Surface modification of tungsten oxide by oxygen vacancies for hydrogen adsorption

doi:10.1016/j.jmst.2021.10.048

Abstract

Abstract:

A model for describing the adsorption process of hydrogen on surface of tungsten oxide was proposed based on the first-principle calculations. Multiple factors such as type of active surface, adsorption site and distribution of oxygen vacancies were considered to evaluate the hydrogen adsorption capability of tungsten oxide. The adsorption Gibbs free energies, electronic structures and bonding characteristics under various conditions were examined to reveal the influence of oxygen vacancies on the surface. It is found that the capability of hydrogen adsorption of tungsten oxide can be significantly enhanced by adjusting the oxygen vacancy on the outermost layer of certain active surfaces. The modeling predicts that the surface structure stability and gas adsorption ability of tungsten oxide can be simultaneously improved through the formation of W—H bonds. The proposed strategy for moderating surface provides a new approach to obtain excellent gas-sensitive metal oxide materials.

Key words: Metal oxide, Gas-sensitive material, Surface adsorption, Oxygen vacancy, First-principles calculation

Q. Zhang, F.W. Tang, Z. Zhao, Z.R. Nie, X.Y. Song. Surface modification of tungsten oxide by oxygen vacancies for hydrogen adsorption[J]. J. Mater. Sci. Technol., 2022, 117: 23-35.

Figures/Tables 14

Fig. 1. Diagrams for crystal and surface structures of monoclinic WO3: (a) WO3 crystal supercell; (b) W—O-terminated (0 0 1)WO3 surface; (c) O-terminated (0 0 1)WO3 surface; (d) (1 1 0)WO3 surface. The green and blue balls represent O and W atoms, respectively.

Fig. 2. The tendency of H atoms (represented by red balls) moving to stable adsorption sites on O-terminated (0 0 1)WO3 surface, observed from perpendicular and parallel directions of the surface.

Fig. 3. Adsorption Gibbs free energy, Mulliken bond population and bond lengths after H adsorption on (0 0 1)WO3 surface: (a) H adsorption on O-terminated (0 0 1)WO3 surface; (b) H adsorption on W—O-terminated (0 0 1)WO3 surface.

Fig. 4. Charge population after H adsorption on (0 0 1)WO3 surface: (a) H adsorption on O-terminated (0 0 1)WO3 surface; (b) H adsorption on W—O-terminated (0 0 1)WO3 surface.

Fig. 5. Typical adsorption sites on W—O-terminated (0 0 1)WO3 surface: (a) on top of oxygen atom (represented as O-top site); (b) on top of the tungsten atom, (represented as W-top site); (c) at bridge position between the tungsten and oxygen atoms (represented as bridge site); (d) at geometric central position of four oxygen atoms (represented as central site). The insets show different adsorption sites viewed from the top of the structure.

Fig. 6. The local charge density distributions on W—O-terminated (0 0 1)WO3 surface after H adsorption at different positions: (a) O-top; (b) W-top; (c) bridge; (d) central.

Fig. 7. PDOS of W—O-terminated (0 0 1)WO3 surface after H adsorption at different positions: (a) O-top; (b) W-top; (c) bridge; (d) central.

Fig. 8. Four types of H adsorption sites on (1 1 0)WO3 surface: (a) before adsorption; (b) after adsorption.

Fig. 9. Adsorption Gibbs free energy, Mulliken bond population and bond lengths on (1 1 0)WO3 surface with oxygen vacancies locating at different positions.

Fig. 10. Typical (1 1 0)WO3 surfaces with different distributions of oxygen vacancies: (a) oxygen vacancy on outermost surface (represented as vacancy-1) and on internal surface (represented as vacancy-2); (b) symmetric mode (represented as vacancies-1,S) and adjacent mode (represented as vacancies-1,A).

Fig. 11. TDOS of (1 1 0) surfaces with no oxygen vacancy and with different distributions of oxygen vacancies.

Fig. 12. Charge population after H adsorption on (1 1 0)WO3 surface with different distribution of oxygen vacancies.

Fig. 13. Charge density distribution on (1 1 0)WO3 surface with different distribution of oxygen vacancies after H adsorption on O-top site: (a) no vacancy on surface; (b) oxygen vacancy on the outermost surface.

Fig. 14. PDOS of (1 1 0)WO3 surface after H adsorption on O-top site: (a) (1 1 0)WO3 surfaces with different distributions of oxygen vacancies; (b) surface with no oxygen vacancy; (c) oxygen vacancy on the outermost surface; (d) oxygen vacancy on internal surface.

