CC(OCCOC)=CN=C1NS(=O)(=O)C1=CC=CC=C1 QFWPJPIVLCBXFJ-UHFFFAOYSA-N 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
- H01M8/184—Regeneration by electrochemical means
- H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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- Sustainable Development (AREA)
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- General Chemical & Material Sciences (AREA)
- Fuel Cell (AREA)
Abstract
Description
技术领域technical field
本发明涉及电池制造及能量存储领域，具体为一种无机酸作为提高钒电池电池效率添加剂的应用。The invention relates to the field of battery manufacturing and energy storage, in particular to the application of an inorganic acid as an additive for improving the efficiency of a vanadium battery.
背景技术Background technique
全钒氧化还原液流电池(简称钒电池)是一种新型的电化学储能系统，与传统的蓄电池相比，具有可快速、大容量充放电、自放电率低和电池结构简单等特点，它是满足风能、太阳能等新型能源大规模储能的理想电源形式之一。钒电池正负极电解液为含V4+/V5+与V2+/V3+氧化还原电对的硫酸溶液，它不仅是导电介质，更是实现能量存储的电活性物质，是钒电池储能及能量转化的核心。All-vanadium redox flow battery (referred to as vanadium battery) is a new type of electrochemical energy storage system. Compared with traditional batteries, it has the characteristics of fast, large-capacity charge and discharge, low self-discharge rate and simple battery structure. It is one of the ideal forms of power supply for large-scale energy storage of new energy sources such as wind energy and solar energy. The positive and negative electrode electrolytes of vanadium batteries are sulfuric acid solutions containing V 4+ /V 5+ and V 2+ /V 3+ redox couples. It is not only a conductive medium, but also an electroactive material for energy storage. The core of battery energy storage and energy conversion.
目前，使用的钒电池电解液钒浓度为1.5～2mol/L，硫酸为3mol/L左右，在钒电池充电运行过程中，由于钒电池电解液一直在系统中循环，一旦出现相变会造成液体流到管道和电池组内部管道的堵塞，影响系统的稳定运行；另外，由于钒离子在硫酸中的溶解度有限，在一定程度上限制了系统能量密度的提高。同时，由于正负极平衡电位升高速度的不同，导致电解液利用率较低，进而使得电解液容量衰减较快。如何提高电池效率，容量保持率并使其在电池运行过程中保持良好的稳定性成为亟待解决的问题。At present, the concentration of vanadium in the vanadium battery electrolyte is 1.5-2 mol/L, and the sulfuric acid is about 3 mol/L. During the charging and operation of the vanadium battery, since the vanadium battery electrolyte has been circulating in the system, once a phase change occurs, it will cause liquid The blockage of the flow pipes and the internal pipes of the battery pack affects the stable operation of the system; in addition, due to the limited solubility of vanadium ions in sulfuric acid, the improvement of the energy density of the system is limited to a certain extent. At the same time, due to the difference in the rising speed of the equilibrium potential of the positive and negative electrodes, the utilization rate of the electrolyte is low, and the capacity of the electrolyte decays rapidly. How to improve battery efficiency, capacity retention and maintain good stability during battery operation has become an urgent problem to be solved.
发明内容Contents of the invention
本发明的目的在于提供一种无机酸作为提高钒电池电池效率添加剂的应用，提高钒电池电解液的电导率和钒离子的活性，降低电化学极化。另外，也提高电池容量，以实现提高电池效率和稳定运行的目的。The purpose of the present invention is to provide an inorganic acid as an additive for improving the efficiency of the vanadium battery, improve the conductivity of the electrolyte of the vanadium battery and the activity of vanadium ions, and reduce the electrochemical polarization. In addition, the battery capacity is also increased to achieve the purpose of improving battery efficiency and stable operation.
本发明的技术方案是：Technical scheme of the present invention is:
一种无机酸作为提高钒电池电池效率添加剂的应用，以具有钒离子和硫酸的钒电池电解液为原料，在钒电池电解液中同时添加两种无机酸为电解液，无机酸为磷酸和氢碘酸，提高钒电池的电池效率。An application of an inorganic acid as an additive to improve the efficiency of a vanadium battery. The vanadium battery electrolyte with vanadium ions and sulfuric acid is used as a raw material, and two inorganic acids are added to the vanadium battery electrolyte at the same time as the electrolyte. The inorganic acids are phosphoric acid and hydrogen. Iodic acid, which improves the battery efficiency of vanadium batteries.
