Figure 1 shows the TGA trace for a particulate material according to the invention,
comprising a high level of surface silicon and a low level of bulk coarse silicon.
Figure 2 shows the TGA trace for a particulate material comprising a low level of surface
5 silicon and a high level of bulk coarse silicon.
Figure 3 shows the instantaneous flow functions of samples from Example 2.
Figure 4 shows the instantaneous flow functions of samples from Example 3.
DETAILED DESCRIPTION OF THE INVENTION
The process of the first aspect of the invention comprises the steps of:
10 (a) providing a plurality of porous particles comprising micropores and
meso pores
15
(b)
wherein the micropores and mesopores have a total pore volume as
measured by nitrogen gas adsorption of 0.4 to 2.0 cm3/g, and
wherein the porous particles have a D1 particle diameter of at least
0.5 1-Jm, and a Dso particle diameter in the range from 1 to 20 1-1m;
contacting the porous particles with a precursor of an electroactive
material at a temperature effective to cause deposition of a plurality of
electroactive material domains in the pores of the porous particles.
The porous particles function as a framework for the electroactive material, which is
20 typically deposited in the form of a plurality of electroactive material domains. The term
"electroactive material domain" refers to a body of electroactive material, e.g. elemental
silicon, having maximum dimensions that are determined by the dimensions of the
micropores and/or mesopores of the porous particles in which they are located. The
electroactive domains may therefore be described as nanoscale electroactive domains,
25 wherein the term "nanoscale" is understood to refer generally to dimensions less than
100 nm. Although, due to the dimensions of micropores and mesopores, the
electroactive material domains typically have maximum dimensions in any direction of
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less than 50 nm, and usually significantly less than 50 nm. A domain may for example
take the form of a regular or irregular particle or a bounded layer or region of coating.
The process of the present invention is characterized by the use of a porous particle
starting material having a 01 particle diameter of at least 0.5 1-1m in combination with a
5 carefully controlled pore volume and pore size distribution. Taken together, these
factors ensure that composite particles are obtained having a high content of "surface
silicon" as compared to the use of starting materials in which particle fines are present
in the porous particle starting material. Preferably, the 01 particle diameter of the porous
particles is at least 0.8 1-Jm, or at least 1.0 1-Jm, or at least 1.2 1-Jm, or at least 1.4 1-Jm, or
1 o at least 1.5 1-Jm, or at least 1.6 1-Jm, or at least 1.8 1-Jm, or at least 2.0 1-Jm, or at least 2.2
1-Jm, or at least 2.4 1-Jm, or at least 2.5 1-Jm, or at least 2.6 1-Jm, or at least 2.8 1-Jm, or at
least 3.0 1-Jm.
In general, the porous particles have a Oso particle diameter in the range from 1 to
20 1-Jm. Preferably, the Oso particle diameter of the porous particles is at least 1.5 1-Jm,
15 or at least 2 1-Jm, or at least 2.5 1-Jm, or at least 3 1-Jm. Preferably, the Oso particle
diameter of the porous particles is no more than 18 1-Jm, or no more than 15 1-Jm, or no
more than 12 1-Jm, or no more than 10 1-Jm, or no more than 8 1-Jm. For example, the Oso
particle diameter of the porous particles may be in the range from 1.5 to 18 1-Jm, or in
the range from 1.5 to 15 1-Jm, or in the range from 2 to 12 1-Jm, or in the range from 2 to
20 10 1-Jm, or in the range from 2.5 to 8 1-Jm, or in the range from 3 to 8 1-Jm.
The Ogo particle diameter of the porous particles is preferably no more than 30 1-Jm, or
no more than 25 1-Jm, or no more than 20 1-Jm, or no more than 18 1-Jm, or no more than
15 1-Jm, or no more than 13 1-Jm, or no more than 12 1-Jm.
Preferably, the 01 particle diameter is in the range from 0.8 to 5.0 1-1m and the Ogo particle
25 diameter is in the range from 6 to 15 1-Jm, preferably the 01 particle diameter is in the
range from 1.0 to 5.0 1-1m and the Ogo particle diameter is in the range from 7.5 to 15
1-Jm, preferably the 01 particle diameter is in the range from 1.5. to 4.5 1-1m and the Ogo
particle diameter is in the range from 9 to 15 1-Jm, preferably wherein the 01 particle
diameter is in the range from 2 to 4 1-1m and the Ogo particle diameter is in the range
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from 10 to 14 1-Jm, preferably wherein the D1 particle diameter is in the range from 2.5
to 3.5 1-1m and the Ogo particle diameter is in the range from 11 to 13 1-Jm.
