CN1357934A - Manganese dioxide electrode and primary alkaline zinc-manganese battery thereof - Google Patents
Manganese dioxide electrode and primary alkaline zinc-manganese battery thereof Download PDFInfo
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- CN1357934A CN1357934A CN00130847A CN00130847A CN1357934A CN 1357934 A CN1357934 A CN 1357934A CN 00130847 A CN00130847 A CN 00130847A CN 00130847 A CN00130847 A CN 00130847A CN 1357934 A CN1357934 A CN 1357934A
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Abstract
The invention relates to a manganese dioxide electrode applied to a zinc-manganese battery, which comprises an electrode substance, wherein the electrode substance comprises manganese dioxide, graphite, a binder and an additive, the additive comprises at least one of substance groups consisting of oxides of vanadium, niobium, tantalum and titanium, and the addition amount is 0.1-5 wt% relative to the electrode substance.
Description
The invention relates to a manganese dioxide electrode applied to a zinc-manganese battery, in particular to an electrode additive in the manganese dioxide electrode; the invention also relates to a primary alkaline zinc-manganese battery with the manganese dioxide electrode.
The production and application of zinc-manganese battery have been in history for hundreds of years, but the technology of the disclosed zinc-manganese battery product and manufacturing method is generally directed to the primary alkaline zinc-manganese battery, while the product and production technology of the secondary alkaline zinc-manganese battery are developed in recent years. Among them, regarding the technical improvement of manganese dioxide electrode of zinc-manganese battery, chinese patent CN1123584A published in 1996, 5.29.discloses an improvement method for manganese dioxide electrode of primary alkaline zinc-manganese battery, namely adding 0.1-5wt% of anatase titanium dioxide in the conventional manganese dioxide cathode, and obtaining about 5% improvement of effective life in AA (LR 6) type zinc-manganese battery test; however, the inventor of the present invention has found that the added titanium dioxide is preferable and has better effect, and other metal oxide additives with semiconductor electrical property can also be selected to obtain good improvement effect. Therefore, the temperature of the molten steel is controlled,
the invention aims to solve the problem of poor electrochemical conversion performance of manganese dioxide in the discharge process, and provides a manganese dioxide electrode applied to a zinc-manganese battery;
it is a further object of the present invention to provide a primary alkaline zinc-manganese battery containing the manganese dioxide electrode, which is improved in medium and high rate discharge performance and pulse discharge performance.
The invention relates to a manganese dioxide electrode applied to a zinc-manganese battery, which comprises an electrode material, wherein the electrode material comprises manganese dioxide, graphite, a binder and an additive, and is characterized in that: the additive comprises at least one of the substances of vanadium, niobium, tantalum and titanium oxide, wherein the titanium oxide is anatase titanium dioxide with the purity of more than 99.99% and the fineness of 1-100 nanometers. The above-mentioned additives, which are respectively preferred, include: vanadium pentoxide, niobium pentoxide, tantalum pentoxide and anatase titanium dioxide with purity of more than 99.99% and fineness of 1-100 nm.
In the manganese dioxide electrode of the present invention, the additive is preferably added in an amount of 0.1 to 5wt%, particularly preferably 0.5 to 2wt%, based on the weight percentage of the electrode material.
The primary alkaline zinc-manganese battery containing the manganese dioxide electrode comprises a zinc anode, a manganese dioxide cathode, a diaphragm, alkaline electrolyte and a battery container, wherein the manganese dioxide cathode comprises an electrode material, and the electrode material comprises manganese dioxide, graphite, a binder and an additive, and is characterized in that: the additive comprises at least one of the substances consisting of oxides of vanadium, niobium, tantalum and titanium, wherein the oxide of titanium is anatase titanium dioxide with the purity of more than 99.99 percent and the fineness of 1-100 nanometers. The above-mentioned additives, which are respectively preferred, include: vanadium pentoxide, niobium pentoxide, tantalum pentoxide and anatase titanium dioxide with purity of more than 99.99% and fineness of 1-100 nm.