所述的无机酸作为提高钒电池电池效率添加剂的应用，原料中钒离子的价态为单一的五价、四价、三价或二价；或者，原料中钒离子的价态为四价和五价的混合物；或者，原料中钒离子的价态为四价和三价的混合物；或者，原料中钒离子的价态为三价和二价的混合物。In the application of the inorganic acid as an additive to improve the efficiency of vanadium batteries, the valence state of the vanadium ions in the raw material is a single pentavalent, tetravalent, trivalent or divalent; or, the valence state of the vanadium ions in the raw material is tetravalent and Pentavalent mixture; or, the valence state of vanadium ions in the raw material is a mixture of tetravalent and trivalent; or, the valence state of vanadium ions in the raw material is a mixture of trivalent and divalent.
所述的无机酸作为提高钒电池电池效率添加剂的应用，钒离子在钒电池电解液中的浓度为1～3mol/L。When the inorganic acid is used as an additive for improving the efficiency of the vanadium battery, the concentration of vanadium ions in the vanadium battery electrolyte is 1-3 mol/L.
所述的无机酸作为提高钒电池电池效率添加剂的应用，硫酸在钒电池电解液中的浓度为0.5～3mol/L。For the application of the inorganic acid as an additive for improving the battery efficiency of the vanadium battery, the concentration of sulfuric acid in the electrolyte solution of the vanadium battery is 0.5-3 mol/L.
所述的无机酸作为提高钒电池电池效率添加剂的应用，添加无机酸的浓度为H3PO4：0.1～3mol/L，HI：0.1～3mol/L。The application of the inorganic acid as an additive for improving the battery efficiency of the vanadium battery, the concentration of the added inorganic acid is H 3 PO 4 : 0.1-3 mol/L, HI: 0.1-3 mol/L.
所述的无机酸作为提高钒电池电池效率添加剂的应用，优选添加无机酸的浓度为H3PO4：0.5～1.7mol/L，HI：0.5～1.7mol/L。For the application of the inorganic acid as an additive for improving the battery efficiency of vanadium batteries, the concentration of adding the inorganic acid is preferably H 3 PO 4 : 0.5-1.7 mol/L, HI: 0.5-1.7 mol/L.
所述的无机酸作为提高钒电池电池效率添加剂的应用，无机酸加入后，搅拌30～60min。The application of the inorganic acid as an additive for improving the battery efficiency of the vanadium battery, after the inorganic acid is added, it is stirred for 30-60 minutes.
所述的无机酸作为提高钒电池电池效率添加剂的应用，无机酸在室温加入。The application of the inorganic acid as an additive for improving the battery efficiency of the vanadium battery is added at room temperature.
本发明的设计思想是：Design idea of the present invention is:
本发明以具有一定钒浓度和硫酸浓度的电解液为原料，在电解液中添加一定浓度的无机酸，一方面提高钒电池电解液的电导率和钒离子的活性，降低了电池充放电过程中的极化现象，实现了电池电压效率和能量效率的提高，另一方面能够有效增强电解液的稳定性，抑制了电池运行时的容量衰减问题，实现电池效率的提高和稳定运行。In the present invention, the electrolyte with a certain concentration of vanadium and sulfuric acid is used as a raw material, and a certain concentration of inorganic acid is added to the electrolyte, on the one hand, the conductivity of the electrolyte of the vanadium battery and the activity of vanadium ions are improved, and the process of charging and discharging the battery is reduced. The polarization phenomenon of the battery realizes the improvement of battery voltage efficiency and energy efficiency. On the other hand, it can effectively enhance the stability of the electrolyte, suppress the capacity fading problem during battery operation, and realize the improvement of battery efficiency and stable operation.
本发明的优点及有益效果是：Advantage of the present invention and beneficial effect are:
1、本发明工艺方法简单，操作容易且原料易得，成本低，可以得到稳定性好的钒电池电解液，并能提高钒电池的电池效率。1. The process method of the present invention is simple, the operation is easy, the raw materials are readily available, and the cost is low, the electrolyte solution of the vanadium battery with good stability can be obtained, and the battery efficiency of the vanadium battery can be improved.
2、使用无机酸作为添加剂，一方面提高了电解液的电导率，降低了电化学极化现象，提高了电池的电压效率和能量效率；另一方面能够有效增强电解液的稳定性，实现电池的稳定运行。2. Using inorganic acid as an additive, on the one hand, it improves the conductivity of the electrolyte, reduces the electrochemical polarization phenomenon, and improves the voltage efficiency and energy efficiency of the battery; on the other hand, it can effectively enhance the stability of the electrolyte and realize the battery stable operation.
附图说明Description of drawings
图1为实施例1中加入添加剂的充放电曲线。Fig. 1 is the charging and discharging curve of adding additive in embodiment 1.