The Oga particle diameter of the porous particles is preferably no more than 35 1-Jm, or
no more than 30 1-Jm, or no more than 25 1-Jm, or no more than 20 1-Jm, or no more than
5 18 1-Jm, or no more than 16 1-Jm, or no more than 15.5 1-Jm, or no more than 15 1-Jm, or no
more than 12 1-Jm.
The D10o particle diameter of the porous particles is preferably no more than 40 1-Jm, or
no more than 35 1-Jm, or no more than 30 1-Jm, or no more than 25 1-Jm, or no more than
20 1-Jm, or no more than 16 1-Jm.
10 The deposition of electroactive materials into porous particles that are excessively large
may be less efficient due to the longer distance that precursor molecules must diffuse
through the pore structure to reach the innermost pores. Deposition of the electroactive
material in pores nearer to the particle surface can obstruct access of the precursor
molecules to the innermost pores, resulting in particles that are underfilled and thus
15 non-homogenous deposition of the electroactive material between particles of different
sizes Also, as discussed above, outsize particles also pack less efficiently and therefore
obstruct the formation of electrode layers of homogenous structure and composition.
Preferably, the difference between the Oga particle diameter and the 01 particle diameter
of the porous particles (Oga-01) is no more than 18 1-Jm, or no more than 16 1-Jm, or no more
20 than 15 1-Jm, or no more than 14 1-Jm, or no more than 13 1-Jm, or no more than 12 1-Jm. As
set out above, controlling both the D1 particle diameter and the Oga particle diameter
provides a solution to the problems associated with both fine particles and outsize
particles. In particular, by maintaining a small particle size distribution between the D1
and Oga particle sizes, the present invention provides a population of composite particles
25 which is able to pack efficiently in electrode layers and which also provides for efficient
and homogenous thermal infiltration and deposition behaviour during manufacture of
the composite particles.
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Preferably, the ratio of the Oga particle diameter to the 01 particle diameter of the porous
particles (Oga/01) is no more than 12, or no more than 10, or no more than 8, or no more
than 6, or no more than 5.
Preferably, (Oga-01)/0so is no more than 2.2, or no more than 2, or no more than 1.9, or
5 no more than 1.8, or no more than 1.7, or no more than 1.6.
Preferably, the difference between the Ogo particle diameter and the 01 particle diameter
of the porous particles (Ogo-01) is no more than 12.0 1-Jm, or no more than 10.0 1-Jm, or no
more than 9.0 1-Jm, or no more than 8.0 1-Jm.
Preferably, the ratio of the Ogo particle diameter to the 01 particle diameter of the porous
10 particles (Ogo/01) is no more than 12.0, or no more than 10.0, or no more than 9.0, or no
more than 8.0, or no more than 7.0, or no more than 6.0, or no more than 5.0.
Preferably, (Ogo-01)/0so is no more than 2.2, or no more than 2, or no more than 1.9, or
no more than 1.8, or no more than 1.7, or no more than 1.6.
The porous particles preferably have a narrow particle size distribution span. For
15 instance, the particle size distribution span (defined as (Ogo-010)/0so) is preferably 3 or
less, more preferably 2 or less, more preferably 1.5 or less and most preferably 1.2 or
less. By maintaining a narrow particle size distribution span, efficient packing of the
particles into dense powder beds is more readily achievable.
The ratio of the Oso particle diameter to the 01 particle diameter of the porous particles
20 (Oso/01) is preferably no more than no more than 1 0.0, or no more than 8.0, or no more
than 7.0, or no more than 6.0, or no more than 5.0, or no more than 4.0, or no more
than 3.0, or no more than 2.5. For example, the ratio of the Oso particle diameter to the
01 particle diameter of the porous particles in the range from 2.0 to 1 0.0, or from 2.0 to
8.0, or from 2.0 to 5.0, or from 2.0 to 4.0.
25 The ratio of the 010o particle diameter to the Oso particle diameter of the porous particles
is preferably no more than 3, or no more than 2.5 or no more than 2.
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Preferred porous particles include those in which the 01 particle diameter is at least
1.0 1-1m and the ratio of the Oso particle diameter to the 01 particle diameter is no more
than 5.0, or no more than 4.0, or no more than 3.0.
