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Layered oxide material, preparation method, pole piece, secondary cell and application

A secondary battery and oxide technology, applied in the field of materials, can solve the problems of low electronic conductivity, difficult application, and low capacity, and achieve excellent cycle performance, low manufacturing cost, and good safety performance

Active Publication Date: 2015-07-22
LIYANG HINA BATTERY TECH CO LTD
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

At present, there have been a large number of literature reports as electrode materials for sodium-ion batteries; the positive electrode materials mainly include NaSCION-structured Na 3 V 2 (PO 4 ) 3 [Electrochem.Commun., 2012, 14, 86-89, Adv. Energy Mater., 2013, 3, 156-160], NaVPO 4 , Na 3 V 2 (PO 4 ) 3 f 3 【J. Mater. Chem., 2012, 22, 20535-20541】, Na 3 V 2 O(PO 4 ) 3 F, NaTi 2 (PO 4 ) 3 etc., but due to the low electronic conductivity and poor kinetic performance of this type of material, it is often necessary to obtain a relatively stable cycle through nanonization and carbon coating, and the vanadium element contained in it is also a toxic element, so it is relatively difficult to apply Disaster
Na 4 mn 9 o 18 [Adv.Mater., 2011, 23, 3155-3160] structure, in which the movable sodium ion is in the S-type large channel, this structure is very stable throughout the cycle, and can achieve 2000 long cycles , but because this structure mainly depends on the change from manganese trivalent to manganese tetravalent, and the original sodium content is relatively low, the average voltage of the entire positive electrode material is low, and the capacity is relatively low
[0004] Layered cathode materials are also a hot topic of research in recent years. Na in the P2 phase x TMO 2 NaTMO with O3 phase 2 It is currently the most researched material [Physical B&C, 1980, 99, 81-85]. The O3 phase has a high sodium content and a high charge capacity in the first week, but its electrochemical cycle performance is poor, and it is sensitive to air and water, so it is difficult to apply. A certain degree of difficulty; P2 phase has good stability in the electrochemical cycle process due to the large space where the sodium ions are located, and the deintercalation of sodium ions is relatively fast, but most P2 phase materials are unstable in the air and due to the relatively low sodium content Its first week charging capacity is generally low
In 2001, Lu et al prepared the P2 phase Na 2 / 3 Ni 1 / 3 mn 2 / 3 o 2 material, and its electrochemical performance was characterized, it has a capacity of 160mAh / g between 2.0-4.5V [Z.H.Lu and J.R.Dahn, J.Electrochem.Soc., 2001, 148, A1225-A1229], but Its electrochemical curve shows multiple platforms, and the cycle stability is extremely poor
The compounds of these two elements are costly, toxic and not environmentally friendly.

Method used

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  • Layered oxide material, preparation method, pole piece, secondary cell and application
  • Layered oxide material, preparation method, pole piece, secondary cell and application
  • Layered oxide material, preparation method, pole piece, secondary cell and application

Examples

Experimental program
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Embodiment 1

[0075] Embodiment 1 of the present invention provides a layered oxide material whose general chemical formula is: Na x Cu i Fe j mn k m y o 2+β ;

[0076] Among them, M is an element for doping and replacing the transition metal site, specifically Li + , Ni 2+ ,Mg 2+ ,Mn 2+ ,Zn 2+ ,Co 2+ , Ca 2+ , Ba 2+ ,Sr 2+ ,Mn 3+ ,Al 3+ ,B 3+ ,Cr 3+ ,Co 3+ ,V 3+ ,Zr 4+ , Ti 4+ ,Sn 4+ ,V 4+ ,Mo 4+ ,Mo 5+ , Ru 4+ , Nb 5+ ,Si 4+ ,Sb 5+ ,Nb 5+ ,Mo 6+ , Te 6+ one or more of

[0077] Said x, y, i, j, k, and β are respectively the molar percentages of corresponding elements; wherein the relationship between x, y, i, j, k, and β satisfies y+i+j+k=1, And x+my+2i+3j+4k=2(2+β); where 0.8≤x≤1; 0<i≤0.3; 0<j≤0.5; 0<k≤0.5; -0.02≤β≤0.02; m is the valence state of said M;

[0078] The space group of the layered oxide material is

[0079] exist figure 1 The X-ray diffraction (X-ray diffraction, XRD) collection of a plurality of layered oxide materials of different elem...

