Citation: LI Lu, LI Yi, GUO Xin, ZHANG Yong-Fan, CHEN Wen-Kai. Adsorption and Dissociation of Water on HfO₂(111) and (110) Surfaces[J]. Acta Physico-Chimica Sinica, ;2013, 29(05): 937-945. doi: 10.3866/PKU.WHXB201303081 shu

Adsorption and Dissociation of Water on HfO₂(111) and (110) Surfaces

LI Lu ¹ ,
LI Yi ¹ ,
GUO Xin ² ,
ZHANG Yong-Fan ¹ ,
CHEN Wen-Kai ^1,3,

1.
1 Department of Chemistry, Fuzhou University, Fuzhou 350116, P. R. China;
2 States Key Laboratory of Coal combustion, Huazhong University of Science and Technology, Wuhan, Hubei, 410074, P. R. China;
3 Fujian Provincial Key Laboratory of Photocatalysis-State Key Laboratory Breeding Base, Fuzhou University, Fuzhou 350002, P. R. China

Received Date: 12 November 2012
Available Online: 8 March 2013
Fund Project: 福建省自然科学基金(2012J01032, 2012J01041) (2012J01032, 2012J01041)华中科技大学煤燃烧国家重点实验室开放基金(FSKLCC1110)资助项目 (FSKLCC1110)

First-principles calculations based on density functional theory (DFT) with the generalized gradient approximation (GGA-PW91) have been used to investigate the adsorption and dissociation of H₂O molecules on HfO₂(111) and (110) surfaces at different sites with different coverages. It was found that the surface hafnium atom was the active adsorption position of the (111) and (110) surfaces when compared different adsorption energies and various geometrical parameters. Adsorption energies of water on the HfO₂ (111) and (110) surfaces varied slightly as the coverage increased. It was shown that the most favorable configuration of H₂O on the HfO₂(111) and (110) surfaces corresponded to the coordination of H₂O via its oxygen to a surface hafnium atom. Adsorption geometries, Mulliken population charges, density of states, and frequency calculations for HfO₂-OH, HfO₂-O, and HfO₂-H at both surfaces were also carried out. The results showed that the hydroxyl group interacted with the surface by its oxygen atom to surface hafnium atoms. Isolated oxygen atoms bound to surface hafnium and oxygen atoms, while hydrogen atoms interact only with surface oxygen atoms to form hydroxyl groups. For the dissociation reaction, according to transition searching, H₂O→H (ads)+OH (ads). The energy barriers were endothermic by 9.7 and 17.3 kJ· mol^-1 for the (111) surfaces and exothermic by -59.9 and -47.6 kJ·mol^-1 for the (110) surfaces.
- Ddensity functional theory,
- HfO₂,
- H₂O molecule,
- Adsorption,
- Dissociation
1. [1]
  