Preferred porous particles also include those in which the 01 particle diameter is at least
5 1.0 1-1m and the ratio of the Ogo particle diameter to the 01 particle diameter of the porous
particles (Ogo/01) is no more than 9.0, or no more than 8.0, or no more than 7.0, or no more
than 6.0, or no more than 5.0.
Preferred porous particles also include those in which the 01 particle diameter is at least
1.0 1-1m and the difference between the Ogo particle diameter and the 01 particle diameter
10 of the porous particles (Ogo-01) is no more than 10.0 1-Jm, or no more than 9.0 1-Jm, or no
more than 8.0 1-Jm.
Preferred porous particles also include those in which the 01 particle diameter is at least
1.0 1-1m and the ratio of the Oga particle diameter to the 01 particle diameter of the porous
particles (Oga/01) is no more than 10, or no more than 8.
15 Preferred porous particles also include those in which the 01 particle diameter is at least
1.0 1-1m and the difference between the Oga particle diameter and the 01 particle diameter
of the porous particles (Oga-01) is no more than 15 1-Jm, or no more than 14 1-Jm, or no more
than 13 1-Jm, or no more than 12 1-Jm.
Preferred porous particles also include those in which the 01 particle diameter is at least
20 1.0 1-1m and (Oga-01)/0so is no more than 2, or no more than 1.9, or no more than 1.8, or
no more than 1.7, or no more than 1.6.
Preferred porous particles include those in which the 01 particle diameter is at least
1.5 1-1m and the ratio of the Oso particle diameter to the 01 particle diameter is no more
than 6.0, or no more than 5.0, or no more than 4.0, or no more than 3.0.
25 Preferred porous particles also include those in which the 01 particle diameter is at least
1.5 1-1m and the ratio of the Ogo particle diameter to the 01 particle diameter of the porous
particles (Ogo/01) is no more than 10.0, or no more than 9.0, or no more than 8.0, or no
more than 7.0, or no more than 6.0, or no more than 5.
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Preferred porous particles also include those in which the 01 particle diameter is at least
1.5 1-1m and the difference between the Ogo particle diameter and the 01 particle diameter
of the porous particles (Ogo-01) is no more than 10.0 1-Jm, or no more than 9 1-Jm, or no
more than 8.0 1-Jm.
5 Preferred porous particles also include those in which the 01 particle diameter is at least
1.5 1-1m and the ratio of the Oga particle diameter to the 01 particle diameter of the porous
particles (Oga/01) is no more than 12, or no more than 10, or no more than 8.
Preferred porous particles also include those in which the 01 particle diameter is at least
1.5 1-1m and the difference between the Oga particle diameter and the 01 particle diameter
10 of the porous particles (Oga-01) is no more than 18 1-Jm, or no more than 16 1-Jm, or no more
than 15 1-Jm, or no more than 14 1-Jm, or no more than 13 1-Jm, or no more than 12 1-Jm.
Preferred porous particles also include those in which the 01 particle diameter is at least
1.5 1-1m and (Oga-01)/0so is no more than 2, or no more than 1.9, or no more than 1.8, or
no more than 1.7, or no more than 1.6.
15 The porous particles preferably have a positive skew in the volume-based distribution,
for example, such that the volume based distribution is asymmetric with a longer tail on
the right hand side. A positive skew in the volume-based particle diameter distribution
is advantageous since the natural packing factor will be higher than if all particles are
the same size, thereby reducing the need for calendering or other physical densification
20 processes when the composite particle product is formed into an electrode layer.
Preferably, the Oso particle diameter is less than the volume-based mean of the particle
diameter distribution (0[4.3]). Preferably, the skew of the particle diameter distribution
(as measured by a Malvern Mastersizer™ 3000 analyzer) is no more than 5, or no more
than 3, preferably no more than 2. Preferably, the skew is at least 0.2, or at least 0.3,
25 or at least 0.4.
The particle diameter distribution of the porous particles may be monomodal, bimodal
or multimodal. Preferably the particle diameter distribution is monomodal.
The porous particles may have an average sphericity (as defined herein) of more than
0.5. Preferably they have an average sphericity of at least 0.55, or at least 0.6, or at
A process for preparing composite particles, the process comprising the steps
of:
(a)
(b)
providing a plurality of porous particles comprising micropores and
meso pores
wherein the micropores and mesopores have a total pore volume as
measured by nitrogen gas adsorption of 0.4 to 2.0 cm3/g, and
wherein the porous particles have a 01 particle diameter of at least
0.5 1-Jm, and a Oso particle diameter in the range from 1 to 20 1-1m;
contacting the porous particles with a precursor of an electroactive
material at a temperature effective to cause deposition of a plurality of
electroactive material domains in the pores of the porous particles.
