Microscopic insights into hydrophobicity of cerium oxide: Effects of crystal orientation and lattice constant

doi:10.1016/j.jmst.2021.08.064

Abstract

Abstract:

Cerium oxide possesses intrinsic hydrophobic properties ascribed to the unique electronic structure. However, the relationship between the crystal structure and hydrophobicity of cerium oxide has not been systematically studied. Herein, it is experimentally and theoretically demonstrated that the water contact angle (105.9°) of the (111) surface is higher than that (91.7°) of the (220) surface, associated with the lower surface free energy (28.44 mN/m) of (111) surface than that (38.48 mN/m) of (220) surface. Furthermore, cerium oxide films with (111)-terminated surface are annealed at 300 °C and 600 °C for 1 h, respectively. The lattice constant increases (5.4594 Å < 5.4613 Å < 5.4670 Å) with decreasing the annealing temperature (600 °C > 300 °C > the as-deposited), leading to the increased water contact angle (96.7° < 96.8° < 99.0°). The First-principles calculation provides microscopic insights into the wetting mechanism, originating from the weakened adsorption capacity of the (111) surface for water molecules with the increasing lattice constant.

Key words: Cerium oxide, Hydrophobicity, Lattice constant, Crystal orientation

Dapeng Zhu, Weiwei Liu, Rongzhi Zhao, Zhen Shi, Xiangyang Tan, Zhenhua Zhang, Yixing Li, Lianze Ji, Xuefeng Zhang. Microscopic insights into hydrophobicity of cerium oxide: Effects of crystal orientation and lattice constant[J]. J. Mater. Sci. Technol., 2022, 109: 20-29.

Figures/Tables 11

Fig. 1. (a) The XRD patterns of different oxygen flow rations (2% and 42%), (b) The magnified XRD patterns in (a).

Fig. 2. (a) The FIB cut cerium oxide sample cross-sectional images with oxygen flow ratio 42%. (b) and (c) the HRTEM images take from the dotted rectangle in (a) and (d), respectively. (d) The cross-section EDS images of the cerium oxide sample take from the dotted rectangle in (a). (e) and (f) Fast Fourier Transform (FFT) patterns taken from the dotted square in (b) and (c), respectively. (g) The FIB cut cerium oxide sample cross-sectional images with oxygen flow ratio 2%. (h) and (i) the HRTEM images take from the dotted rectangle in (g) and (j), respectively. (j) The cross-section EDS images of cerium oxide sample take from the dotted rectangle in (g). (k) and (l) Fast Fourier Transform (FFT) patterns taken from the dotted square in (h) and (i), respectively.

Table 1. Atomic fraction of cerium oxide with different oxygen flow rations.

Oxygen flow ratios (at.%)	Atomic fraction (at.%)			O/Ce
Empty Cell	Si	O	Ce	Empty Cell
42%	0.56	68.47	30.97	2.21
2%	1.57	68.96	29.47	2.34

Fig. 3. (a) The XPS spectra of cerium oxide surface with high oxygen and low oxygen. (b), (c) and (d) O 1 s and C 1 s and Ce 3d XPS spectra of the cerium oxide surface, respectively. (e) The relative content of Ce3+ and Ce4+. (f) The relative element content of Olatt and C-C/C-H.

Fig. 4. (a) and (b) Schematic representation of the adsorption energy of water molecules on the (111) surface and the (220) surface, respectively. (c) The relationship between adsorption energy and different orientations. (d) and (e) the projected density of states (PDOS) of O(a)-H(a) bond and O(b)-H(b) bond of the (111) surface, respectively. (f) and (g) the projected density of states (PDOS) of O(a)-H(a) bond and O(b)-H(b) bond of the (220) surface, respectively.

Fig. 5. (a) The XRD pattern of different annealing temperatures (as-deposited, 300 °C and 600 °C). (b) The magnified XRD pattern of (111) orientation in (a).

Fig. 6. (a) The XPS spectra of the cerium oxide surface with different annealing temperatures. (b), (c) and (d) are O 1 s, C 1 s and Ce 3d XPS spectra of the cerium oxide surface, respectively. (e) The relative element content of Ce3+ and Ce4+. (f) The relative element content of C-C/C-H and molecular water.

Fig. 7. (a), (b) and (c) Schematic representations of the adsorption energy of the water molecule on the (111) surface under different lattice strain (0.012, 0.018 and 0.042), respectively. (d) The relationship between lattice constant and interplanar spacing of (111) surface. (e) The relationship between adsorption energy and lattice constant of (111) surface.

Fig. 8. (a), (d) and (g) O(a)-H(a) bond of the projected density of states (PDOS) of the water molecule on the (111) surface under different lattice constants (5.394 Å, 5.426 Å and 5.554 Å), respectively. (b), (e) and (h) O(b)-H(b) bond of the projected density of states (PDOS) of the water molecule on the (111) surface under different lattice constants (5.394 Å, 5.426 Å and 5.554 Å), respectively. (c), (e) and (i) schematic of the O-H bond of the projected density of states (PDOS) of the water molecule on the (111) surface under different lattice constants (5.394 Å, 5.426 Å and 5.554 Å), respectively.

Fig. 9. (a) The relationship between the water contact angle and the different crystal orientations. (c) The relationship between water contact angle and different lattice constants.

Table 2. The water contact angle (WCA) and the diiodiomethane contact angle (DCA) and surface free energy (SFE), the polar parts and the dispersive parts of surface free energy of solid and liquid $\left( \gamma _{\text{SV}}^{\text{p}},\gamma _{\text{LV}}^{\text{p}},\gamma _{\text{SV}}^{\text{d}},\gamma _{\text{LV}}^{\text{d}} \right)$.

Oxygen flow ratio	High oxygen (42%)	Low oxygen (2%)
WCA (°)	105.9	91.7
DCA (°)	60.4	43.9
SFE (mN/m)	28.44	38.48
$\gamma _{\text{SV}}^{\text{d}}$ (mN/m)	28.38	37.60
$\gamma _{\text{SV}}^{\text{p}}$ (mN/m)	0.06	0.88
$\gamma _{\text{LV}}^{\text{d}}$ (mN/m)	51.00	51.00
$\gamma _{\text{LV}}^{\text{p}}$ (mN/m)	21.80	21.80

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