Density Functional Theory Study of Water Activation at Au-Ceria Interfaces

Eunji Kang; Hyuk Choi; Ju Hyeok Lee; Hyun You Kim

doi:10.3740/MRSK.2021.31.4.232

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2021 Vol.31, Issue 4 Preview Page Next Page

Density Functional Theory Study of Water Activation at Au-Ceria Interfaces 세륨산화물과 금 나노입자의 계면에서 일어나는 물 분자의 활성화

April 2021. pp. 232-236

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Abstract

We use vdW-corrected density functional theory (DFT) calculations with additional electron distribution correction to study the water binding chemistry of an Au nanoparticle supported on CeO₂(111) with a linear step-edge. The initial structural model of Au/CeO₂ used for DFT calculations is constructed by stabilizing a Au9 nanoparticle at the linear step-edge on a CeO₂(111) slab. The calculated binding energy of a water molecule clearly shows that the interfacial site between Au and CeO₂ binds water more strongly than the binding sites at the surface of Au nanoparticle. Subsequent water dissociation calculation result shows that the interface-bound water can be relatively easily dissociated into–OH and –H, providing a hydroxyl group that can be utilized as an oxygen source for CO oxidation. Based on the low dissociation energy of the interface bound water molecule, we suggest that the water at the Au-CeO₂ interface can facilitate further oxidation of Au-bound CO. Our results point out that Au-CeO₂ interface-bound water is beneficial for low-temperature oxidation reactions such as the water-gas shift reaction or preferential CO oxidation reaction.

Keywords

density functional theory

cerium oxide

chemisorption

water

References

T. Risse, S. Shaikhutdinov, N. Nilius, M. Sterrer and H.- J. Freund, Acc. Chem. Res., 41, 949 (2008). 10.1021/ar800078m18616299

S. Schauermann and H.-J. Freund, Acc. Chem. Res., 48, 2775 (2015). 10.1021/acs.accounts.5b0023726366783

S. Schauermann, N. Nilius, S. Shaikhutdinov and H.-J. Freund, Acc. Chem. Res., 46, 1673 (2013). 10.1021/ar300225s23252628

M. Cargnello, V. V. Doan-Nguyen, T. R. Gordon, R. E. Diaz, E. A. Stach, R. J. Gorte, P. Fornasiero and C. B. Murray, Science, 341, 771 (2013). 10.1126/science.124014823868919

H. Y. Kim and G. Henkelman, J. Phys. Chem. Lett., 4, 216 (2013). 10.1021/jz301778b26291234

J. Graciani, K. Mudiyanselage, F. Xu, A. E. Baber, J. Evans, S. D. Senanayake, D. J. Stacchiola, P. Liu, J. Hrbek and J. F. Sanz, Science, 345, 546 (2014). 10.1126/science.125305725082699

J. A. Rodriguez, D. C. Grinter, Z. Liu, R. M. Palomino and S. D. Senanayake, Chem. Soc. Rev., 46, 1824 (2017). 10.1039/C6CS00863A28210734

H. Ha, S. Yoon, K. An and H. Y. Kim, ACS Catal., 8, 11491 (2018). 10.1021/acscatal.8b03539

Y. Choi, S. K. Cha, H. Ha, S. Lee, H. K. Seo, J. Y. Lee, H. Y. Kim, S. O. Kim and W. Jung, Nat. Nanotechnol., 14, 245 (2019). 10.1038/s41565-019-0367-430778213

10.

M. Yoo, Y.-S. Yu, H. Ha, S. Lee, J.-S. Choi, S. Oh, E. Kang, H. Choi, H. An and K.-S. Lee, Energy Environ. Sci., 13, 1231 (2020). 10.1039/C9EE03492G

11.

H. Y. Kim and G. Henkelman, J. Phys. Chem. Lett., 3, 2194 (2012). 10.1021/jz300631f26295770

12.

H. Y. Kim, H. M. Lee and G. Henkelman, J. Am. Chem. Soc., 134, 1560 (2012). 10.1021/ja207510v22191484

13.

L. Zhang, H. Y. Kim and G. Henkelman, J. Phys. Chem. Lett., 4, 2943 (2013). 10.1021/jz401524d

14.