References 51

[1]	C.J. Dong, R.J. Zhao, L.J. Yao, Y. Ran, X. Zhang, Y.D. Wang, J. Alloy. Compd. 820 (2020) 153194. DOI URL
[2]	Y.H. Yang, R.H. Xie, H. Li, C.J. Liu, W.H. Liu, F.Q. Zhan, Trans. Nonferr. Met. Soc. China 26 (2016) 2390-2396. DOI URL
[3]	M. Bourdin, I. Mjejri, A. Rougier, C. Labrugere, T. Cardinal, Y. Messaddeq, M. Gaudon, J. Alloy. Compd. 823 (2020) 153690. DOI URL
[4]	M.B. Zheng, H. Tang, Q. Hu, L.L. Li, J. Xu, H. Pang, Adv. Funct. Mater. 28 (2018) 1707500. DOI URL
[5]	J. Kukkola, J. Mäklin, N. Halonen, T. Kyllönen, G. Tóth, M. Szabó, A. Shchukarev, J. Mikkola, H. Jantunen, K. Kordás, Actuators B Chem. 153 (2011) 293-300. DOI URL
[6]	H.Q. Zuo, J.X. Tao, H. Shi, J. He, Z.Y. Zhou, C. Zhang, Acta Biomater. 80 (2018) 296-307. DOI URL
[7]	A. Boudiba, C. Zhang, C. Bittencourt, P. Umek, M.G. Olivier, R. Snyders, M. De- bliquy, Procedia Eng. 47 (2012) 228-231. DOI URL
[8]	C.S. Rout, M. Hegde, C.N.R. Rao, Sensor. Actuators B Chem. 128 (2008) 488-493. DOI URL
[9]	T. Samerjai, N. Tamaekong, C. Liewhiran, A. Wisitsoraat, A. Tuantranont, S. Phanichphant, Sens. Actuators B Chem. 157 (2011) 290-297. DOI URL
[10]	D.V. DAO, K. Shibuya, T.T. Bui, S. Sugiyama, Procedia Eng. 25 (2011) 1149-1152. DOI URL
[11]	T. Hübert, L. Boon-Brett, G. Black, U. Banach, Sens. Actuators B Chem. 157 (2011) 329-352. DOI URL
[12]	W.J. Buttner, M.B. Post, R. Burgess, C. Rivkin, Int. J. Hydrog. Energy 36 (2011) 2462-2470. DOI URL
[13]	S.J. Ippolito, S. Kandasamy, K. Kalantar-zadeh, W. Wlodarski, Sens. Actuators B Chem. 108 (2005) 154-158. DOI URL
[14]	H. Nakagawa, N. Yamamoto, S. Okazaki, T. Chinzei, S. Asakura, Sens. Actuators B Chem. 93 (2003) 468-474. DOI URL
[15]	B. Liu, D.P. Cai, Y. Liu, D.D. Wang, L.L. Wang, Y.R. Wang, H. Li, Q.H. Li, T.H. Wang, Sens. Actuators B Chem. 193 (2014) 28-34. DOI URL
[16]	Y.X. Qin, D.Y. Hua, M. Liu, J. Alloy. Compd. 587 (2014) 227-233. DOI URL
[17]	F. Li, Q.X. Qin, N. Zhang, C. Chen, L. Sun, X. Liu, Y. Chen, C.N. Li, S.P. Ruan, Sens. Actuators B Chem. 244 (2017) 837-848. DOI URL
[18]	J.C. Lim, C. Jin, M.S. Choi, M.Y. Kim, S. Kim, S.M. Choi, S.H. Baek, K.H. Lee, H.S. Kim, Ceram. Int. 47 (2021) 20956-20964. DOI URL
[19]	F.H. Tian, C. Gong, R. Wu, Z.Z. Liu, Mater. Today Chem. 9 (2018) 28-33.
[20]	P.S. Venkatesh, P. Dharmaraj, V. Purushothaman, V. Ramakrishnan, K. Je- ganathan, Sens. Actuators B Chem. 212 (2015) 10-17. DOI URL
[21]	G. Pacchioni, ChemPhysChem 4 (2003) 1041-1047. DOI URL
[22]	C. Zhang, G.F. Liu, X. Geng, K.K. Wu, M. Debliquy, Sens. Actuators A Phys. 309 (2020) 112026. DOI URL
[23]	X.W. Shen, C.Z. Huang, Y.F. Li, Talanta 72 (2007) 1432-1437. DOI URL
[24]	G.S. Zakharova, Y.L. Liu, A.N. Enyashin, X. Yang, J. Zhou, W. Jin, W. Chen, Sens. Actuators B Chem. 256 (2018) 1021-1029. DOI URL
