CN111883835A - Non-aqueous electrolyte of lithium ion battery and lithium ion battery - Google Patents
Non-aqueous electrolyte of lithium ion battery and lithium ion battery Download PDFInfo
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
- H01M10/0566—Liquid materials
- H01M10/0567—Liquid materials characterised by the additives
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0025—Organic electrolyte
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Abstract
The invention provides a lithium ion battery non-aqueous electrolyte and a lithium ion battery. The special additive can improve the oxidation stability of the electrolyte under the high-temperature condition, and can reduce the reductive decomposition of the electrolyte solvent to a certain extent so as to improve the high-temperature performance of the lithium ion battery, and has wide market application prospect.
Description
Technical Field
The invention belongs to the field of lithium ion batteries, and particularly relates to a lithium ion battery non-aqueous electrolyte and a lithium ion battery.
Background
Along with the progress of human civilization, people increasingly move to the living standard with high quality and high safety, and the development of new energy automobiles, power energy storage and high-performance digital products is a necessary condition for improving the living quality of people, so that higher requirements are made on the performance and the application range of the battery, and the lithium ion battery which can meet the increasing demand is required to be developed. It is particularly important to improve the cycle life and temperature applicability of the battery.
Disclosure of Invention
In view of the defects of the prior art, the invention aims to provide a lithium ion battery nonaqueous electrolyte and a lithium ion battery. The lithium ion battery non-aqueous electrolyte has good cycle characteristics and less gas generation in high-temperature storage, and solves the problems of too fast cycle capacity attenuation and severe high-temperature gas expansion of the conventional lithium ion battery non-aqueous electrolyte.
In order to achieve the purpose, the invention adopts the following technical scheme:
in one aspect, the invention provides a lithium ion battery nonaqueous electrolyte, which comprises a methyl bis-sulfonyl diamino methane bis-lithium additive with a structure shown in formula I:
the synthetic route is as follows:
the specific synthesis steps are as follows: mixing a mixture of 1: 1, mixing the methyl disulfonic acid with diaminomethane, then reacting for 4-8 hours at the temperature of 40-70 ℃, adding lithium hydroxide after the reaction is finished, and reacting for 1-2 hours to obtain the methyl bis-sulfonyldiamino methane bis-lithium salt.
In the invention, the special additive can improve the oxidation stability of the electrolyte under the high-temperature condition, and can reduce the reductive decomposition of the electrolyte solvent to a certain extent so as to improve the high-temperature performance of the lithium ion battery.
In the present invention, the nonaqueous electrolytic solution refers to a nonaqueous organic solvent as a solvent contained in the electrolytic solution.
Preferably, the mass percentage of the methyldisulfonyldiaminomethanedilithium additive is 0.1-5%, for example, 0.1%, 0.3%, 0.5%, 0.8%, 1%, 1.5%, 1.8%, 2%, 2.5%, 2.8%, 3%, 3.5%, 3.8%, 4%, 4.5%, 4.8% or 5%, based on 100% of the total mass of the lithium ion battery nonaqueous electrolyte.
Preferably, the solvent in the lithium ion nonaqueous electrolyte is selected from any one of ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate or propyl methyl carbonate or a combination of at least two of the ethylene carbonate, the propylene carbonate, the butylene carbonate, the dimethyl carbonate, the diethyl carbonate, the ethyl methyl carbonate or the propyl methyl carbonate.
Preferably, the lithium ion battery non-aqueous electrolyte further comprises other additives besides the methyl bis-sulfonyl diamino methane bis-lithium additive.
Preferably, the other additive is at least one of unsaturated cyclic carbonate ester compounds or sultone compounds.
Preferably, the unsaturated cyclic carbonate-based compound includes at least one of vinylene carbonate (abbreviated as VC) and vinyl ethylene carbonate (abbreviated as VEC).
Preferably, the sultone compound comprises at least one of 1, 3-Propane Sultone (PS) or 1, 4-butane sultone.
Preferably, the unsaturated cyclic carbonate compound is contained in an amount of 0.1 to 5% by mass, for example, 0.1%, 0.3%, 0.5%, 0.8%, 1%, 1.5%, 1.8%, 2%, 2.5%, 2.8%, 3%, 3.5%, 3.8%, 4%, 4.5%, 4.8% or 5% by mass based on 100% by mass of the total nonaqueous electrolyte solution of the lithium ion battery.