具体实施方式detailed description
在具体实施方式中，本发明无机酸作为提高钒电池电池效率添加剂的应用，将无机酸为磷酸和氢碘酸作为提高钒电解液稳定性添加剂，以具有一定钒浓度和硫酸浓度的钒电池电解液为原料，钒离子的价态可以为单一的五价、四价、三价、二价或四价和五价的混合物，四价和三价的混合物及三价和二价的混合物，钒浓度为1～3mol/L，硫酸浓度为0.5～3mol/L，在电解液中添加一定浓度的无机酸，无机酸浓度为0.2～3mol/L(优选为0.5～1.7mol/L)，无机酸为H3PO4和HI。无机酸在室温加入后，搅拌30～60min，获得钒电池的电池效率指标范围如下：In a specific embodiment, the inorganic acid of the present invention is used as an additive for improving the efficiency of a vanadium battery, and the inorganic acid is phosphoric acid and hydroiodic acid as an additive for improving the stability of the vanadium electrolyte, and the electrolysis of the vanadium battery with a certain concentration of vanadium and sulfuric acid The valence state of vanadium ions can be single pentavalent, tetravalent, trivalent, divalent or a mixture of tetravalent and pentavalent, a mixture of tetravalent and trivalent, and a mixture of trivalent and divalent. The concentration is 1-3mol/L, the concentration of sulfuric acid is 0.5-3mol/L, add a certain concentration of inorganic acid in the electrolyte, the concentration of inorganic acid is 0.2-3mol/L (preferably 0.5-1.7mol/L), the inorganic acid For H 3 PO 4 and HI. After the inorganic acid is added at room temperature, stir for 30-60 minutes, and the battery efficiency index range of the vanadium battery is as follows:
电压效率VE＝80.3～88.6％，能量效率EE＝79.7～86.4％，50个充放电循环容量衰减为17.4～8.2％。The voltage efficiency VE=80.3-88.6%, the energy efficiency EE=79.7-86.4%, and the capacity decay of 50 charge-discharge cycles is 17.4-8.2%.
下面，通过实施例对本发明进一步详细阐述。Below, the present invention is described in further detail through examples.
实施例1Example 1
取1.1mol V5+、1.1mol V4+和2mol H2SO4混合价态电解液，加入0.8mol H3PO4和1molHI，室温搅拌30min后，倒入容量瓶中，定容至1000mL，得到1.1mol V5+、1.1mol V4+的混合价态钒电解液。另外，不含任何添加剂的原电解液作为空白电解液，分别组装钒电池。其中电池隔膜为nafion膜，电极为活性炭毡，双极板为石墨板，电流密度为80mAcm-1。单电池在室温下进行恒流充放电，截止电压为1.75V，由此得到如图1所示的电池充放电曲线。空白电解液对应的电池性能为：库仑效率CE＝98.6％，电压效率VE＝84.3％，能量效率EE＝83.1％；而本实施例中，添加H3PO4+HI的电解液对应的电池性能为CE＝98.8％，VE＝86.2％，EE＝85.0％。Take 1.1mol V 5+ , 1.1mol V 4+ and 2mol H 2 SO 4 mixed valence state electrolyte, add 0.8mol H 3 PO 4 and 1mol HI, stir at room temperature for 30min, pour it into a volumetric flask, and set the volume to 1000mL, A mixed valence state vanadium electrolyte of 1.1 mol V 5+ and 1.1 mol V 4+ was obtained. In addition, the original electrolyte without any additives was used as a blank electrolyte, and vanadium batteries were assembled respectively. The battery diaphragm is nafion film, the electrode is activated carbon felt, the bipolar plate is graphite plate, and the current density is 80mAcm -1 . The single battery is charged and discharged at a constant current at room temperature, and the cut-off voltage is 1.75V, thus obtaining the battery charge and discharge curve as shown in Figure 1. The battery performance corresponding to the blank electrolyte is: Coulombic efficiency CE = 98.6%, voltage efficiency VE = 84.3%, energy efficiency EE = 83.1%; and in this example, the battery performance corresponding to the electrolyte added with H 3 PO 4 +HI CE=98.8%, VE=86.2%, EE=85.0%.
实施例2Example 2
取1.8mol V5+和1mol H2SO4电解液，加入0.2mol H3PO4和0.4mol HI，室温搅拌30min后，倒入容量瓶中，定容至1000mL，得到1.8mol/L V5+的钒电解液。另外，不含任何添加剂的原电解液作为空白电解液，分别组装钒电池。其中电池隔膜为nafion膜，电极为活性炭毡，双极板为石墨板，电流密度为80mAcm-1。单电池在室温下进行恒流充放电，截止电压为1.75V。空白电解液对应的电池性能为：CE＝97.8％，VE＝82.5％，EE＝80.7％；而本实施例中，添加H3PO4+HI的电解液的电池性能为CE＝97.7％VE＝84.8％，EE＝82.8％。Take 1.8mol V 5+ and 1mol H 2 SO 4 electrolyte, add 0.2mol H 3 PO 4 and 0.4mol HI, stir at room temperature for 30min, pour it into a volumetric flask, and set the volume to 1000mL to obtain 1.8mol/LV 5+ vanadium electrolyte. In addition, the original electrolyte without any additives was used as a blank electrolyte, and vanadium batteries were assembled respectively. The battery diaphragm is nafion film, the electrode is activated carbon felt, the bipolar plate is graphite plate, and the current density is 80mAcm -1 . The single cell is charged and discharged at a constant current at room temperature, and the cut-off voltage is 1.75V. The battery performance corresponding to the blank electrolyte is: CE=97.8%, VE=82.5%, EE=80.7%; and in this example, the battery performance of the electrolyte added with H 3 PO 4 +HI is CE=97.7%VE= 84.8%, EE=82.8%.
