Density function theory calculations were carried out to clarify storage states of Lithium (Li) ions in graphene clusters. The adsorption energy, spin polarization, charge distribution, electronic gap, surface curvature, and dipole momentum were calculated for each cluster. Li-ion adsorbed graphene, doped by one Li atom is spin polarized, so there would be different gaps for different spin polarization in electrons. Calculation results demonstrated that a smaller cluster between each two larger clusters is preferable, because it could improve graphene Li-ion batteries; consequently, the most proper graphene anode structure has been proposed.

1.
S. L.
Cheekatia
,
Y.
Xing
,
Y.
Zhuang
, and
H.
Huang
, “
Lithium storage characteristics for nano-graphene plates
,” in
Material Challenges in Alternative and Renewable Energy: Ceramic Transaction
, edited by
W. G.
George
,
J.
Simon
R.
Zidan
,
E.
Lara-Curzio
,
T.
Adams
,
J.
Zayas
 et al (
Wiley
,
2011
), Vol.
224
, pp.
117
127
.
2.
K.
Sato
,
M.
Noguchi
,
A.
Demachi
,
N.
Oki
, and
M.
Endo
, “
A mechanism of lithium storage in disordered carbons
,”
Science
264
,
556
558
(
1994
).
3.
J. M.
Tarascon
and
M.
Armand
, “
Issues and challenges facing rechargeable lithium batteries
,”
Nature (London)
414
,
359
367
(
2001
).
4.
P.
Lian
,
X.
Zhu
,
S.
Liang
,
Z.
Li
,
W.
Yang
, and
H.
Wang
, “
Large reversible capacity of high quality graphene sheets as an anode material for lithium-ion batteries
,”
Electrochim. Acta.
55
,
3909
3914
(
2010
).
5.
Y.
Idota
,
T.
Kubota
,
A.
Matsufuji
,
Y.
Maekawa
, and
T.
Miyasaka
, “
Tin-based amorphous oxide: A high-capacity lithium-ion-storage material
,”
Science
276
,
1395
1397
(
1997
).
6.
P.
Poizot
,
S.
Laruelle
,
S.
Grugeon
,
L.
Dupont
, and
J. M.
Tarascon
, “
Nano-sized transition-metal oxides as negative-electrode materials for lithium-ion batteries
,”
Nature (London)
407
,
496
499
(
2000
).
7.
H.
Zhou
,
S.
Zhu
,
M.
Hibino
,
I.
Honma
, and
M.
Ichihara
, “
Lithium storage in ordered mesoporous carbon (CMK-3) with high reversible specific energy capacity and good cycling performance
,”
Adv. Mater.
15
,
2107
2111
(
2003
).
8.
P. L.T.
aberna
,
S.
Mitra
,
P.
Poizot
,
P.
Simon
, and
J. M.
Tarascon
, “
High rate capabilities Fe3O4-based Cu nano-architectured electrodes for lithium-ion battery applications
,”
Nat. Mater.
5
,
567
573
(
2006
).
9.
C. K.
Chan
,
H.
Peng
,
G.
Liu
,
K. M.
Wrath
,
X. F.
Zhang
,
R. A.
Huggins
 et al, “
High-performance lithium battery anodes using silicon nanowires
,”
Nat. Nanotechnol.
3
,
31
35
(
2008
).
10.
K. S.
Novoselov
,
A. K.
Geim
,
S. V.
Morozov
,
Y.
Zhang
,
S. V.
Dubonos
 et al, “
Electric field effect in atomically thin carbon films
,”
Science
306
,
666
669
(
2004
).
11.
J. C.
Meyer
,
A. K.
Geim
,
M. I.
Katsnelson
,
K. S.
Novoselov
,
T. J.
Booth
,
S.
Roth
 et al, “
The structure of suspended graphene sheets
,”
Nature (London)
446
,
60
63
(
2007
).
12.
J.
Hou
,
Y.
Shao
,
M.
Ellis
,
B. R.
Moore
, and
B.