  (1) Lee, S. J.; Jeon, T. S.; Kwong, D. L.; Clark, R. J. Appl. Phys.2002, 92, 2807. doi: 10.1063/1.1500420
2. [2]
  (2) Wilk, G. D.;Wallace, R. M.; Anthony, J. M. J. Appl. Phys. 2001,89, 5243. doi: 10.1063/1.1361065
3. [3]
  (3) Yeo, Y.; King, T.; Hu, C. J. Appl. Phys. 2002, 92, 7266. doi: 10.1063/1.1521517
4. [4]
  (4) Aarik, J.; Mandar, H.; Kirm, M.; Pung, L. Thin Solid Films2004, 466, 41. doi: 10.1016/j.tsf.2004.01.110
5. [5]
  (5) Terki, R.; Feraoun, H.; Bertrand, G.; Aourag, H. Comput. Mater.Sci. 2005, 33, 44. doi: 10.1016/j.commatsci.2004.12.059
6. [6]
  (6) Cockayn, E. Phys. Rev. B 2007, 75, 094103. doi: 10.1103/PhysRevB.75.094103
7. [7]
  (7) Mavrou, G.; Galata, S.; Tsipas, P.; Sotiropoulos, A.;Panayiotatos, Y.; Dimoulas, A.; Evangelou, E. K.; Seo, J.W.;Dieker, C. J. Appl. Phys. 2008, 103, 014506.
8. [8]
  (8) Atashi, B. M.; Javier, F. S.; Charles, B. M. Phys. Rev. B 2006,73, 115330. doi: 10.1103/PhysRevB.73.115330
9. [9]
  (9) Ryshkewitch, E.; Richerson, D.W. Oxide Ceramics, PhysicalChemistry and Technology; Academic: Floride, 1985.
10. [10]
  (10) Waldorf, A. J.; Dobrowolski, J. A.; Sullivan, B. T.; Plante, L. M.Appl. Opt. 1993, 32, 5583. doi: 10.1364/AO.32.005583
11. [11]
  (11) He, G.; Zhu, L. Q.; Liu, M.; Zhang, Q. Appl. Surf. Sci. 2007,253, 3413. doi: 10.1016/j.apsusc.2006.07.055
12. [12]
  (12) Mukhopadhyay, A. B.; Musgrave, C. B.; Sanz, J. F. J. Am.Chem. Soc. 2008, 130, 11996. doi: 10.1021/ja801616u
13. [13]
  (13) Biercuk, M. J.; Mason, N.; Marcus, C. M. Nano Lett. 2004, 4, 1.
14. [14]
  (14) Widjaja, Y.; Musgrave, C. B. J. Chem. Phys. 2002, 117, 1931.doi: 10.1063/1.1495847
15. [15]
  (15) Alam, M. A.; Green, M. L. J. Appl. Phys. 2003, 94, 3403. doi: 10.1063/1.1599978
16. [16]
  (16) Fihol, J. S.; Neurock, M. Angew. Chem. Int. Edit. 2006, 45, 402.doi: 10.1002/(ISSN)1521-3773
17. [17]
  (17) khale, A. A.; Dumesic, J. A.; Mavrikakis, M. J. Am. Chem.Soc. 2008, 130, 1402. doi: 10.1021/ja0768237
18. [18]
  (18) Phatak, A. A.; Delgass,W. N.; Riberiro, F. H.; Scheider,W. F.J. Phys. Chem. C 2009, 113, 7269. doi: 10.1021/jp810216b
19. [19]
  (19) Zhang, J. L.;Wang, C.; Fu, Y.; Che, Y. C.; Zhou, C.W. ACSNano 2011, 5, 3284. doi: 10.1021/nn2004298
20. [20]
  (20) Javey, A.; Guo, J.; Farmer, D. B.;Wang, Q. Nano Lett. 2004, 4,447. doi: 10.1021/nl035185x
21. [21]
  (21) Wang, T.; Ekerdt, J. G. Chem. Mater. 2009, 21, 3096. doi: 10.1021/cm9001064
22. [22]
  (22) Iskandarova, I. M.; Knizhnik, A. A.; Rykova, E. A.;Bagaturyants, A. A.; Potapkin, B. V.; Korkin, A. A.Microelectron. Eng. 2003, 69, 587. doi: 10.1016/S0167-9317(03)00350-2
23. [23]
  (23) Atashi, B.; Mukhopadhyay, J. F. S.; Musgrave, C. B. Chem.Mater. 2006, 18, 3397. doi: 10.1021/cm060679r
24. [24]
  (24) Serge, V.; Navrotsky, U. A. Appl. Phys. Lett. 2005, 87, 164103.doi: 10.1063/1.2108113
25. [25]