B. Qiao, A. Wang, X. Yang, L. F. Allard, Z. Jiang, Y. Cui, J. Liu, J. Li and T. Zhang, Nat. Chem., 3, 634 (2011). 10.1038/nchem.109521778984

15.

A. Wang, J. Li and T. Zhang, Nat. Rev. Chem., 2, 65 (2018). 10.1038/s41570-018-0010-1

16.

J. A. Rodriguez, P. Liu, J. Hrbek, J. Evans and M. Perez, Angew. Chem., Int. Ed., 46, 1329 (2007). 10.1002/anie.20060393117205589

17.

J. A. Rodriguez, J. Graciani, J. Evans, J. B. Park, F. Yang, D. Stacchiola, S. D. Senanayake, S. Ma, M. Perez and P. Liu, Angew. Chem., 121, 8191 (2009). 10.1002/ange.200903918

18.

J. A. Rodriguez, J. C. Hanson, D. Stacchiola and S. D. Senanayake, Phys. Chem. Chem. Phys., 15, 12004 (2013). 10.1039/c3cp50416f23660768

19.

A. Bruix, J. A. Rodriguez, P. J. Ramírez, S. D. Senanayake, J. Evans, J. B. Park, D. Stacchiola, P. Liu, J. Hrbek and F. Illas, J. Am. Chem. Soc., 134, 8968 (2012). 10.1021/ja302070k22563752

20.

H. Y. Kim and P. Liu, ChemCatChem, 5, 3673 (2013). 10.1002/cctc.201300449

21.

J. B. Park, J. Graciani, J. Evans, D. Stacchiola, S. Ma, P. Liu, A. Nambu, J. F. Sanz, J. Hrbek and J. A. Rodriguez, Proc. Natl. Acad. Sci. U. S. A., 106, 4975 (2009). 10.1073/pnas.081260410619276120PMC2664040

22.

H. Ha, H. An, M. Yoo, J. Lee and H. Y. Kim, J. Phys. Chem, 121, 26895 (2017). 10.1021/acs.jpcc.7b09780

23.

G. Kresse and J. Furthmuller, Phys. Rev. B, 54, 11169 (1996). 10.1103/PhysRevB.54.111699984901

24.

S. L. Dudarev, G. A. Botton, S. Y. Savrasov, C. J. Humphreys and A. P. Sutton, Phys. Rev. B, 57, 1505 (1998). 10.1103/PhysRevB.57.1505

25.

D. Fernandez-Torre, K. Kosmider, J. Carrasco, M. V. Ganduglia-Pirovano and R. Perez, J. Phys. Chem. C, 116, 13584 (2012). 10.1021/jp212605g

26.

K. Jiri, R. B. David and M. Angelos, J. Phys.: Condens. Matter, 22, 022201 (2010). 10.1088/0953-8984/22/2/02220121386245

27.

J. Klimes, D. R. Bowler and A. Michaelides, Phys. Rev. B, 83, 195131 (2011). 10.1103/PhysRevB.83.195131

28.

P. E. Blochl, Phys. Rev. B, 50, 17953 (1994). 10.1103/PhysRevB.50.179539976227

29.

K. Shin, L. Zhang, H. An, H. Ha, M. Yoo, H. M. Lee, G. Henkelman, H. Y. Kim, Nanoscale, 9, 5244 (2017). 10.1039/C7NR01382E28397916

30.

H. Choi, E. Kang, H. Y. Kim, Korean J. Mater. Res., 30, 267 (2020). 10.3740/MRSK.2020.30.5.267

Information

Publisher :Materials Research Society of Korea
Publisher(Ko) :한국재료학회
Journal Title :Korean Journal of Materials Research
Journal Title(Ko) :한국재료학회지
Volume : 31
No :4
Pages :232-236
Received Date : 2021-01-31
Revised Date : 2021-03-14
Accepted Date : 2021-03-16
DOI :https://doi.org/10.3740/MRSK.2021.31.4.232

Korean Journal of Materials Research ISSN:1225-0562(Print) 2287-7258(Online) 한국재료학회지

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