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Author:

Bo, Tao (Bo, Tao.) | Lan, Jian-Hui (Lan, Jian-Hui.) | Zhang, Yu-Juan (Zhang, Yu-Juan.) | Zhao, Yao-Lin (Zhao, Yao-Lin.) | He, Chao-Hui (He, Chao-Hui.) | Chai, Zhi-Fang (Chai, Zhi-Fang.) | Shi, Wei-Qun (Shi, Wei-Qun.)

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SCIE Scopus

Abstract:

The interfacial interaction of uranium mononitride (UN) with water from the environment unavoidably leads to corrosion of nuclear fuels, which affects a lot of processes in the nuclear fuel cycle. In this work, the microscopic adsorption behaviors of water on the UN(001) surface as well as water dissociation and accompanying H-2 formation mechanisms have been investigated on the basis of DFT+U calculations and ab initio atomistic thermodynamics. For adsorption of one H2O monomer, the predicted adsorption energies are -0.88, -2.07, and -2.07 eV for the most stable molecular, partially dissociative, and completely dissociative adsorption, respectively. According to our calculations, a water molecule dissociates into OH and H species via three pathways with small energy barriers of 0.78, 0.72, and 0.85 eV, respectively. With the aid of the neighboring H atom, H-2 formation through the reaction of H* + OH* can easily occur via two pathways with energy barriers of 0.61 and 0.36 eV, respectively. The molecular adsorption of water shows a slight coverage dependence on the surface while this dependence becomes obvious for partially dissociative adsorption as the water coverage increases from 1/4 to 1 ML. In addition, based on the "ab initio atomistic thermodynamic'' simulations, increasing H2O partial pressure will enhance the stability of the adsorbed system and water coverage, while increasing temperature will decrease the H2O coverage. We found that the UN(001) surface reacts easily with H2O at room temperature, leading to dissolution and corrosion of the UN fuel materials.

Keyword:

Author Community:

  • [ 1 ] [Bo, Tao; Lan, Jian-Hui; Chai, Zhi-Fang; Shi, Wei-Qun] Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China
  • [ 2 ] [Bo, Tao; Lan, Jian-Hui; Chai, Zhi-Fang; Shi, Wei-Qun] Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China
  • [ 3 ] [Bo, Tao; Zhao, Yao-Lin; He, Chao-Hui] Xi An Jiao Tong Univ, Sch Nucl Sci & Technol, Xian 710049, Peoples R China
  • [ 4 ] [Zhang, Yu-Juan] Univ Sci & Technol Beijing, Sch Mat Sci & Engn, Beijing 100083, Peoples R China
  • [ 5 ] [Bo, Tao]Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China
  • [ 6 ] [Lan, Jian-Hui]Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China
  • [ 7 ] [Chai, Zhi-Fang]Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China
  • [ 8 ] [Shi, Wei-Qun]Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China
  • [ 9 ] [Bo, Tao]Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China
  • [ 10 ] [Lan, Jian-Hui]Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China
  • [ 11 ] [Chai, Zhi-Fang]Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China
  • [ 12 ] [Shi, Wei-Qun]Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China
  • [ 13 ] [Bo, Tao]Xi An Jiao Tong Univ, Sch Nucl Sci & Technol, Xian 710049, Peoples R China
  • [ 14 ] [Zhao, Yao-Lin]Xi An Jiao Tong Univ, Sch Nucl Sci & Technol, Xian 710049, Peoples R China
  • [ 15 ] [He, Chao-Hui]Xi An Jiao Tong Univ, Sch Nucl Sci & Technol, Xian 710049, Peoples R China
  • [ 16 ] [Zhang, Yu-Juan]Univ Sci & Technol Beijing, Sch Mat Sci & Engn, Beijing 100083, Peoples R China

Reprint Author's Address:

  • Chinese Acad Sci, Inst High Energy Phys, Lab Nucl Energy Chem, Beijing 100049, Peoples R China.; Shi, WQ (reprint author), Chinese Acad Sci, Inst High Energy Phys, Key Lab Biomed Effects Nanomat & Nanosafety, Beijing 100049, Peoples R China.

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Source :

PHYSICAL CHEMISTRY CHEMICAL PHYSICS

ISSN: 1463-9076

Year: 2016

Issue: 19

Volume: 18

Page: 13255-13266

4 . 1 2 3

JCR@2016

3 . 4 3 0

JCR@2019

ESI Discipline: CHEMISTRY;

ESI HC Threshold:177

JCR Journal Grade:2

CAS Journal Grade:2

Cited Count:

WoS CC Cited Count: 13

SCOPUS Cited Count: 22

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 9

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