实施例3Example 3
取1.5mol V4+、1.5mol V3+和1.5mol H2SO4混合价态电解液，加入1mol H3PO4和0.6mol HI，室温搅拌30min后，倒入容量瓶中，定容至1000mL，得到1.5molV4+、1.5mol V3+的混合价态钒电解液。另外，不含任何添加剂的原电解液作为空白电解液，分别组装钒电池。其中电池隔膜为nafion膜，电极为活性炭毡，双极板为石墨板，电流密度为80mAcm-1。单电池在室温下进行恒流充放电，截止电压为1.75V。空白电解液对应的电池性能为：CE＝98.2％，VE＝84.6％，EE＝83.1％；而本实施例中，添加H3PO4+HI的电解液的电池性能为CE＝98.7％，VE＝86.8％，EE＝85.7％。Take 1.5mol V 4+ , 1.5mol V 3+ and 1.5mol H 2 SO 4 mixed valence electrolyte, add 1mol H 3 PO 4 and 0.6mol HI, stir at room temperature for 30min, pour it into a volumetric flask, and set the volume to 1000mL, a mixed valence state vanadium electrolyte of 1.5mol V 4+ and 1.5mol V 3+ was obtained. In addition, the original electrolyte without any additives was used as a blank electrolyte, and vanadium batteries were assembled respectively. The battery diaphragm is nafion film, the electrode is activated carbon felt, the bipolar plate is graphite plate, and the current density is 80mAcm -1 . The single cell is charged and discharged at a constant current at room temperature, and the cut-off voltage is 1.75V. The battery performance corresponding to the blank electrolyte is: CE=98.2%, VE=84.6%, EE=83.1%. In this example, the battery performance of the electrolyte with H 3 PO 4 +HI is CE=98.7%, VE =86.8%, EE=85.7%.
实施例4Example 4
取2.0mol V4+和1mol H2SO4电解液，加入0.8mol H3PO4和0.6mol HI，室温搅拌30min后，倒入容量瓶中，定容至1000mL，得到2mol/L V4+的钒电解液。另外，不含任何添加剂的原电解液作为空白电解液。分别组装钒电池。其中电池隔膜为nafion膜，电极为活性炭毡，双极板为石墨板，电流密度为80mAcm-1。单电池在室温下进行恒流充放电，截止电压为1.75V，考察电池容量衰减情况。50个充放电循环容量衰减结果可以看出，空白电解液容量衰减较快，约衰减18.5％；而本实施例中，添加H3PO4+HI的电解液的电池容量衰减仅为10.3％。Take 2.0mol V 4+ and 1mol H 2 SO 4 electrolyte, add 0.8mol H 3 PO 4 and 0.6mol HI, stir at room temperature for 30min, pour it into a volumetric flask, and set the volume to 1000mL to obtain 2mol/LV 4+ Vanadium electrolyte. In addition, the original electrolyte without any additives was used as a blank electrolyte. Vanadium batteries were assembled separately. The battery diaphragm is nafion film, the electrode is activated carbon felt, the bipolar plate is graphite plate, and the current density is 80mAcm -1 . The single battery is charged and discharged at a constant current at room temperature, and the cut-off voltage is 1.75V, and the capacity decay of the battery is investigated. From the results of capacity fading after 50 charge-discharge cycles, it can be seen that the capacity fading of the blank electrolyte is faster, about 18.5%; while in this example, the capacity fading of the electrolyte added with H 3 PO 4 +HI is only 10.3%.
表1.空白电解液与加入添加剂电解液效率Table 1. Efficiency of blank electrolyte and electrolyte with additives
如表1所示，实施例结果表明，本发明通过加入磷酸和氢碘酸，能够有效提高电解液导电率，增强电解液稳定性，抑制电池自放电率，减缓电池容量衰减，减小电化学极化，很大程度上提高了电池效率。As shown in Table 1, the results of the examples show that the present invention can effectively improve the conductivity of the electrolyte by adding phosphoric acid and hydroiodic acid, enhance the stability of the electrolyte, inhibit the self-discharge rate of the battery, slow down the capacity decay of the battery, and reduce the electrochemical Polarization greatly improves the battery efficiency.
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