The additive is added in the primary alkaline zinc-manganese dioxide battery of the invention, the weight percentage of the additive relative to the electrode material is preferably 0.1-5wt%, particularly preferably 0.5-2wt%,
it is not known how to improve the pulse discharge and medium and high rate discharge performance of the primary alkaline zinc-manganese dioxide battery using the additive, but it is thought preliminarily that the primary alkaline zinc-manganese dioxide battery is doped with A-TiO 2 、V 2 O 5 、 Nb 2 O 5 、Ta 2 O 5 Improves MnO 2 The ionic mobility of the trivalent manganese complex ions in solution, which are formed during the discharge, causes the reduction products to leave the surface of the active material at a faster rate in the electric field, resulting in an increase in the following reaction (I): the effect represented on the polarization curve of the battery discharge is then: 1. MnO due to accelerated MnOOH leaving the active material surface x Tetravalent manganese in the particles transfers to the surface layer, protons (H) + ) And the time required for electrons to enter crystal lattices is shortened, so that the cathode polarization is reduced, the discharge platform is improved, and the medium and high rate discharge time of the zinc-manganese battery is prolonged by 5-10%; 2. for pulse discharge, the lower limit of the discharge plateau is raised by 1 in the discharge period due to MnOOH (dissolved into [ Mn (OH)) 4 ] - ) Is removed so that MnO is x The average valence of medium Mn is increased, so that the open-circuit voltage of the battery is quickly increased in the discharge intermittent period, namely the upper limit of a discharge platform is also increased, and the pulse frequency of the zinc-manganese battery is increased by 4-9% in general.
Specific embodiments of the present invention are described below, but it should be understood that the present invention is not limited to these embodiments, and the scope of the claims and their equivalents are also reflected. Comparative example 1:
manufacturing a battery: an LR6 (AA type) primary alkaline zinc-manganese battery (also called alkaline-manganese battery for short) is prepared from electrolytic manganese dioxide (MnO for short) through conventional process 2 ) The graphite comprises the following components in percentage by weight: 85: 15, adding 30wt% potassium hydroxide (KOH) aqueous solution 8 wt% of the mixture, mixing, grinding, and pulverizing to obtain the final product containing MnO 2 A cathode ring; mixing commercially available mercury-free zinc powder with binder such as carboxymethylcellulose sodium salt (CMC) and sodium polyacrylate, dry-pulverizing at ratio of 97: 3, vacuumizing, and adding zinc oxide (CMC) prepared in advanceZnO) saturated 41wt% koh mixed solution, mixed under vacuum to form anode paste, and cathode ring, anode paste, and separator combined by conventional method to form LR6 alkaline manganese cell A0.
And (3) testing the battery: the LR6 alkaline manganese battery discharge performance is tested according to the discharge condition of the Chinese national standard GB/T7112-1998:
1. pulse discharge performance (abbreviated as D) Pulse of light ): pulse discharge is carried out under the load of 1.8 omega for 15 seconds and the discharge is left for 45 seconds, the cut-off voltage is 0.9V, and the pulse frequency is 580 times (calculated by 100 percent);
2. high current discharge performance (D for short) suitable for motor/toy Big (a) ): continuously discharged to 0.8V under a load of 3.9 Ω, and the discharge time was measured to be 6.8 hours (in 100%);
3. medium current discharge performance (D for short) suitable for recorder In ): discharge was continued to 0.9V under a load of 10.0 Ω, and the discharge time was measured to be 17.6 hours (in 100%).
Comparative examples 2 to 8:
manufacturing a battery: referring to the method of comparative example 1, common commercially available anatase type titanium dioxide having a fineness of 200 to 400 nm was added to the cathode in an amount of 0.01, 0.1, 0.5, 1, 2, 5, 7% by weight of the entire cathode material while reducing MnO 2 In such an amount that the weight of the cathode in this example is the same as that in the comparative example, reference numeral a 1 、a 2 、a 3 、a 4 、a 5 、a 6 、a 7 LR6 alkaline zinc-manganese dioxide battery of (1);
and (3) testing the battery: the discharge performance of the LR6 alkaline manganese battery was measured under the discharge conditions according to the chinese national standard GB/T7112-1998, and the number of pulse discharges was measured as 100, 101, 102, 103, 99, and 94% in percentage terms with respect to comparative example 1, and the discharge times of large current were measured as 100, 101, 104, 103, 97, and 92% in percentage terms, and the discharge times of medium current were measured as 100, 101, 103, 101, 97, and 90% in percentage terms.
