Selenium-mesoporous carrier compound, as well as preparation method and application thereof

A composite and mesoporous technology, applied in the field of electrochemical power supply, can solve the problems of easy shedding, complex preparation method, unstable reaction and so on

Active Publication Date: 2013-06-26
INST OF CHEM CHINESE ACAD OF SCI
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  • Abstract
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  • Claims
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Problems solved by technology

Not long ago, Amine et al. (J.Am.Chem.Soc.2012, 134, 4505-4508) made a pioneering work on lithium-selenium batteries and explored the reaction mechanism of selenium, but due to its Using carbon nanotubes as the conductive substrate, the prepared selenium-carbon mixture is used as the positive electrode. Selenium exists in the form of blocks, and the substrate has a weak limiting effect on selenium. Therefore, the electrochemical activity of selenium cannot be effectively exerted, and the reaction is unstable. The cycle capacity of lithium-selenium battery is low, the discharge capacity decays quickly, and the battery life is limited
Patent CN101794877A discloses a copper fluoride-selenium nanocomposite negative electrode material for lithium ion batteries and its preparation method, in which copper fluoride and elemental selenium are formed into a nanocomposite material by laser sputtering, and the nanocomposite material is used to As the negative electrode material of lithium-ion thin film battery, however, the preparation method here is complicated, only suitable for special purpose but not suitable for large-scale application, and the battery capacity of the battery obtained in this way is on the low side, only 310mA h / g
Patent CN102623678A discloses a preparation method of Li-Se batteries and lithium battery electrode materials, which discloses the use of thermal evaporation to grow selenium microspheres on substrates and grow selenium nanowires or selenium nanowires on substrates loaded with gold catalysts Nanobelts are used as lithium battery materials, but because the noble metal gold needs to be used in this invention, and the selenium vapor reacts in a fluid atmosphere, it will cause a great waste of selenium. In addition, selenium is deposited on the surface of the substrate, and the effect is unstable. It is easy to fall off, and the most important thing is that in this invention, the discharge voltage of selenium as a positive electrode material is too low (about 0.25V), and for lithium battery electrode materials, the voltage platform is below 1V and can only be used as a negative electrode material

Method used

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  • Selenium-mesoporous carrier compound, as well as preparation method and application thereof
  • Selenium-mesoporous carrier compound, as well as preparation method and application thereof
  • Selenium-mesoporous carrier compound, as well as preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0040] (1) Preparation of Se-Mesoporous Carrier Complex

[0041] The mesoporous carrier used in the experiment is mesoporous carbon (purchased from Nanjing Xianfeng Nano Material Technology Co., Ltd.), with a specific surface area of ​​612.3m 2 g -1 , the pore volume is 0.697cm 3 g -1 , the average pore size is 4.3nm, and the mass fraction of selenium in the prepared selenium-mesoporous carbon composite is 50%.

[0042] The preparation method of selenium-mesoporous carbon composite is as follows:

[0043] (1) Weigh selenium and mesoporous carbon according to the mass ratio of 1:1 and mix them evenly;

[0044] (2) The mixture of selenium and mesoporous carbon was heated at 5°C min in a constant volume reactor filled with argon. -1 The heating rate is heated to 260 ° C and maintained for 12 hours, so that selenium is fully dispersed in the mesoporous carbon;

[0045] (3) Stop heating and return to room temperature to obtain a selenium-mesoporous carbon composite.

[0046]...

Embodiment 2

[0056] Other conditions are the same as in Example 1, except that the binder used in step (2) is not sodium alginate (with water as solvent), but polyvinylidene fluoride (PVDF) (with N-methyl pyrrolidone (NMP) as solvent). The assembled lithium-selenium battery uses a charge-discharge instrument to perform a constant-current charge-discharge test on the above-mentioned lithium-selenium battery. The test voltage range is 1.0-3.0V, and the test temperature is 25°C. The battery capacity and charge and discharge current are calculated based on the mass of elemental selenium. Figure 5 It is the lithium-selenium battery described in this example in the carbonate electrolyte 0.1C (equivalent to 68mA g -1 ) charge-discharge curve at the rate. The first cycle discharge capacity of the lithium-selenium battery in the above voltage range is 932mA h g -1 , the first cycle charging capacity is 578mA h g -1 , the discharge capacity remains at 550mA h g after 50 cycles from the second c...

Embodiment 3

[0058] (1) Preparation of mesoporous carbon supports

[0059] The mesoporous carrier used in the experiment is mesoporous carbon with a specific surface area of ​​1789 m 2 g -1 , the pore volume is 2.37cm 3 g -1 , the average pore size is 3.8nm.

[0060] The preparation method of mesoporous carbon is as follows:

[0061] Dissolve 1.25g of sucrose in 5mL of aqueous solution containing 0.14g of concentrated sulfuric acid, then add 1.0g of nanoporous silica-based molecular sieve (purchased from Shanghai Carbon Union Environmental Protection Technology Co., Ltd.), ultrasonically disperse for 1h, then heat to 100°C and maintain Heating for 12h, then heating to 160°C and maintaining heating for 12h. Then add 0.8g sucrose, 0.09g concentrated sulfuric acid and 5mL water, repeat heating to 100°C and maintain heating for 12h, then heat to 160°C and maintain heating for 12h. The product was heated at 10°C for min under an argon atmosphere -1 The heating rate was heated to 900 ° C ...

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Abstract

The invention discloses a lithium-selenium battery and a preparation method of the lithium-selenium battery. The lithium-selenium battery comprises a metal lithium cathode, a selenium-mesoporous carrier compound anode and an organic electrolyte, wherein the selenium-mesoporous carrier compound anode is formed by mixing selenium with a mesoporous carrier in a certain proportion and then heating a mixture; the selenium is uniformly dispersed in a mesoporous channel of the mesoporous carrier in an annular selenium molecular form and / or an amorphous chain selenium molecular form; and the mesoporous carrier comprises a carbon mesoporous carrier, a non-carbon mesoporous carrier and compositions thereof. The lithium-selenium battery provided by the invention has the advantages of small size, high capacity, long service life, high efficiency, simplicity in reaction platform and the like, and is a novel secondary energy storage battery with high volume energy density. The preparation method of the main component namely the selenium-mesoporous carrier compound anode of the battery is simple. Raw materials are easily available. The lithium-selenium battery is suitable for large-scale production and high in practicability.

Description

technical field [0001] The invention belongs to the field of electrochemical power sources, and specifically relates to a selenium-mesoporous carrier composite, a preparation method thereof, a selenium-mesoporous carrier composite positive electrode material and a preparation method thereof, a method for preparing a positive electrode containing the composite, and using the positive electrode The new lithium-selenium battery and its application in high volume energy density energy storage devices. Background technique [0002] Lithium-selenium battery refers to a type of metal lithium secondary battery that uses elemental selenium or selenium-containing compounds as the positive electrode and metallic lithium as the negative electrode, and realizes the mutual conversion between chemical energy and electrical energy through the chemical reaction between selenium and lithium. Elemental selenium, because of its two-electron reaction mechanism and high density in the electrochem...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M4/38H01M4/62H01M4/134H01M4/1395H01M10/052
CPCY02E60/10
Inventor 郭玉国杨春鹏殷雅侠万立骏
Owner INST OF CHEM CHINESE ACAD OF SCI
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