Anode active material for lithium secondary battery, method for preparing same, and lithium secondary battery comprising same
An embodiment of the present invention provides an anode active material for a lithium secondary battery, which is a porous silicon-carbon composite including a plurality of nano-silicon particles embedded in a carbon-based material and having a plurality of pores, wherein the carbon-based material includes graphite particles, soft carbon, hard carbon, or a combination thereof, and based on 100 wt % of the porous silicon-carbon composite, a weight ratio of the graphite particles to the soft carbon, the hard carbon, or a combination thereof is 1:5 to 5:1.
1. A method of preparing an anode active material for a lithium secondary battery, comprising:
preparing a porous silicon-carbon mixed powder by mixing nano-silicon particles, graphite particles, and pitch particles by dry milling;
adding the porous silicon-carbon mixed powder and a binder to distilled water to prepare a mixed solution;
spray-drying the mixed solution to prepare primary particles;
inserting the primary particles into a mold and press-molding to produce secondary particles;
heat-treating the secondary particles to produce heat-treated secondary particles; and
pulverizing and sieving the heat-treated secondary particles,
wherein, in the preparing of the porous silicon-carbon mixed powder, the pitch particles are included in an amount of greater than or equal to 30 wt % based on 100 wt % of the porous silicon-carbon mixed powder.
2. The method of claim 1 , wherein
in the preparing of the porous silicon-carbon mixed powder by mixing the nano-silicon particles, graphite particles, and pitch particles by dry milling,
a weight of the pitch particles is greater than or equal to a weight of the graphite particles.
3. The method of claim 2 , wherein
in the preparing of the porous silicon-carbon mixed powder by mixing the nano-silicon particles, graphite particles, and pitch particles by dry milling,
a weight ratio of the pitch particles and the graphite particles is 1:1 to 5:1.
4. The method of claim 1 , wherein
the pitch particles include a combination of coal-based pitch and petroleum-based pitch, and
a weight of the coal-based pitch is greater than or equal to a weight of the petroleum- based pitch.
5. The method of claim 4 , wherein a weight ratio of the coal-based pitch: the petroleum-based pitch is in a range of 5:5 to 9:1 based on 100 wt % of the pitch particles.
6. The method of claim 1 , wherein a softening point of the pitch particles is greater than or equal to 250° C.
7. The method of claim 6 , wherein
the heat-treating of the secondary particles comprises:
a first isothermal process in which the secondary particles are heated up to a temperature of 50° C. to 350° C. higher than the softening point of the pitch particles and maintained at a rate of less than or equal to 7° C./min; and
a second isothermal process in which after the first isothermal process, the secondary particles are heated up to a temperature range of 700° C. to 1000° C. at a rate of less than or equal to 7° C./min and then maintained.
8. The method of claim 7 , wherein the first isothermal process and the second isothermal process are maintained for 1 hour to 4 hours.
9. The method of claim 1 , wherein
after the pulverizing and sieving of the heat-treated secondary particles,
forming a carbon coating layer on a surface of the secondary particles is further included, and
the forming of the carbon coating layer is performed at 750° C. to 1,000° C.
10. The method of claim 1 , wherein
after the heat-treating of the secondary particles,
a carbonization yield of the secondary particles is 60% to 95%.
11. The method of claim 1 , wherein
by the heat-treating of the secondary particles,
the pitch particles are carbonized into soft carbon, and
the binder is carbonized into hard carbon.