  (25) Fang, Z. F.; Outlaw, M. D.; Smith, K. K.; Gist, N.; Li, S. G.;Dixon, D. A. J. Phys. Chem. C 2012, 116, 8475.
26. [26]
  (26) Jung, C.; Koyama, M.; Kubo, M.; Imamura, A.; Miyamoto, A.Appl. Surf. Sci. 2005, 244, 644. doi: 10.1016/j.apsusc.2004.10.141
27. [27]
  (27) Yang, Y. L.; Lu, C. H.; Huang, J.; Li, Y.; Chen,W. K. Chin. J.Catal. 2009, 30, 328. [杨亚丽, 陆春海, 黄娟, 李奕, 陈文凯. 催化学报, 2009, 30, 328.]
28. [28]
  (28) Chen, G. H.; Hou, Z. F.; ng, X. G. Comput. Mater. Sci. 2008,44, 46. doi: 10.1016/j.commatsci.2008.01.051
29. [29]
  (29) Caravaca, M. A.; Casali, R. A. J. Phys., Condens. Matter. 2005,17, 5795. doi: 10.1088/0953-8984/17/37/015
30. [30]
  (30) Rignanese, G. M.; nze, X.; Jun, G..; Cho, K.; Pasquarello, A.Phys. Rev. B 2004, 69, 4301.
31. [31]
  (31) Demkov, A. A. Phys. Status Solidi B 2001, 26, 57.
32. [32]
  (32) Wang, J.; Li, H.; Stevens, R. J. Mater. Sci. 1992, 27, 5397. doi: 10.1007/BF00541601
33. [33]
  (33) Delly, B. J. Chem. Phys. 1990, 92, 508. doi: 10.1063/1.458452
34. [34]
  (34) Delly, B. J. Chem. Phys.2000, 113, 7756. doi: 10.1063/1.1316015
35. [35]
  (35) Perdew, J. P.;Wang, Y. Phys. Rev. B 1992, 45, 13244. doi: 10.1103/PhysRevB.45.13244
36. [36]
  (36) Du, Y. D.; Zhao,W. N.; Guo, X.; Zhang, Y. F.; Chen,W. K. ActaPhys. -Chim. Sin. 2011, 27, 1075. [杜玉栋, 赵伟娜, 郭欣,章永凡, 陈文凯. 物理化学学报, 2011, 27, 1075.] doi: 10.3866/PKU.WHXB20110444
37. [37]
  (37) Sun, B. Z.; Chen,W. K.; Xu, Y. J. J. Phys. Chem. C 2010, 114,6543. doi: 10.1021/jp912075t
38. [38]
  (38) Sun, B. Z.; Chen,W. K.; Xu, Y. J. J. Phys. Chem. C 2011, 115,5800. doi: 10.1021/jp111045t
39. [39]
  (39) Verlusi, L.; Zeigler, T. Chem. Phys. 1988, 88, 322.
40. [40]
  (40) Ortmann, F.; Bechstedt, F.; Schmidt,W. G. Phys. Rev. B 2006,73, 5101.
41. [41]
  (41) Halgren, T. A.; Lipscomb,W. N. Chem. Phys. Lett. 1977, 49,225. doi: 10.1016/0009-2614(77)80574-5
42. [42]
  (42) Ma, M.; Zhang, X.; Peng. L. L.;Wang, J. B. Tetrahedron Lett.2007, 48, 1095. doi: 10.1016/j.tetlet.2006.12.090
43. [43]
  (43) Ziolek, M.; Kujawa, J.; Saur, O.; Lavalley, J. C. J. Mol. Catal.A: Chem. 1995, 97, 49. doi: 10.1016/1381-1169(94)00068-9
44. [44]
  (44) Xu, H.; Zhang, R. Q.; Ng, A. M. C.; Djurisic, A. B.; Chan, H. T.;Chan,W. K.; Tong, S. Y. J. Phys. Chem. C 2011, 115, 19710.doi: 10.1021/jp2032884
45. [45]
  (45) Bandura, A. V.; Kubicki, J. D.; Sofo, J. O. J. Phys. Chem. B2008, 112, 11616. doi: 10.1021/jp711763y
46. [46]
  (46) Batzill, M.; Bergermayer,W.; Tanaka, I.; Diebold, U. Surf. Sci.Lett. 2006, 600, 29. doi: 10.1016/j.susc.2005.11.034
47. [47]
  (47) Bustamanta, M.; Valencia, I.; Castro, M. J. Phys. Chem. A 2011,115, 4115. doi: 10.1021/jp108503e
48. [48]
  (48) Paul, J.; Hoffmann, F. M. J. Phys. Chem. 1986, 90, 5321. doi: 10.1021/j100412a083
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Adsorption and Dissociation of Water on HfO₂(111) and (110) Surfaces