Preferably, the content of the sultone-based compound is 0.1 to 5% by mass, for example, 0.1%, 0.3%, 0.5%, 0.8%, 1%, 1.5%, 1.8%, 2%, 2.5%, 2.8%, 3%, 3.5%, 3.8%, 4%, 4.5%, 4.8% or 5% by mass based on 100% by mass of the total nonaqueous electrolyte of the lithium ion battery.
Preferably, the lithium ion nonaqueous electrolyte further comprises a lithium salt additive, and the lithium salt additive is selected from LiBOB (bis (oxalato) borate), LiFSI (difluorosulfonimide lithium), LiODFB (difluorooxalato lithium borate), LiBF4 (tetrafluoroborato lithium borate), LiPO2F2Any one of (lithium difluorophosphate) or LiDFOP (lithium difluorobis (oxalato) phosphate) or a combination of at least two of them.
Preferably, the mass percentage of the lithium salt additive is 0.1-5% based on 100% of the total mass of the lithium ion battery non-aqueous electrolyte; e.g., 0.1%, 0.3%, 0.5%, 0.8%, 1%, 1.5%, 1.8%, 2%, 2.5%, 2.8%, 3%, 3.5%, 3.8%, 4%, 4.5%, 4.8%, or 5%.
Preferably, the lithium ion nonaqueous electrolyte comprises a lithium salt electrolyte, and the lithium salt electrolyte is preferably LiPF6。
Preferably, the lithium ion battery nonaqueous electrolyte contains 0.1 to 20% by mass of a lithium salt electrolyte, for example, 0.1%, 0.5%, 0.8%, 1%, 2%, 3%, 5%, 7%, 9%, 10%, 12%, 15%, 18% or 20%.
In another aspect, the present invention provides a lithium ion battery, including a positive electrode, a negative electrode, a separator disposed between the positive electrode and the negative electrode, and an electrolyte, wherein the electrolyte is the above-mentioned lithium ion battery non-aqueous electrolyte.
In the present invention, the positive electrode, the negative electrode, and the separator are not particularly limited, and any of the positive electrode, the negative electrode, and the separator that are conventional in the art can be used.
Preferably, the positive electrode includes an active material that is LiNixCoyMnzL(1-x-y-z)O2、LiCox'L(1-x')O2、LiNix”Ly'Mn(2-x”-y')O4、Liz'MPO4At least one of; wherein L is at least one of Co, Al, Sr, Mg, Ti, Ca, Zr, Zn, Si and Fe, x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, z is more than 0 and less than or equal to 1, x + y + z is more than 0 and less than or equal to 1, x 'is more than 0 and less than or equal to 1, x is more than 0.3 and less than or equal to 0.6, and y' is more than 0.01 and less than or equal to 0.2; z' is more than or equal to 0.5 and less than or equal to 1, and M is at least one of Fe, Mn and Co.
The lithium ion battery non-aqueous electrolyte provided by the invention effectively improves the cycle and high-temperature storage performance of the battery, and the lithium ion battery containing the non-aqueous electrolyte has excellent cycle performance and high-temperature storage performance.
Compared with the prior art, the invention has the following beneficial effects:
the lithium ion battery non-aqueous electrolyte contains the methyl bis-sulfonyl diamino methane dilithium additive, so that the electrolyte has stable performance, the cycle performance of the battery is improved when the lithium ion battery non-aqueous electrolyte is applied to the lithium ion battery, the high-temperature performance of the battery is improved, the gas generation of the lithium ion battery in high-temperature storage is less, the problems of too fast cycle capacity attenuation and serious high-temperature ballooning of the conventional lithium ion battery non-aqueous electrolyte are solved, and the lithium ion battery non-aqueous electrolyte has wide market application prospect.
Detailed Description
The technical solution of the present invention is further explained by the following embodiments. It should be understood by those skilled in the art that the examples are only for the understanding of the present invention and should not be construed as the specific limitations of the present invention.
Example 1
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Example 2
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Example 3
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP (polypropylene) diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Example 4
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Example 5
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Example 6
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Example 7
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Example 8
LiNi0.5Co0.2Mn0.3O2The artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is non-aqueous electricityAn electrolyte solution, wherein the total weight of the nonaqueous electrolyte solution is 100%, and the nonaqueous electrolyte solution contains the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Example 9
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Comparative example 1
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Comparative example 2
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Comparative example 3
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Comparative example 4
LiNi0.5Co0.2Mn0.3O2Artificial graphiteThe battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the battery comprises the components with the mass percentage content shown in example 1 in Table 1 and 12% of LiPF6And (3) salt.
