Water confined within nanochannels with specific functionalities serves as the foundation for a variety of emerging nanofluidic applications. However, the structure and dynamics of the confined liquid are susceptibly influenced by practically hard-to-avoid defects, yet knowledge of this fact remains largely unexplored. Here, using extensive molecular dynamics simulations, we elucidate the significant influence of geometric and charge defects on one-dimensional confined water. We show that the two types of defects can both reshape the water density distribution by constraining the translocation of water molecules along the circumferential direction. In addition to structural alterations, collective translocation and rotation of water slabs arise during transportation under external pressure. Below the temperature threshold marking the initiation of liquid-solid transition, the geometric defect retards water diffusion through a pinning effect, while the charge defect induces an anti-freezing effect. The latter is attributed to the electrostatic interaction between the charge defect and water molecules that hinders the formation of a stable hydrogen bond network by disrupting molecular dipole orientation. Consequently, this behavior results in a reduction in the number and lifetime of hydrogen bonds within the phase transition interval. The distinct roles of the two types of defects could be utilized to control the structure and dynamics of confined liquids that may result in distinct functionalities for nanofluidic applications.

1.
Y.
Li
,
S.
Gu
,
C.
Dai
, and
Y.
Wu
,
Geofluids
2021
,
1
.
2.
I.
Johansson
,
M.
Karlsson
,
U.
Johanson
,
C.
Larsson
, and
P.
Kjellbom
,
Biochim. Biophys. Acta, Biomembr.
1465
,
324
(
2000
).
3.
J.
Qian
,
X.
Gao
, and
B.
Pan
,
Environ. Sci. Technol.
54
,
8509
(
2020
).
5.
F.
Wang
,
J.
Qian
,
J.
Fan
,
J.
Li
,
H.
Xu
, and
H.
Wu
,
Sci. China: Phys., Mech. Astron.
65
,
264601
(
2022
).
6.
A.
Esfandiar
,
B.
Radha
,
F. C.
Wang
,
Q.
Yang
,
S.
Hu
,
S.
Garaj
,
R. R.
Nair
,
A. K.
Geim
, and
K.
Gopinadhan
,
Science
358
,
511
(
2017
).
8.
G.
Hummer
,
J. C.
Rasaiah
, and
J. P.
Noworyta
,
Nature
414
,
188
(
2001
).
9.
D.
Takaiwa
,
I.
Hatano
,
K.
Koga
, and
H.
Tanaka
,
Proc. Natl. Acad. Sci. U. S. A.
105
,
39
(
2008
).
10.
A.
Noy
,
H. G.
Park
,
F.
Fornasiero
,
J. K.
Holt
,
C. P.
Grigoropoulos
, and
O.
Bakajin
,
Nano Today
2
,
22
(
2007
).
12.
P.
Robin
and
L.
Bocquet
,
J. Chem. Phys.
158
,
160901
(
2023
).
14.
L.
Bocquet
and
E.
Charlaix
,
Chem. Soc. Rev.
39
,
1073
(
2010
).
15.
S. G.
Louie
, “
Electronic properties, junctions, and defects of carbon nanotubes
,” in
Carbon Nanotubes: Synthesis, Structure, Properties, and Applications
(
Springer
,
2001
), Vol.
113
.
16.
M. S.
Dresselhaus
,
A.
Jorio
,
A. G.
Souza Filho
, and
R.
Saito
,
Philos. Trans. R. Soc., A
368
,
5355
(
2010
).
17.
A.
Seal
and
A.
Govind Rajan
,
Nano Lett.
21
,
8008
(
2021
).
18.
C. Y.
Won
and
N. R.
Aluru
,
J. Am. Chem. Soc.
130
,
13649
(
2008
).
19.
N.
Karousis
,
N.
Tagmatarchis
, and
D.
Tasis
,
Chem. Rev.
110
,
5366
(
2010
).
20.
21.
S.