2. A process according to claim 1, wherein the 01 particle diameter of the porous
particles is at least 0.8 1-Jm, or at least 1.0 1-Jm, or at least 1.2 1-Jm, or at least 1.4 1-Jm, or
15 at least 1.5 1-Jm, or at least 1.6 1-Jm, or at least 1.8 1-Jm, or at least 2.0 1-Jm, or at least 2.2
1-Jm, or at least 2.4 1-Jm, or at least 2.5 1-Jm, or at least 2.6 1-Jm, or at least 2.8 1-Jm, or at
least 3.0 1-Jm.
3. A process according to claim 1 or claim 2, wherein the Oso particle diameter of
the porous particles is in the range from 1.5 to 18 1-Jm, or in the range from 1.5 to 15 1-Jm,
20 or in the range from 2 to 12 1-Jm, or in the range from 2 to 10 1-Jm, or in the range from
2.5 to 8 1-Jm, or in the range from 3 to 8 1-Jm.
4. A process according to any preceding claim, wherein the Ogo particle diameter
of the porous particles is no more than 25 1-Jm, or no more than 20 1-Jm, or no more than
18 1-Jm, or no more than 15 1-Jm, or no more than 13 1-Jm, or no more than 12 1-Jm.
25 5. A process according to any preceding claim, wherein the 01 particle diameter is
in the range from 0.8 to 5.0 1-1m and the Ogo particle diameter is in the range from 6 to
15 1-Jm, preferably wherein the 01 particle diameter is in the range from 1.0 to 5.0 1-1m
and the Ogo particle diameter is in the range from 7.5 to 15 1-Jm, preferably wherein the
01 particle diameter is in the range from 1.5. to 4.5 1-1m and the Ogo particle diameter is
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in the range from 9 to 15 1-Jm, preferably wherein the 01 particle diameter is in the range
from 2 to 4 1-1m and the Ogo particle diameter is in the range from 10 to 14 1-Jm, preferably
wherein the 01 particle diameter is in the range from 2.5 to 3.5 1-1m and the Ogo particle
diameter is in the range from 11 to 13 1-Jm.
5 6. A process according to any preceding claim, wherein the Oga particle diameter
of the porous particles is no more than 35 1-Jm, or no more than 30 1-Jm, or no more than
25 1-Jm, or no more than 20 1-Jm, or no more than 18 1-Jm, or no more than 16 1-Jm, or no
more than 15 1-Jm, or no more than 12 1-Jm.
7. A process according to any preceding claim, wherein the 010o particle diameter
10 of the porous particles is no more than 40 1-Jm, or no more than 35 1-Jm, or no more than
30 1-Jm, or no more than 25 1-Jm, or no more than 20 1-Jm, or no more than 16 1-Jm.
8. A process according to any preceding claim, wherein the difference between the
Oga particle diameter and the 01 particle diameter of the porous particles (Oga-01) is no
more than 18 1-Jm, or no more than 16 1-Jm, or no more than 15 1-Jm, or no more than 14 1-Jm,
15 or no more than 13 1-Jm, or no more than 12 1-Jm.
9. A process according to any preceding claim, wherein the ratio of the Oga particle
diameter to the 01 particle diameter of the porous particles (Oga/01) is no more than 12, or
no more than 10, or no more than 8, or no more than 6, or no more than 5.
10. A process according to any preceding claim, wherein (Oga-01)/0so is no more
20 than 2.2, or no more than 2, or no more than 1.9, or no more than 1.8, or no more than
1.7, or no more than 1.6.
11. A process according to any preceding claim, wherein the difference between the
Ogo particle diameter and the 01 particle diameter of the porous particles (Ogo-01) is no
more than 12.0 1-Jm, or no more than 10.0 1-Jm, or no more than 9.0 1-Jm, or no more than
25 8.0 1-Jm.
12. A process according to any preceding claim, wherein the ratio of the Ogo particle
diameter to the 01 particle diameter of the porous particles (Ogo/01) is no more than 12.0,
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or no more than 10.0, or no more than 9.0, or no more than 8.0, or no more than 7.0, or no
more than 6.0, or no more than 5.0.