Comparative example 5
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Comparative example 6
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Comparative example 7
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
Comparative example 8
LiNi0.5Co0.2Mn0.3O2An artificial graphite battery comprises a ternary NCM523 positive electrode material, an artificial graphite negative electrode, a PP diaphragm and an electrolyte, wherein the electrolyte is a non-aqueous electrolyte, the total weight of the non-aqueous electrolyte is 100%, and the artificial graphite battery comprises the components with the mass percentage content shown in the example 1 in the table 1 and 12% of LiPF6And (3) salt.
The performance tests of the examples 1-9 and the comparative examples 1-8 of the invention are carried out, and the test indexes and the test method are as follows:
(1) the cycle performance is shown by testing the capacity retention rate of 1C cycle at 45 ℃ for N times, and the specific method comprises the following steps: the battery after formation (which can be used after activation) is charged to 4.35V (LiNi) at 45 ℃ with a 1C constant current and constant voltage0.5Co0.2Mn0.3O2Artificial graphite), the off current was 0.02C, and then the discharge was made to 3.0V with a constant current of 1C. After such charge/discharge cycles, the capacity retention rate after 200 weeks' cycles was calculated to evaluate the high-temperature cycle performance thereof.
The calculation formula of the capacity retention rate after 200 cycles at 45 ℃ is as follows:
the 200 th cycle capacity retention (%) was (200 th cycle discharge capacity/1 st cycle discharge capacity) × 100%
(2) The cycle performance is shown by testing the capacity retention rate of the cycle at 25 ℃ and 1C for N times, and the specific method comprises the following steps: the formed battery was charged to 4.35V (LiNi) at 25 ℃ with a 1C constant current and a constant voltage0.5Co0.2Mn0.3O2Artificial graphite), the off current was 0.02C, and then the discharge was made to 3.0V with a constant current of 1C. After such charge/discharge cycles, the capacity retention rate after 100 th cycle was calculated to evaluate the normal temperature cycle performance.
The calculation formula of the capacity retention rate after 100 cycles at 25 ℃ is as follows:
capacity retention (%) at 100 th cycle (100 th cycle discharge capacity/1 st cycle discharge capacity) × 100%
(3) Method for testing capacity retention rate, capacity recovery rate and thickness expansion rate after 30 days of storage at 60 ℃: charging the formed battery to 4.4V (LiNi) at normal temperature by using a 1C constant current and constant voltage0.5Co0.2Mn0.3O2Artificial graphite) with cutoff current of 0.02C, discharging with 1C constant current to 3.0V, measuring initial discharge capacity of the battery, charging with 1C constant current and constant voltage to 4.4V, with cutoff current of 0.01C, measuring initial thickness of the battery, storing the battery at 60 deg.C for 30 days, measuring thickness of the battery, discharging with 1C constant current to 3.0V, measuring holding capacity of the battery, and discharging with 1C constant current and constant voltageThe recovery capacity was measured by charging to 3.0V, stopping the battery at 0.02C, and then discharging to 3.0V with a constant current of 1C. The calculation formulas of the capacity retention rate, the capacity recovery rate and the thickness expansion are as follows:
battery capacity retention (%) retention capacity/initial capacity × 100%
Battery capacity recovery (%) -recovery capacity/initial capacity X100%
Battery thickness swelling ratio (%) (thickness after 30 days-initial thickness)/initial thickness × 100%
TABLE 1
The test results of experimental examples 1 to 9 and comparative examples 1 to 8 are shown in tables 2 and 3 below.
TABLE 2
TABLE 3
According to the results in tables 2 and 3, it can be seen that the addition of the additive for non-aqueous lithium ion battery electrolyte can make the capacity retention rate at 60 ℃ of the lithium ion battery at high temperature of 74% or more, even 80% or more, the capacity recovery rate at 79% or more, the thickness expansion rate at 36.3% or less, the retention rate at 100 times of normal temperature cycles at 83% or more, and the retention rate at 200 times of high temperature cycles at 70% or more. The comparative example, in which such an additive was not added, resulted in a significant decrease in high-temperature capacity retention rate, capacity recovery rate, and cycle performance, and a significant increase in thick expansion rate.
