DFT study on water oxidation on nitrogen-doped ceria oxide

Yong Chao Zhang; Ya Kun Liu; Lei Zhang; Xiu tian feng E; Lun Pan; Xiangwen Zhang; Fazal-e-Aleem; De Rong Zou; Song Hua Liu; Ji Jun Zou

doi:10.1016/j.apsusc.2018.05.048

DFT study on water oxidation on nitrogen-doped ceria oxide

Yong Chao Zhang
, Ya Kun Liu
, Lei Zhang
, Xiu tian feng E
, Lun Pan
, Xiangwen Zhang
, Fazal-e-Aleem
, De Rong Zou
, Song Hua Liu
, Ji Jun Zou^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

23 Citations (Scopus)

Abstract

Heteroatom doping is effective to regulate electronic structure and improve the performance of photocatalyst. Herein, water oxidation on nitrogen-doped CeO ₂ (1 1 0) was investigated by using density functional theory calculation to understand the role of nitrogen doping. The results show that the optimal pathway of water oxidation on perfect and nitrogen-doped CeO ₂ (1 1 0) is H ₂ O → OH + H → O + 2H; O + 2H + H ₂ O → OOH + 3H → O ₂ + 4H, and the rate-limiting step of whole water oxidation process is O + 2H + H ₂ O → OOH + 3H. The presence of nitrogen dopant in CeO ₂ (1 1 0) induces new characteristic peak of impurity level, and reduces the activation energies of water oxidation, especially for the rate-limiting step of O–O bond formation. The reverse reaction of O and H to OH that is easily occur on perfect CeO ₂ (1 1 0) is effectively prohibited on nitrogen-doped counterpart. Additionally, nitrogen dopant makes the rate-limiting step easier than that on oxygen-defective CeO ₂ (1 1 0) from the kinetic perspective. Therefore, nitrogen-doped CeO ₂ is expected to be a promising photocatalyst for water oxidation.

Original language	English
Pages (from-to)	423-428
Number of pages	6
Journal	Applied Surface Science
Volume	452
DOIs	https://doi.org/10.1016/j.apsusc.2018.05.048
Publication status	Published - 15 Sept 2018
Externally published	Yes

Keywords

Ceria oxide
Density functional theory
Nitrogen doping
Water oxidation

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10.1016/j.apsusc.2018.05.048

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@article{e302860f14b9402285aa96e201154aa1,

title = "DFT study on water oxidation on nitrogen-doped ceria oxide",

abstract = " Heteroatom doping is effective to regulate electronic structure and improve the performance of photocatalyst. Herein, water oxidation on nitrogen-doped CeO 2 (1 1 0) was investigated by using density functional theory calculation to understand the role of nitrogen doping. The results show that the optimal pathway of water oxidation on perfect and nitrogen-doped CeO 2 (1 1 0) is H 2 O → OH + H → O + 2H; O + 2H + H 2 O → OOH + 3H → O 2 + 4H, and the rate-limiting step of whole water oxidation process is O + 2H + H 2 O → OOH + 3H. The presence of nitrogen dopant in CeO 2 (1 1 0) induces new characteristic peak of impurity level, and reduces the activation energies of water oxidation, especially for the rate-limiting step of O–O bond formation. The reverse reaction of O and H to OH that is easily occur on perfect CeO 2 (1 1 0) is effectively prohibited on nitrogen-doped counterpart. Additionally, nitrogen dopant makes the rate-limiting step easier than that on oxygen-defective CeO 2 (1 1 0) from the kinetic perspective. Therefore, nitrogen-doped CeO 2 is expected to be a promising photocatalyst for water oxidation.",

keywords = "Ceria oxide, Density functional theory, Nitrogen doping, Water oxidation",

author = "Zhang, \{Yong Chao\} and Liu, \{Ya Kun\} and Lei Zhang and E, \{Xiu tian feng\} and Lun Pan and Xiangwen Zhang and Fazal-e-Aleem and Zou, \{De Rong\} and Liu, \{Song Hua\} and Zou, \{Ji Jun\}",

note = "Publisher Copyright: {\textcopyright} 2018 Elsevier B.V.",

year = "2018",

month = sep,

day = "15",

doi = "10.1016/j.apsusc.2018.05.048",

language = "English",

volume = "452",

pages = "423--428",

journal = "Applied Surface Science",

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TY - JOUR

T1 - DFT study on water oxidation on nitrogen-doped ceria oxide

AU - Zhang, Yong Chao

AU - Liu, Ya Kun

AU - Zhang, Lei

AU - E, Xiu tian feng

AU - Pan, Lun

AU - Zhang, Xiangwen

AU - Fazal-e-Aleem,

AU - Zou, De Rong

AU - Liu, Song Hua

AU - Zou, Ji Jun

PY - 2018/9/15

Y1 - 2018/9/15

N2 - Heteroatom doping is effective to regulate electronic structure and improve the performance of photocatalyst. Herein, water oxidation on nitrogen-doped CeO 2 (1 1 0) was investigated by using density functional theory calculation to understand the role of nitrogen doping. The results show that the optimal pathway of water oxidation on perfect and nitrogen-doped CeO 2 (1 1 0) is H 2 O → OH + H → O + 2H; O + 2H + H 2 O → OOH + 3H → O 2 + 4H, and the rate-limiting step of whole water oxidation process is O + 2H + H 2 O → OOH + 3H. The presence of nitrogen dopant in CeO 2 (1 1 0) induces new characteristic peak of impurity level, and reduces the activation energies of water oxidation, especially for the rate-limiting step of O–O bond formation. The reverse reaction of O and H to OH that is easily occur on perfect CeO 2 (1 1 0) is effectively prohibited on nitrogen-doped counterpart. Additionally, nitrogen dopant makes the rate-limiting step easier than that on oxygen-defective CeO 2 (1 1 0) from the kinetic perspective. Therefore, nitrogen-doped CeO 2 is expected to be a promising photocatalyst for water oxidation.

AB - Heteroatom doping is effective to regulate electronic structure and improve the performance of photocatalyst. Herein, water oxidation on nitrogen-doped CeO 2 (1 1 0) was investigated by using density functional theory calculation to understand the role of nitrogen doping. The results show that the optimal pathway of water oxidation on perfect and nitrogen-doped CeO 2 (1 1 0) is H 2 O → OH + H → O + 2H; O + 2H + H 2 O → OOH + 3H → O 2 + 4H, and the rate-limiting step of whole water oxidation process is O + 2H + H 2 O → OOH + 3H. The presence of nitrogen dopant in CeO 2 (1 1 0) induces new characteristic peak of impurity level, and reduces the activation energies of water oxidation, especially for the rate-limiting step of O–O bond formation. The reverse reaction of O and H to OH that is easily occur on perfect CeO 2 (1 1 0) is effectively prohibited on nitrogen-doped counterpart. Additionally, nitrogen dopant makes the rate-limiting step easier than that on oxygen-defective CeO 2 (1 1 0) from the kinetic perspective. Therefore, nitrogen-doped CeO 2 is expected to be a promising photocatalyst for water oxidation.

KW - Ceria oxide

KW - Density functional theory

KW - Nitrogen doping

KW - Water oxidation

UR - https://www.scopus.com/pages/publications/85046763436

U2 - 10.1016/j.apsusc.2018.05.048

DO - 10.1016/j.apsusc.2018.05.048

M3 - Article

AN - SCOPUS:85046763436

SN - 0169-4332

VL - 452

SP - 423

EP - 428

JO - Applied Surface Science

JF - Applied Surface Science

ER -

DFT study on water oxidation on nitrogen-doped ceria oxide

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