Examples 1 to 7:
manufacturing a battery: referring to the method of the comparative example, anatase titanium dioxide (abbreviated as A-TiO) with a purity of more than 99.99% and a fineness of 1-100 nm, which accounts for 0.01, 0.1, 0.5, 1, 2, 5, 7% of the total weight of the cathode material, is added to the cathode 2 ) While reducing MnO 2 In such an amount that the weight of the cathode in this example is the same as that in the comparative example, reference numeral A 1 、A 2 、A 3 、A 4 、A 5 、A 6 、A 7 LR6 alkaline zinc-manganese dioxide battery of (1);
and (3) testing the battery: the discharge performance of the LR6 alkaline manganese battery is tested according to the discharge condition of Chinese national standard GB/T7112-1998, the measured pulse discharge times are respectively 100, 102, 106, 108, 105, 103 and 96 percent, the measured high-current discharge time is respectively 101, 102, 105, 110, 106, 102 and 97 percent, and the measured medium-current discharge time is respectively 101, 103, 104, 107, 103, 101 and 98 percent.
The discharge properties of comparative examples 1-8 and examples 1-7 were compared as shown in Table one:
| A 0 | a 1 | a 2 | a 3 | a 4 | a 5 | a 6 | a 7 | A 1 | A 2 | A 3 | A 4 | A 5 | A 6 | A 7 | |
| D pulse of light | 100 | 100 | 100 | 101 | 102 | 103 | 99 | 94 | 100 | 102 | 106 | 108 | 105 | 103 | 96 |
| D Big (a) | 100 | 100 | 100 | 101 | 104 | 103 | 97 | 92 | 101 | 102 | 105 | 110 | 106 | 102 | 97 |
| D In | 100 | 100 | 100 | 101 | 103 | 101 | 97 | 90 | 101 | 103 | 104 | 107 | 103 | 101 | 98 |
From table one, it can be derived: anatase titanium dioxide with purity of more than 99.99% and fineness of 1-100 nm is added into manganese dioxide cathode of alkaline manganese cell to improve high-rate discharge performance and pulse discharge performance, compared with no additive, D Pulse of light Increased by 2-8%, D Big (a) Increased by 2-10%, D In The improvement is 2 to 7 percent; compared with ordinary titanium dioxide, D Pulse of light Increased by 2-5%, D Big (a) The improvement is 2 to 6 percent,D in (1) The improvement is 2 to 4 percent.
Examples 8 to 14:
manufacturing a battery: vanadium pentoxide (V for short) 2 O 5 ) Instead of A-TiO 2 Reference numerals B were prepared in accordance with the methods of examples 1 to 7 1 、B 2 、B 3 、B 4 、B 5 、B 6 、B 7 LR6 alkaline zinc manganese cell of (1);
and (3) testing the battery: the discharge performance of the LR6 alkaline manganese battery is tested according to the discharge condition of the Chinese national standard GB/T7112-1998 and is shown in the attached table II:
examples 15 to 21:
manufacturing a battery: niobium pentoxide (Nb for short) 2 O 5 ) Instead of A-TiO 2 Reference numerals C were prepared according to the methods described in examples 1 to 7 1 、C 2 、C 3 、C 4 、C 5 、C 6 、C 7 LR6 alkaline zinc manganese cell of (1);
and (3) testing the battery: the discharge performance of the LR6 alkaline manganese battery is tested according to the discharge condition of the Chinese national standard GB/T7112-1998 and is shown in the attached table II:
examples 22 to 28:
manufacturing a battery: by tantalum pentoxide (Ta for short) 2 O 5 ) Instead of A-TiO 2 Reference is made to the corresponding method of examples 1 to 7, reference numeral D 1 、D 2 、D 3 、D 4 、D 5 、D 6 、D 7 LR6 alkaline zinc manganese cell of (1);