13. A process according to any preceding claim, wherein (Ogo-D1)/Dso is no more
than 2.2, or no more than 2, or no more than 1.9, or no more than 1.8, or no more than
5 1.7, or no more than 1.6.
14. A process according to any preceding claim wherein the ratio of the Dso particle
diameter to the D1 particle diameter of the porous particles (Dso/D1) is no more than
1 0.0, or no more than 8.0, or no more than 7.0, or no more than 6.0, or no more than
5.0, or no more than 4.0, or no more than 3.0, or no more than 2.5.
10 15. A process according to any preceding claim, wherein the particle size distribution
of the porous particles has a positive skew.
16. A process according to any preceding claim, wherein the total pore volume of
micropores and mesopores in the porous particles as measured by gas adsorption is in
the range from 0.4 to 1.8 cm3/g, or from 0.4 to 1.7 cm3/g, or from 0.5 to 1.6 cm3/g, or
15 from 0.5 to 1.55 cm3/g, or from 0.6 to 1.5 cm3/g, or from 0.6 to 1.45 cm3/g, or from 0.65
to 1.4 cm3/g, or from 0.65 to 1.35 cm3/g, or from 0.7 to 1.3 cm3/g, or from 0.7 to
1.25 cm3/g, or from 0.75 to 1.2 cm3/g, or from 0.75 to 1.1 cm3/g, or from 0.8 to
1.15 cm3/g, or from 0.8 to 1.1 cm3/g.
17. A process according to any preceding claim, wherein the PDso pore diameter of
20 the porous particles is no more than 10 nm, or no more than 8 nm, or no more than
6 nm, or no more than 5 nm, or no more than 4 nm, or no more than 3 nm, or no more
than 2.5 nm, or no more than 2 nm, or no more than 1.9 nm, or no more than 1.8 nm,
or no more than 1. 7 nm, or no more than 1.6 nm.
18. A process according to any preceding claim, wherein the POgo pore diameter of
25 the porous particles is in the range from 1.5 to 20 nm, or from 2 to 20 nm, or from 3.2
to 20 nm, or from 3.5 to 15 nm, or from 3.8 to 10 nm, or from 4 to 8 nm.
19. A process according to any preceding claim, wherein the micropore volume
fraction is in the range from 0.35 to 0.98, or in the range from 0.4 to 0.95, or in the range
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from 0.4 to 0.90, or in the range from 0.4 to 0.85, or in the range from 0.45 to 0.85, or
in the range from 0.5 to 0.8, or in the range from 0.55 to 0.8, or in the range from 0.6 to
0.8, or in the range from 0.61 to 0.79.
20. A process according to any preceding claim, wherein the porous particles have
5 a BET surface area in the range from 500 m2/g to 4,000 m2/g, or from 750 m2/g to
3,500 m2/g, or from 1,000 m2/g to 3,250 m2/g, or from 1,000 m2/g to 3,000 m2/g, or from
1,000 m2/g to 2,500 m2/g, or from 1,000 m2/g to 2,000 m2/g.
21. A process according to any preceding claim, wherein step (a) comprises a step
of classifying porous particles by size to provide a plurality of porous particles having
10 the specified D1 and Dso values.
15
22. A process according to claim 21, wherein step (a) comprises:
(i) providing a precursor population of porous particles comprising micropores
and mesopores, wherein the micropores and mesopores have a total pore
volume as measured by nitrogen gas adsorption of 0.4 to 2.0 cm3/g, and
(ii) classifying the precursor population of particles to obtain the plurality of
porous particles as defined herein for use in step (a).
23. A process according to any preceding claim, wherein the porous particles are
conductive porous particles, preferably conductive porous carbon particles, more
preferably conductive porous carbon particles comprising at least 80 wt% carbon, or at
20 least 85 wt% carbon, or at least 90 wt% carbon, or at least 95 wt% carbon.
24. A process according to any preceding claim, wherein the precursor of the
electroactive material is a gaseous precursor.
25. A process according to claim 24, wherein step (b) comprises contacting the porous
particles with a gas comprising at least 30 val%, or at least 40 val%, or at least 50 val%, or
25 at least 60 val%, or at least 70 val%, or at least 80 val%, or at least 90 val%, or at least 95
val%, or at least 97 val%, or at least 99 val% of the precursor of the electroactive material
based on the total volume of the gas.