The applicant states that the present invention is described by the above examples for the lithium ion battery nonaqueous electrolytic solution and the lithium ion battery of the present invention, but the present invention is not limited to the above examples, that is, the present invention is not meant to be implemented by relying on the above examples. It should be understood by those skilled in the art that any modification of the present invention, equivalent substitutions of the raw materials of the product of the present invention, addition of auxiliary components, selection of specific modes, etc., are within the scope and disclosure of the present invention.
Claims (10)
1. The non-aqueous electrolyte of the lithium ion battery is characterized by comprising a methyl bis-sulfonyl diamino methane bis-lithium additive shown in a structural formula I:
2. the nonaqueous electrolyte solution for lithium ion batteries according to claim 1, wherein the mass percentage of the methyldisulfonyldiaminomethanedilithium additive is 0.1 to 5% based on 100% of the total mass of the nonaqueous electrolyte solution for lithium ion batteries.
3. The nonaqueous electrolyte solution for a lithium ion battery according to claim 1 or 2, wherein a solvent in the nonaqueous electrolyte solution is selected from any one or a combination of at least two of ethylene carbonate, propylene carbonate, butylene carbonate, dimethyl carbonate, diethyl carbonate, ethyl methyl carbonate, and propyl methyl carbonate.
4. The lithium-ion battery nonaqueous electrolyte solution of any one of claims 1 to 3, wherein the lithium-ion battery nonaqueous electrolyte solution further comprises other additives besides a methyldisulfonyldiaminomethanedilithium additive;
preferably, the other additive is at least one of unsaturated cyclic carbonate ester compounds or sultone compounds;
preferably, the unsaturated cyclic carbonate compound comprises at least one of vinylene carbonate and ethylene carbonate;
preferably, the sultone compound comprises at least one of 1, 3-propane sultone or 1, 4-butane sultone.
5. The nonaqueous electrolyte solution for lithium ion batteries according to any one of claims 1 to 4, wherein the unsaturated cyclic carbonate compound is contained in an amount of 0.1 to 5% by mass based on 100% by mass of the total mass of the nonaqueous electrolyte solution for lithium ion batteries;
preferably, the content of the sultone compounds in percentage by mass is 0.1-5% based on 100% of the total mass of the lithium ion battery nonaqueous electrolyte.
6. The nonaqueous electrolyte solution for lithium-ion batteries according to any one of claims 1 to 5, further comprising a lithium salt additive selected from the group consisting of LiBOB, LiFSI, LiODFB and LiBF4、LiPO2F2Or a combination of any one or at least two of the foregoing;
preferably, the lithium salt additive accounts for 0.1-5% of the total mass of the lithium ion battery nonaqueous electrolyte solution as 100%.
7. The nonaqueous electrolyte for lithium-ion batteries according to any one of claims 1 to 6, wherein the nonaqueous electrolyte for lithium-ion batteries comprises a lithium salt electrolyte, preferably LiPF6。
8. The nonaqueous electrolyte solution for lithium ion batteries according to any one of claims 1 to 7, wherein the content of the lithium salt electrolyte in the nonaqueous electrolyte solution for lithium ion batteries is 0.1 to 20% by mass.
9. The lithium ion battery is characterized by comprising a positive electrode, a negative electrode, a diaphragm arranged between the positive electrode and the negative electrode and an electrolyte, wherein the electrolyte is the lithium ion battery non-aqueous electrolyte.
10. The lithium ion battery of claim 9, wherein the positive electrode comprises an active material that is LiNixCoyMnzL(1-x-y-z)O2、LiCoxL(1-x')O2、LiNix”Ly'Mn(2-x”-y')O4、Liz'MPO4At least one of; wherein L is at least one of Co, Al, Sr, Mg, Ti, Ca, Zr, Zn, Si and Fe; x is more than or equal to 0 and less than or equal to 1, y is more than or equal to 0 and less than or equal to 1, z is more than 0 and less than or equal to 1, x + y + z is more than 0 and less than or equal to 1, x 'is more than 0.3 and less than or equal to 0.6, and y' is more than 0.01 and less than or equal to 0.; l' is at least one of Co, Al, Sr, Mg, Ti, Ca, Zr, Zn, Si and Fe; z' is more than or equal to 0.5 and less than or equal to 1, and M is at least one of Fe, Mn and Co.
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