and (3) testing the battery: the discharge performance of the LR6 alkaline manganese battery is tested according to the discharge condition of the Chinese national standard GB/T7112-1998 and is shown in the attached table II:
the discharge properties of examples 8-28 are compared as in Table two:
| B 1 | B 2 | B 3 | B 4 | B 5 | B 6 | B 7 | |
| D | 100 | 102 | 103 | 105 | 104 | 102 | 96 |
| D pulse of light | 100 | 102 | 104 | 107 | 105 | 101 | 94 |
| D In (1) | 100 | 101 | 102 | 104 | 102 | 100 | 97 |
| C 1 | C 2 | C 3 | C 4 | C 5 | C 6 | C 7 | |
| D Big (a) | 100 | 103.5 | 105 | 108 | 103.5 | 102 | 95 |
| D Pulse of light | 101 | 102 | 104.5 | 106.5 | 104.5 | 101 | 93 |
| D In | 101 | 101 | 101.5 | 102.5 | 102 | 100 | 97 |
| D 1 | D 2 | D 3 | D 4 | D 5 | D 6 | D 7 | |
| D Big (a) | 101 | 101 | 101.5 | 106.5 | 105 | 102 | 98 |
| D Pulse of light | 100 | 100 | 102.5 | 105 | 104.5 | 101 | 96 |
| D In | 100 | 100 | 102 | 104.5 | 103.5 | 101 | 95 |
From table two, it can be derived:
with V 2 O 5 Instead of A-TiO 2 D, in comparison with no additive Pulse of light Increased by 2-7%, D Big (a) Increased by 2-5%, D In The improvement is 2 to 4 percent;
by Nb 2 O 5 Instead of A-TiO 2 D, compared with no additive Pulse of light Increased by 2-6%, D Big (a) Increased by 2-8%, D In The improvement is 2 to 3 percent;
with Ta 2 O 5 In place of A-TiO 2 D, in comparison with no additive Pulse of light Increased by 2-7%, D Big (a) Increased by 2-5%, D In (1) The improvement is 2 to 4 percent;
examples 22 to 28:
manufacturing a battery:
compositions with the following oxides respectively:
(0.5％TiO 2 +0.5％V 2 O 5 )、
(0.5％TiO 2 +0.5％Nb 2 O 5 )、
(0.5％TiO 2 +0.5％Ta 2 O 5 )、
(0.5％Nb 2 O 5 +0.5％V 2 O 5 )、
(0.5％Nb 2 O 5 +0.5％Ta 2 O 5 )、
(0.5％V 2 O 5 +0.5％Ta 2 O 5 )、
(0.5％TiO 2 +0.5％Ta 2 O 5 +0.5％Nb 2 O 5 )、
(0.5％Ta 2 O 5 +0.5％Nb 2 O 5 +0.5％V 2 O 5 )、
(0.5％TiO 2 +0.5％V 2 O 5 +0.5％Nb 2 O 5 ) Instead of TiO 2 Reference example 1 was made to corresponding method No. E 1 、E 2 、E 3 、E 4 、E 5 、 E 6 、E 7 、E 8 、E 9 LR6 alkaline zinc-manganese dioxide battery of (1);
and (3) testing the battery: the discharge performance of the LR6 alkaline manganese battery is tested according to the discharge condition of the Chinese national standard GB/T7112-1998 and is shown in the attached table III:
| E 1 | E 2 | E 3 | E 4 | E 5 | E 6 | E 7 | E 8 | E 9 | |
| D pulse of light | 108 | 109 | 107.5 | 108 | 104 | 108 | 105 | 103.5 | 106 |
| D Big (a) | 111 | 110 | 109 | 107 | 109 | 106 | 107 | 106 | 108 |
| D In (1) | 105.5 | 106.5 | 106 | 104 | 105 | 105.5 | 103.5 | 104.5 | 105 |
From table three, it can be derived: with 1% or 1.5% of the above-mentioned oxide composition as additive, D is compared with the additive-free composition Pulse of light Increased by 4-9%, D Big (a) Increased by 6-10%, D In The improvement is 4 to 6 percent.
Claims (12)
1. A manganese dioxide electrode applied to a zinc-manganese battery comprises an electrode material, wherein the electrode material comprises manganese dioxide, graphite and an additive, and is characterized in that: the additive comprises at least one of the substances consisting of oxides of vanadium, niobium, tantalum and titanium, wherein the oxide of titanium is anatase titanium dioxide with the purity of more than 99.99 percent and the fineness of 1-100 nanometers.