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26. A process according to any preceding claim, wherein the electroactive material
deposited in step (b) is selected from silicon, tin, germanium, aluminium and mixtures
and alloys thereof, preferably wherein the electroactive material deposited in step (b) is
silicon, preferably wherein the precursor of the electroactive material is selected from
5 silane, disilane, trisilane, tetrasilane, methylsilane, dimethylsilane and chlorosilanes.
27. A process according to any preceding claim, wherein the particles formed in step
(b) comprise at least 26 wt% of the electroactive material, or at least 28 wt% of the
electroactive material, or at least 30 wt% of the electroactive material, or at least 32 wt%
of the electroactive material, or at least 34 wt% of the electroactive material, or at least
10 36 wt% of the electroactive material, or at least 38 wt% of the electroactive material, or
at least 40 wt% of the electroactive material, or at least 42 wt% of the electroactive
material, or at least 44 wt% of the electroactive material, preferably wherein the
electroactive material is silicon.
28. A process according to claim 26 or claim 27, wherein the weight ratio of silicon
15 deposited in step (b) to the porous particles in the range from [0.50xP1 to 1.9xP1
] : 1,
or from [0.6xP1 to 1.8xP1
] : 1 or from [0. 7xP1 to 1. 7xP1
] : 1, or from [0.8xP1 to 1.6xP1
] :
1, wherein P1 is a dimensionless number having the same value as the total pore
volume of micropores and mesopores in the porous particles as measured by gas
adsorption as expressed in cm3/g.
20 29. A process according to any preceding claim, further comprising one or more of
the following steps (c) to (g):
25
30
(c) subjecting the particles from step (b) to heat treatment at a temperature
of at least 400 oc and in the presence of an inert gas;
(d)
(e)
(f)
(g)
contacting the surface of the particles from step (b) or step (c) with a
passivating agent;
depositing a lithium ion permeable material into the pores and/or onto the
outer surface of the composite particles from step (b), (c) or step (d);
subjecting the particles from step (b), (c), (d) or (e) to a deagglomeration
step to reduce the presence of agglomerated particles;
classifying the composite particles from step (b), (c), (d), (e) or (f) such
that the classified particles have a D1 particle diameter of at least 0.5 1-Jm.
5
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30. A particulate material consisting of a plurality of composite particles, wherein the
composite particles comprise:
(a)
(b)
a porous particle framework comprising micropores and mesopores,
wherein the micropores and mesopores have a total pore volume as
measured by nitrogen gas adsorption of 0.4 to 2.0 cm3/g, and
a plurality of nanoscale electroactive material domains located within the
pores of the porous particle framework,
wherein the composite particles have a 01 particle diameter of at least 0.5 1-Jm, and a
Oso particle diameter in the range from 1 to 20 1-Jm, and a BET surface area of no more
1 o than 50 m2/g.
31. A particulate material according to claim 30, wherein the 01 particle diameter of
the composite particles is at least 0.8 1-Jm, or at least 1.0 1-Jm, or at least 1.2 1-Jm, or at
least 1.4 1-Jm, or at least 1.5 1-Jm, or at least 1.6 1-Jm, or at least 1.8 1-Jm, or at least 2.0 1-Jm,
or at least 2.2 1-Jm, or at least 2.4 1-Jm, or at least 2.5 1-Jm, or at least 2.6 1-Jm, or at least
15 2.8 1-Jm, or at least 3.0 1-Jm.
32. A particulate material according to claim 30 or claim 31, wherein the Oso particle
diameter of the composite particles is in the range from 1.5 to 18 1-Jm, or in the range
from 1.5 to 15 1-Jm, or in the range from 2 to 12 1-Jm, or in the range from 2 to 10 1-Jm, or
in the range from 2.5 to 8 1-Jm, or in the range from 3 to 8 1-Jm.
20 33. A particulate material according to any of claims 30 to 32, wherein the Ogo
particle diameter of the composite particles is no more than 30 1-Jm, or no more than
25 1-Jm, or no more than 20 1-Jm, or no more than 18 1-Jm, or no more than 16 1-Jm, or no
more than 15 1-Jm, or no more than 12 1-Jm.