Yi
, “
Graphene-based electrochemical energy conversion and storage: fuel cells, supercapacitors and lithium ion batteries
,”
Phys. Chem. Chem. Phys.
13
,
15384
15402
(
2011
).
13.
X.
Du
,
I.
Skachko
,
A.
Barker
, and
E. Y.
Andrei
, “
Approaching ballistic transport in suspended graphene
,”
Nat. Nanotechnol.
3
,
491
495
(
2008
).
14.
C. N. R.
Rao
,
A. K.
Sood
,
R.
Voggu
, and
K. S.
Subrahmanyam
, “
Some novel attributes of graphene
,”
J. Phys. Chem. Lett.
1
,
572
580
(
2010
).
15.
G.
Wang
,
X.
Shen
,
J.
Yao
, and
J.
Park
, “
Graphene nanosheets for enhanced lithium storage in lithium ion batteries
,”
Carbon
47
,
2049
2053
(
2009
).
16.
G.
Forte
,
F.
Grossi
,
G. M.
Lombardo
,
A.
La Magna
,
G. G. N.
Angilella
,
P.
Pucci
 et al, “
Modeling vacancies and hydrogen impurities in graphene: A molecular point of view
,”
Phys. Lett. A
372
,
6168
6174
(
2008
).
17.
C. M.
Dharma-Wandra
and
M. Z.
Zgierski
, “
Magnetism and structure at vacant lattice sites in graphene
,”
Physica E
41
,
80
83
(
2008
).
18.
D.
Moran
,
F.
Sthal
,
H. F.
Bettinger
, and
P.
Schleyer
, “
Towards graphite: Magnetic properties of large polybenzenoid hydrocarbons
,”
J. Am. Chem. Soc.
125
,
6746
6752
(
2003
).
19.
J.
Cho
,
S.
Lim
,
J.
Cha
, and
N.
Park
, “
Analysis of the strong propensity for the delocalized diamagnetic π electronic structure of hydrogenated graphenes
,”
Carbon
49
,
2665
2670
(
2011
).
20.
E. J.
Yoo
,
J.
Kim
,
E.
Hosono
,
H. S.
Zhou
,
T.
Kudo
, and
I.
Honma
, “
Large reversible Li storage of graphene nanosheet families for use in rechargeable lithium ion batteries
,”
Nano Lett.
8
,
2277
2282
(
2008
).
21.
G.
Wang
,
B.
Wang
,
X.
Wang
,
J.
Park
,
S.
Dou
,
H.
Ahn
, and
K.
Kim
, “
Sn/graphene nanocomposite with 3D architecture for enhanced reversible lithium storage in lithium ion batteries
,”
J. Mater. Chem.
19
,
8378
8384
(
2009
).
22.
N.
Kurita
and
M.
Endo
, “
Molecular orbital calculations on electronic and Li-adsorption properties of sulfur-, phosphorus- and silicon-substituted disordered carbons
,”
Carbon
40
,
253
260
(
2002
).
23.
J. R.
Dahn
,
T.
Zheng
,
Y. H.
Liu
, and
J. S.
Xue
, “
Mechanism for lithium insertion in carbonaceous materials
,”
Science
270
,
590
593
(
1995
).
24.
Y. H.
Liu
,
J. S.
Xue
,
T.
Zheng
, and
J. R.
Dahn
, “
Mechanism of lithium insertion in hard carbons prepared by pyrolysis of epoxy resins
,”
Carbon
34
,
193
200
(
1996
).
25.
H.
Tachikawa
and
A.
Shimizu
, “
Diffusion dynamics of the Li atom on amorphous carbon: A direct molecular orbital–molecular dynamics study
,”
J. Phys. Chem. B.
110
,
20445
20450
(
2006
).
26.
C. A.
Lin
,
T.
Liedl
,
R. A.
Sperling
,
M. T.
Fernández-Argüelles
,
J. M.
Costa-Fernández
, and
R.