[25]	J.W. Christian, The Theory of Transformations in Metals and Alloys, Newnes, 2002.
[26]	JJ.M. Órfão, AIChE J. 53 (2007) 2905-2915. DOI URL
[27]	D.D. Wang, D.X. Han, L. Liu, L. Niu, J. Mater. Chem. A 4 (2016) 14416-14422. DOI URL
[28]	V. Nagarajan, R. Chandiramouli, Superlattices Microstruct. 78 (2015) 22-39. DOI URL
[29]	B. Liu, Y.M. Xu, K. Li, H. Wang, L. Gao, Y.Y. Luo, G.T. Duan, ACS Appl. Mater. Interfaces 11 (2019) 16838-16846. DOI URL
[30]	W.Q. Lai, K. Zhang, P.H. Shao, L.M. Yang, L. Ding, S.G. Pavlostathis, H. Shi, L.Z. Zou, D.H. Liang, X.B. Luo, J. Hazard. Mater. 379 (2019) 120791. DOI URL
[31]	L.H. Zhao, F.H. Tian, X.B. Wang, W.W. Zhao, A.P. Fu, Y.Y. Shen, S.G. Chen, S.Q. Yu, Comput. Mater. Sci. 79 (2013) 691-697. DOI URL
[32]	X.B. Wang, F.H. Tian, W.W. Zhao, A.P. Fu, L.H. Zhao, Comput. Mater. Sci. 68 (2013) 218-221. DOI URL
[33]	P.M. Oliver, S.C. Parker, R.G. Egdell, F.H. Jones, J. Chem. Soc. 92 (1996) 2049-2056.
[34]	P.J. Jiang, Y.Y. Xiao, W.J. Liu, X.B. Yu, Results Phys. 12 (2019) 896-902. DOI URL
[35]	M.D. Segall, P.J.D. Lindan, M.J. Probert, C.J. Pickard, P.J. Hasnip, S.J. Clark, M.C. Payne, J. Phys. Condens. Matter 14 (2002) 2717-2744. DOI URL
[36]	M.Y. Wang, W. Wang, M. Ji, X.L. Cheng, Appl. Surf. Sci. 439 (2018) 350-363. DOI URL
[37]	P. Basumatary, D. Konwar, Y.S. Yoon, Appl. Catal. B Environ. 267 (2020) 118724. DOI URL
[38]	Y.H. Dai, Math. Program. 138 (2013) 501-530. DOI URL
[39]	B.K. Zhang, J. Zhou, S.R. Elliott, Z.M. Sun, J. Mater. Chem. A 8 (2020) 23947-23954. DOI URL
[40]	J.G. Howalt, T. Bligaard, J. Rossmeisl, T. Vegge, Phys. Chem. Chem. Phys. 15 (2013) 7785-7795. DOI PMID
[41]	B.K. Zhang, J. Zhou, Z.L. Guo, Q. Peng, Z.M. Sun, Appl. Surf. Sci. 500 (2020) 144248. DOI URL
[42]	B. Grosjean, C. Pean, A. Siria, L. Bocquet, R. Vuilleumier, M.L. Bocquet, J. Phys. Chem. Lett. 7 (2016) 4695-4700. PMID
[43]	A. Jalil, Z.W. Zhuo, Z.T. Sun, F. Wu, C. Wang, X.J. Wu, J. Mater. Chem. A 8 (2020) 1307-1314. DOI URL
[44]	Z. Meng, B.K. Zhang, Q. Peng, Y.D. Yu, J. Zhou, Z.M. Sun, Appl. Surf. Sci. 562 (2021) 150151. DOI URL
[45]	G.X. Tian, Y. Zhang, T.S. Yang, Acta Phys. Chim. Sin. 28 (2012) 1063-1069. DOI URL
[46]	P.G. Jiang, Y.Y. Xiao, W.J. Liu, X.B. Yu, Results Phys. 12 (2019) 896-902. DOI URL
[47]	Q. Liu, F.J. Wang, H.X. Lin, Y.Y. Xie, N. Tong, J.J. Lin, X.Y. Zhang, Z.Z. Zhang, X.X. Wang, Catal. Sci. Technol. 8 (2018) 4399-4406. DOI URL
[48]	H.J. Liu, H. Fu, Y.C. Liu, X.Y. Chen, K.F. Yu, L.W. Wang, Chemosphere 272 (2021) 129534. DOI URL
[49]	Z.M. Wang, H. Wang, X.X. Wang, X. Chen, Y. Yu, W.X. Dai, X.Z. Fu, M. Anpo, J. Phys. Chem. C 125 (2021) 3242-3255. DOI URL
[50]	W.W. Yu, Z.G. Shen, F. Peng, Y. Lu, M.Y. Ge, X.L. Fu, Y. Sun, X. Chen, N. Dai, RSC Adv. 9 (2019) 7723-7728. DOI URL
[51]	H. Wu, Z. Ma, Z.X. Lin, H.Z. Song, S.C. Yan, Y. Shi, Nanomaterials 9 (2019) 388. DOI URL