2. The manganese dioxide electrode of claim 1, wherein: the additive is added in an amount of 0.1 to 5wt% with respect to the weight percentage of the electrode material.
3. The manganese dioxide electrode according to claim 2, characterized in that: the additive is added in an amount of 0.5 to 2wt% with respect to the weight percentage of the electrode material.
4. The manganese dioxide electrode as set forth in claim 1, wherein: the vanadium oxide of the additive comprises vanadium pentoxide.
5. The manganese dioxide electrode as set forth in claim 1, wherein: the niobium oxide of the additive includes niobium pentoxide.
6. The manganese dioxide electrode of claim 1, wherein: the tantalum oxide of the additive comprises tantalum pentoxide.
7. A primary alkaline zinc manganese cell containing a manganese dioxide electrode as in claim 1, comprising a zinc anode, a manganese dioxide cathode, a separator, an alkaline electrolyte and a cell container, said manganese dioxide cathode comprising an electrode material, said electrode material comprising manganese dioxide, graphite and additives, characterized in that: the additive comprises at least one of the substances consisting of oxides of vanadium, niobium, tantalum and titanium, wherein the oxide of the titanium is anatase titanium dioxide with the purity of more than 99.99 percent and the fineness of 1-100 nanometers.
8. The zinc-manganese cell of claim 7, wherein: the additive is added in an amount of 0.1 to 5wt% with respect to the weight percent of the electrode material.
9. The zinc-manganese cell of claim 8, wherein: the additive is added in an amount of 0.5 to 2wt% with respect to the weight percent of the electrode material.
10. The zinc-manganese cell of claim 7, wherein: the vanadium oxide of the additive comprises vanadium pentoxide.
11. The zinc-manganese cell of claim 7, wherein: the niobium oxide of the additive includes niobium pentoxide.
12. The zinc-manganese electrical ground of claim 7, wherein: the tantalum oxide of the additive comprises tantalum pentoxide.
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1300870C (en) * | 2004-11-08 | 2007-02-14 | 中国地质大学（武汉） | Electrolytic manganese dioxide for doped modified lithium manganese dioxide buttery |
| CN102097662A (en) * | 2009-12-11 | 2011-06-15 | 清华大学深圳研究生院 | Zinc ion battery |
| CN102110858A (en) * | 2009-12-29 | 2011-06-29 | 清华大学深圳研究生院 | Chargeable zinc ion battery by taking oxide of vanadium as cathode |
| CN102569751A (en) * | 2010-12-08 | 2012-07-11 | 比亚迪股份有限公司 | Alkaline manganese battery positive electrode material and alkaline manganese battery |
| CN102683757A (en) * | 2011-03-15 | 2012-09-19 | 清华大学深圳研究生院 | High-capacity rechargeable zinc ion battery |
-
2000
- 2000-12-13 CN CNB001308475A patent/CN1198351C/en not_active Expired - Fee Related
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1300870C (en) * | 2004-11-08 | 2007-02-14 | 中国地质大学（武汉） | Electrolytic manganese dioxide for doped modified lithium manganese dioxide buttery |
| CN102097662A (en) * | 2009-12-11 | 2011-06-15 | 清华大学深圳研究生院 | Zinc ion battery |
| CN102097662B (en) * | 2009-12-11 | 2013-05-29 | 清华大学深圳研究生院 | Zinc ion battery |
| CN102110858A (en) * | 2009-12-29 | 2011-06-29 | 清华大学深圳研究生院 | Chargeable zinc ion battery by taking oxide of vanadium as cathode |
| CN102110858B (en) * | 2009-12-29 | 2013-04-17 | 清华大学深圳研究生院 | Chargeable zinc ion battery by taking oxide of vanadium as cathode |
| CN102569751A (en) * | 2010-12-08 | 2012-07-11 | 比亚迪股份有限公司 | Alkaline manganese battery positive electrode material and alkaline manganese battery |
| CN102683757A (en) * | 2011-03-15 | 2012-09-19 | 清华大学深圳研究生院 | High-capacity rechargeable zinc ion battery |
| CN102683757B (en) * | 2011-03-15 | 2014-10-22 | 清华大学深圳研究生院 | High-capacity rechargeable zinc ion battery |
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| CN1198351C (en) | 2005-04-20 |
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