34. A particulate material according to claim 33, wherein the 01 particle diameter of
25 the composite particles is in the range from 1.5. to 4.5 1-1m and the Ogo particle diameter
is in the range from 9 to 15 1-Jm, preferably wherein the 01 particle diameter of the
composite particles is in the range from 2 to 4 1-1m and the Ogo particle diameter is in the
range from 10 to 14 1-Jm, preferably wherein the 01 particle diameter of the composite
particles is in the range from 2.5 to 3.5 1-1m and the Ogo particle diameter is in the range
30 from 11 to 131-Jm,
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35. A particulate material according to any of claims 30 to 34, wherein the Oga
particle diameter of the composite particles is no more than 35 1-Jm, or no more than
30 1-Jm, or no more than 25 1-Jm, or no more than 20 1-Jm, or no more than 18 1-Jm, or no
more than 16 1-Jm, or no more than 15 1-Jm, or no more than 12 1-Jm.
5 36. A particulate material according to any of claims 30 to 35, wherein the D10o
particle diameter of the composite particles is no more than 40 1-Jm, or no more than
35 1-Jm, or no more than 30 1-Jm, or no more than 25 1-Jm, or no more than 20 1-Jm.
37. A particulate material according to any of claims 30 to 36, wherein the difference
between the Oga particle diameter and the 01 particle diameter of the composite particles
10 (Oga-01) is no more than 18 1-Jm, or no more than 16 1-Jm, or no more than 15 1-Jm, or no
more than 14 1-Jm, or no more than 13 1-Jm, or no more than 12 1-Jm.
38. A particulate material according to any of claims 30 to 37, wherein the ratio of
the Oga particle diameter to the 01 particle diameter of the composite particles (Oga/01) is
no more than 12, or no more than 10, or no more than 8, or no more than 6, or no more
15 than5.
39. A particulate material according to any of claims 30 to 38, wherein (Oga-D1)/0so
of the composite particles is no more than 2.2, or no more than 2, or no more than 1.9,
or no more than 1.8, or no more than 1.7, or no more than 1.6.
40. A particulate material according to any of claims 30 to 39, wherein the difference
20 between the Ogo particle diameter and the 01 particle diameter of the composite particles
(Ogo-01) is no more than 12.0 1-Jm, or no more than 10.0 1-Jm, or no more than 9.0 1-Jm, or no
more than 8.0 1-Jm.
41. A particulate material according to any of claims 30 to 40, wherein the ratio of
the Ogo particle diameter to the 01 particle diameter of the composite particles (Ogo/01) is
25 no more than 12.0, or no more than 10.0, or no more than 9.0, or no more than 8.0, or no
more than 7.0, or no more than 6.0, or no more than 5.0.
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42. A particulate material according to any of claims 30 to 41, wherein (Ogo-D1)/Dso
of the composite particles is no more than 2.2, or no more than 2, or no more than 1.9,
or no more than 1.8, or no more than 1.7, or no more than 1.6.
43. A particulate material according to any of claims 30 to 42, wherein the ratio of
5 the Dso particle diameter to the D1 particle diameter of the composite particles is no
more than 1 0.0, or no more than 8.0, or no more than 7.0, or no more than 6.0, or no
more than 5.0, or no more than 4.0, or no more than 3.0.
44. A particulate material according to any of claims 30 to 43, wherein the particle
size distribution of the composite particles has a positive skew.
10 45. A particulate material according to any of claims 30 to 44, wherein the total pore
volume of micropores and mesopores in the porous particle framework as measured by
nitrogen gas adsorption is in the range from 0.4 to 1.8 cm3/g, or from 0.4 to 1.7 cm3/g,
or from 0.5 to 1.6 cm3/g, or from 0.5 to 1.55 cm3/g, or from 0.6 to 1.5 cm3/g, or from 0.6
to 1.45 cm3/g, or from 0.65 to 1.4 cm3/g, or from 0.65 to 1.35 cm3/g, or from 0.7 to
15 1.3 cm3/g, or from 0.7 to 1.25 cm3/g, or from 0.75 to 1.2 cm3/g, or from 0.75 to 1.1 cm3/g,
or from 0.8 to 1.15 cm3/g, or from 0.8 to 1.1 cm3/g.
46. A particulate material according to any of claims 30 to 45, wherein the PDso pore
diameter of the porous particle framework is no more than 10 nm, or no more than 8 nm,
or no more than 6 nm, or no more than 5 nm, or no more than 4 nm, or no more than
20 3 nm, or no more than 2.5 nm, or no more than 2 nm, or no more than 1.9 nm, or no
more than 1.8 nm, or no more than 1. 7 nm, or no more than 1.6 nm.
47. A particulate material according to any of claims 30 to 46, wherein the POgo pore
diameter of the porous particle framework is in the range from 3.2 to 20 nm, or from 3.5
to 15 nm, or from 3.8 to 10 nm, or from 4 to 8 nm.