Embodiment 2

[0082] This embodiment provides a method for preparing a layered oxide material, specifically a solid phase method, such as figure 2 shown, including:

[0083] Step 201, mixing sodium carbonate with a required stoichiometric amount of 100wt% to 108wt% of sodium and required stoichiometric amounts of copper oxide, iron oxide, manganese oxide and M oxide in proportion to form a precursor;

[0084] Specifically, the M is specifically Li + , Ni 2+ ,Mg 2+ ,Mn 2+ ,Zn 2+ ,Co 2+ , Ca 2+ , Ba 2+ ,Sr 2+ ,Mn 3+ ,Al 3+ ,B 3+ ,Cr 3+ ,Co 3+ ,V 3+ ,Zr 4+ , Ti 4+ ,Sn 4+ ,V 4+ ,Mo 4+ ,Mo 5+ , Ru 4+ , Nb 5+ , Si 4+ ,Sb 5+ ,Nb 5+ ,Mo 6+ , Te 6+ one or more of.

[0085] Step 202, using a ball milling method to uniformly mix the precursor to obtain a precursor powder;

[0086] Step 203, placing the precursor powder in a muffle furnace, and heat-treating it in an air atmosphere at 700° C. to 1000° C. for 2 to 24 hours;

[0087] Step 204, grinding the heat-treated prec...

Embodiment 3

[0090] This embodiment provides a preparation method of a layered oxide material, specifically a spray drying method, such as image 3 shown, including:

[0091] Step 301, weighing and mixing sodium carbonate, copper oxide, iron oxide, manganese oxide and M oxide in proportion to the required sodium stoichiometric ratio of 100wt% to 108wt% to form a precursor; or using stoichiometric ratio of sodium nitrate, Copper nitrate, iron nitrate, manganese acetate and M nitrate as precursors;

[0092] Specifically, the M can be Li + , Ni 2+ ,Mg 2+ ,Mn 2+ ,Zn 2+ ,Co 2+ , Ca 2+ , Ba 2+ ,Sr 2+ ,Mn 3+ ,Al 3+ ,B 3+ ,Cr 3+ ,Co 3+ ,V 3+ ,Zr 4+ , Ti 4+ ,Sn 4+ ,V 4+ ,Mo 4+ ,Mo 5+ , Ru 4+ , Nb 5+ , Si 4+ ,Sb 5+ ,Nb 5+ ,Mo 6+ , Te 6+ one or more of.

[0093] Step 302, adding ethanol or water to the precursor and stirring evenly to form a slurry;

[0094] Step 303, spray-drying the slurry to obtain a precursor powder;

[0095] Step 304, placing the precursor powder i...

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Abstract

The invention discloses a layered oxide material, a preparation method, a pole piece, a secondary cell and an application. The material is represented as a general formula of Na<x>CuFe<j>Mn<k>M<y>O<2+beta>. M is an element for replacing a transition metal position through doping; the x, y, i, j, k, beta are mol percentages of corresponding elements; x, y, i, j, k, beta satisfy relationships of y+i+j+k=1 and x+my+2i+3j+4k=2(2+beta), wherein x is less than or equal to 0.8, and is more than or equal to 1, i is more than 0 and is less than or equal to 0.3, j is more than 0 and is less than or equal to 0.5, k is more than 0 and is less than or equal to 0.5, and beta is more than or equal to -0.02 and is less than or equal to 0.02; m is the valance of M; and the space group of the layered oxide material is R3m.

Description

technical field [0001] The invention relates to the field of material technology, in particular to a layered oxide material, a preparation method, a pole piece, a secondary battery and its application. Background technique [0002] With the reduction of non-renewable energy such as oil and coal and the aggravation of environmental pollution, the development of clean energy has become a global issue. The key to solving this problem is to develop wind energy, solar energy and the corresponding energy storage batteries. Existing electrochemical energy storage devices mainly include lead-acid batteries, zinc-nickel batteries, hydrogen-nickel batteries, flow batteries and lithium-ion batteries. Among them, most lithium-ion secondary batteries use lithium ion intercalation compounds as positive and negative electrode materials, and dry organic solvents as electrolytes; lithium ions can reversibly intercalate back and forth between the positive and negative active materials withou...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M4/485H01M4/505H01M4/525H01M4/62H01M4/131H01M10/054
CPCH01M4/131H01M4/366H01M4/485H01M4/505H01M4/525H01M4/62H01M10/054C01G49/0072C01G53/50C01P2002/76C01P2004/62C01P2002/72C01P2004/03C01P2004/61Y02E60/10H01M2220/10C01P2002/70C01P2006/40H01M2004/028
Inventor 胡勇胜穆林沁陈立泉
Owner LIYANG HINA BATTERY TECH CO LTD
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