Pereiro
, “
Bioanalytics and biolabeling with semiconductor nanoparticles (quantum dots)
,”
J. Mater. Chem.
17
,
1343
1346
(
2007
).
27.
D.
Wang
,
R.
Kou
,
D.
Choi
,
Z.
Yang
,
Z.
Nie
,
J.
Li
 et al, “
Ternary self-assembly of ordered metal oxide-graphene nanocomposites for electrochemical energy storage
,”
ACS Nano.
4
,
1587
1595
(
2010
).
28.
M.
Winter
and
R. J.
Broad
, “
What are batteries, fuel cells, and supercapacitors?
Chem. Rev.
105
,
1021
(
2005
).
29.
P. G.
Brouce
,
B.
Scrosati
,
J. M.
Tarascon
, “
Nanomaterials for rechargeable lithium batteries
,”
Angew Chem. Int. Ed.
47
,
2930
2946
(
2008
).
30.
M.
Walkihara
, “
Recent developments in lithium ion batteries
,”
Mater. Sci. Eng. R
33
,
109
134
(
2001
).
31.
A.
Marquez
,
A.
Vargas
, and
P. B.
Balbuena
, “
Computational studies of lithium intercalation in model graphite in the presence of tetrahydrofuran
,”
J. Electrochem. Soc.
145
,
3328
3334
(
1998
).
32.
M.
Nakadaira
,
R.
Saito
,
T.
Kimura
,
G.
Dresselhaus
, and
M. S.
Dresselhaus
, “
Excess Li ions in a small graphite cluster
,”
J. Mater. Res.
12
,
1367
1375
(
1997
).
33.
M.
Fujita
,
K.
Wakabayashi
,
K.
Nakada
, and
K.
Kusakabe
, “
Peculiar localized state at zigzag graphite edge
,”
J. Phys. Soc. Jpn.
65
,
1920
1923
(
1996
).
34.
R. C.
Boehm
and
A.
Banerjee
, “
Theoretical study of lithium intercalated graphite
,”
J. Chem. Phys.
96
,
1150
1158
(
1992
).
35.
D. J.
Hankinson
and
J.
Almlöf
, “
Cluster models for lithium intercalated graphite: Electronic structures and energetic
,”
J. Mol. Struct. Theochem.
388
,
245
256
(
1996
).
36.
S.
Ishikawa
,
G.
Madjarova
, and
T.
Yamaba
, “
First-principles study of the lithium interaction with polycyclic aromatic hydrocarbons
,”
J. Phys. Chem. B
105
,
11986
11993
(
2001
).
37.
H.
Tachikawa
,
Y.
Nagoya
, and
T.
Fukuzumi
, “
Density functional theory (DFT) study on the effects of Li+doping on electronic states of graphene
,”
J. Power Sources
195
,
6148
6152
(
2010
).
38.
M. J.
Frisch
,
G. W.
Trucks
,
H. B.
Schlegel
,
G. E.
Scuseria
,
M. A.
RobbA
,
J. R.
Cheeseman
 et al,
Gaussian 03, Revision B.02
,
Gaussian, Inc
.
Pittsburgh, PA
,
2003
.
39.
A. D.
Becke
, “
Density‐functional thermochemistry. III. The role of exact exchange
,”
J. Chem. Phys.
98
,
5648
5652
(
1993
).
40.
C.
Lee
,
W.
Yang
, and
R. G.
Parr
, “
Development of the Colle-Salvetti correlation-energy formula into a functional of the electron density
,”
Phys. Rev. B
37
,
785
789
(
1988
).
41.
GaussSum 2.1 (c) 2007, Noel O'Boyl.
42.
N.
Kheirabadi
and
A.
Shafiekhani
, “
The ground state of graphene and graphene disordered by vacancies
,”
Physica E
(in press).
43.
T.
Suzuki
,
T.
Hasegawa
,
S.
Mukai
, and
H. A.
Tamon
, “
A theoretical study on storage states of Li ions in carbon anodes of Li ion batteries using molecular orbital calculations
,”
Carbon
41
,
1933
1939
(
2003
).
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