25 48. A particulate material according to any of claims 30 to 47, wherein the micropore
volume fraction of the porous particle framework is at least 0.4, or at least 0.45, or at
least 0.5, or at least 0.55, or at least 0.6 based on the total volume of micropores and
mesopores.
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49. A particulate material according to any of claims 30 to 48, wherein the micropore
volume fraction of the porous particle framework is no more than 0.85, or no more than
0.8 based on the total volume of micropores and mesopores.
50. A particulate material according to any of claims 30 to 49, wherein the porous
5 particle framework has a BET surface area in the range from 100 m2/g to 4,000 m2/g,
or from 500 m2/g to 4,000 m2/g, or from 750 m2/g to 3,500 m2/g, or from 1,000 m2/g to
3,250 m2/g, or from 1,000 m2/g to 3,000 m2/g, or from 1,000 m2/g to 2,500 m2/g, or from
1,000 m2/g to 2,000 m2/g.
51. A particulate material according to any of claims 30 to 50, wherein the porous
10 particle framework is a conductive porous particle framework, preferably a conductive
porous carbon particle framework, more preferably a conductive porous carbon particle
framework comprising at least 80 wt% carbon, or at least 85 wt% carbon, or at least
90 wt% carbon, or at least 95 wt% carbon.
52. A particulate material according to any of claims 30 to 51, wherein the
15 electroactive material is selected from silicon, tin, germanium, aluminium and mixtures
and alloys thereof, preferably wherein the electroactive material is silicon.
53. A particulate material according to any of claims 30 to 52, comprising at least 26
wt% of the electroactive material, or at least 28 wt% of the electroactive material, or at
least 30 wt% of the electroactive material, or at least 32 wt% of the electroactive
20 material, or at least 34 wt% of the electroactive material, or at least 36 wt% of the
electroactive material, or at least 38 wt% of the electroactive material, or at least 40 wt%
of the electroactive material, or at least 42 wt% of the electroactive material, or at least
44 wt% of the electroactive material, preferably wherein the electroactive material is
silicon.
25 54. A particulate material according to claim 52, wherein the weight ratio of silicon
to the porous particle framework is in the range from [0.50xP1 to 1.9xP1
] : 1, or from
[0.6xP1 to 1.8xP1
] : 1 or from [0.7xP1 to 1.7xP1
] : 1, or from [0.8xP1 to 1.6xP1
] : 1,
wherein P1 represents a dimensionless number having the same value as the total pore
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volume of micropores and mesopores in the porous particle framework as measured by
gas adsorption as expressed in cm3/g.
55. A particulate material according to any of claims 52 to 54, wherein at least 22
wt%, or at least 25 wt%, or at least 30 wt%, or at least 35 wt%, or at least 40 wt% of the
5 silicon, or at least 45 wt% of the silicon in the composite particles is surface silicon as
determined by thermogravimetric analysis (TGA).
56. A particulate material according to any of claims 52 to 55, wherein no more than
10 wt% of the silicon, or no more than 8 wt% of the silicon, or no more than 6 wt% of
the silicon, or no more than 5 wt%,or no more than 4 wt%, or no more than 3 wt%, or
10 no more than 2 wt% or no more than 1.5 wt% of the silicon in the composite particles is
coarse bulk silicon as determined by thermogravimetric analysis (TGA).
57. A particulate material according to any of claims 30 to 56, wherein the composite
particles have a BET surface area of no more than 100 m2/g, or no more than 80 m2/g,
or no more than 60 m2/g, or no more than 50 m2/g, or no more than 40 m2/g, or no more
15 than 30 m2/g, or no more than 25 m2/g, or no more than 20 m2/g, or no more than 15
m2/g, or no more than 10 m2/g, or no more than 5 m2/g.
58. A particulate material according to any of claims 30 to 57, further comprising a
passivation layer formed on the surfaces of the nanoscale electroactive material
domains, conductive carbon layer, a conductive metal layer, or a lithium-ion permeable
20 solid electrolyte layer.
59. A particulate material according to any of claims 30 to 58, wherein the composite
particles are non-agglomerated and non-aggregated particles.
60. A composition comprising the particulate material of any of claims 30 to 59 and
at least one other component.
25 61. An electrode comprising the particulate material of any of claims 30 to 59 or the
composition of claim 60.
62. A rechargeable metal-ion battery comprising the electrode of claim 61.