Dissociation of (Li 2 O 2 ) 0,+ on graphene and boron-doped graphene: insights from first-principles calculations
Reducing charge overpotential is of great significance to enhance the efficiency and cyclability of Li–O 2 batteries. Here, a dramatically reduced charge overpotential via boron-doped graphene as a catalytic substrate is successfully predicted. By first-principles calculations, from the perspective...
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Veröffentlicht in: | Physical chemistry chemical physics : PCCP 2020-01, Vol.22 (25), p.14216-14224 |
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Format: | Artikel |
Sprache: | eng |
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Zusammenfassung: | Reducing charge overpotential is of great significance to enhance the efficiency and cyclability of Li–O
2
batteries. Here, a dramatically reduced charge overpotential
via
boron-doped graphene as a catalytic substrate is successfully predicted. By first-principles calculations, from the perspective of reaction thermodynamics and kinetics, the results show that the electrochemical oxidation of the Li
2
O
2
+
cation is easier than the chemical oxidation of the neutral Li
2
O
2
molecule, and the oxidation of (Li
2
O
2
)
0,+
is facilitated by boron-doping in pristine graphene. More importantly, the results reveal the oxidation mechanism of (Li
2
O
2
)
0,+
: two-step dissociation with the LiO
2
molecule as a reactive intermediate has advantages over one-step dissociation; the rate-determining step for the dissociation of (Li
2
O
2
+
)
G
is the oxygen evolution process, while the lithium removal process is the rate-determining step for the dissociation of (Li
2
O
2
0
)
G
, (Li
2
O
2
0
)
BG
, and (Li
2
O
2
+
)
BG
. |
---|---|
ISSN: | 1463-9076 1463-9084 |
DOI: | 10.1039/d0cp02597f |