Faucher
et al,
J. Phys. Chem. C
123
,
21309
(
2019
).
22.
X.
Li
,
L.
Li
,
Y.
Wang
,
H.
Li
, and
X.
Bian
,
J. Phys. Chem. C
117
,
14106
(
2013
).
23.
L.
Joly
,
G.
Tocci
,
S.
Merabia
, and
A.
Michaelides
,
J. Phys. Chem. Lett.
7
,
1381
(
2016
).
24.
W.
Humphrey
,
A.
Dalke
, and
K.
Schulten
,
J. Mol. Graphics
14
,
33
(
1996
).
25.
L.
Kale
et al,
J. Comput. Phys.
151
,
283
(
1999
).
26.
J.
Huang
,
S.
Rauscher
,
G.
Nawrocki
,
T.
Ran
,
M.
Feig
,
B. L.
De Groot
,
H.
Grubmüller
, and
A. D.
MacKerell
, Jr.
,
Nat. Methods
14
,
71
(
2017
).
27.
J.
Huang
and
A. D.
MacKerell
, Jr.
,
J. Comput. Chem.
34
,
2135
(
2013
).
28.
J. L.
Abascal
and
C.
Vega
,
J. Chem. Phys.
123
,
234505
(
2005
).
29.
U.
Essmann
,
L.
Perera
,
M. L.
Berkowitz
,
T.
Darden
,
H.
Lee
, and
L. G.
Pedersen
,
J. Chem. Phys.
103
,
8577
(
1995
).
30.
S. E.
Feller
,
Y.
Zhang
,
R. W.
Pastor
, and
B. R.
Brooks
,
J. Chem. Phys.
103
,
4613
(
1995
).
31.
D. C.
Rapaport
,
The Art of Molecular Dynamics Simulation
(
Cambridge University Press
,
2004
).
32.
A.
Luzar
and
D.
Chandler
,
Phys. Rev. Lett.
76
,
928
(
1996
).
34.
A.
Chandra
,
J. Phys. Chem. B
107
,
3899
(
2003
).
35.
R. J.
Gowers
and
P.
Carbone
,
J. Chem. Phys.
142
,
224907
(
2015
).
36.
K.
Falk
,
F.
Sedlmeier
,
L.
Joly
,
R. R.
Netz
, and
L.
Bocquet
,
Nano Lett.
10
,
4067
(
2010
).
37.
S.
Jiao
,
C.
Duan
, and
Z.
Xu
,
Sci. Rep.
7
,
2646
(
2017
).
38.
M.
Xue
,
Z.
Hu
,
H.
Qiu
,
C.
Shen
,
W.
Guo
, and
Z.
Zhang
,
Natl. Sci. Rev.
9
,
nwab214
(
2022
).
39.
K. V.
Agrawal
,
S.
Shimizu
,
L. W.
Drahushuk
,
D.
Kilcoyne
, and
M. S.
Strano
,
Nat. Nanotechnol.
12
,
267
(
2017
).
41.
Y.-g.
Zheng
,
H.-f.
Ye
,
Z.-q.
Zhang
, and
H.-w.
Zhang
,
Phys. Chem. Chem. Phys.
14
,
964
(
2012
).
42.
H.
Ye
,
H.
Zhang
,
Y.
Zheng
, and
Z.
Zhang
,
Microfluid. Nanofluid.
10
,
1359
(
2011
).
43.
M.
Xue
,
H.
Qiu
,
C.
Shen
,
Z.
Zhang
, and
W.
Guo
,
J. Phys. Chem. Lett.
13
,
4815
(
2022
).
44.
Q.
Wang
,
L.
Liu
,
C.
Liu
,
J.
Song
, and
X.
Gao
,
J. Mol. Liq.
334
,
116034
(
2021
).
45.
J.-P.
Hansen
and
L.
Verlet
,
Phys. Rev.
184
,
151
(
1969
).
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